Durham E-Theses Melting ice and cloud electrication Martin, Peter F. How to cite: Martin, Peter F. (1971) Melting ice and cloud electrication, Durham theses, Durham University. Available at Durham E-Theses Online: http://etheses.dur.ac.uk/10371/ Use policy The full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-prot purposes provided that: • a full bibliographic reference is made to the original source • a link is made to the metadata record in Durham E-Theses • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders. Please consult the full Durham E-Theses policy for further details. Academic Support Oce, Durham University, University Oce, Old Elvet, Durham DH1 3HP e-mail: e-theses.admin@dur.ac.uk Tel: +44 0191 334 6107 http://etheses.dur.ac.uk MELTING ICE AND CLOUD ELECTRIFICATION A t h e s i s presented i n candidature f o r the degree of Doctor of Philosophy i n the U n i v e r s i t y of Durham by Peter F- M a r t i n BoSc. o f Grey College June 1971 \ ,13 APR 1972 jBRARl i. FOREWORD Although t h i s t h e s i s i s p r i m a r i l y concerned w i t h the e l e c t r i c a l e f f e c t s of m e l t i n g ice a chapter on the e l e c t r i f i c a t i o n due t o e v a p o r a t i n g ice has been included as t h i s could be r e a d U y s t u d i e d w i t h the apparatus. The S . I . system of u n i t s has been used w i t h two exceptions. c o n c e n t r a t i o n of ions i n s o l u t i o n s are gram molar c o n c e n t r a t i o n s the e l e c t r i c a l c o n d u c t i v i t y of s o l u t i o n s has been expressed i n The and mho cm 1 I should l i k e to express my sincere thanks t o a l l those people who a s s i s t e d me i n any way d u r i n g the course of my work a t Durham. . have In p a r t i c u l a r I am g r a t e f u l t o my supervisor Dr. W.C.A» Hutchinson f o r h i s guidance throughout the i n v e s t i g a t i o n and t o Professor G.D. Rochester, F.R.S. f o r the p r o v i s i o n of research f a c i l i t i e s i n the Physics Department a t Durham. I would also l i k e t o thank Mr. J. Moralee f o r h i s a s s i s t a n c e d u r i n g the c o n s t r u c t i o n of the wind t u n n e l and Mr. J. S c o t t f o r the c o n s t r u c t i o n of the glassware. I am g r a t e f u l t o the other members of the Atmospheric Physics group f o r t h e i r h e l p f u l comments and i n p a r t i c u l a r t o Dr. I.M. Stromberg and Dr. R. Dawson f o r t h e i r advice d u r i n g the e a r l y stages of the work and Mr. K.M. D a i l y f o r h i s attempts to standardize my English. Thanks are also due t o the N a t u r a l Environment Research Council f o r the p r o v i s i o n of a research studentship. F i n a l l y I wish t o thank Mrs. D. Anson f o r her speed and efficiency i n the p r e p a r a t i o n of the t y p e s c r i p t and Mr. J. Normile f o r c a r r y i n g out the d u p l i c a t i o n of the t h e s i s . it 13 APR 1972 ABSTRACT. A v e r t i c a l wind t u n n e l has been c o n s t r u c t e d i n s i d e a cold room t o simulate the f a l l o f a f r o z e n water drop from the 0°C l e v e l i n a thundercloud. but I t was p o s s i b l e t o f r e e l y support an i c e sphere c l e a r o f the sides the p a r t i c l e crashed e a r l y i n the m e l t i n g process. The i c e spheres were f rozen onto a 120 jim diameter p l a t i n u m wire and d u r i n g the f i n a l stages o f m e l t i n g the p a r t i c l e hung from the w i r e and was f r e e t o r o t a t e about a l l 3 degrees o f freedom. The spheres melted on t h i s type of support produced the same amount o f e l e c t r i f i c a t i o n as those melted on the wire loop support used by DRAKE (1968). The charge on the meltwater was found t o be always p o s i t i v e and t o be h i g h l y dependent on the f r e e z i n g r a t e , and water drops f r o z e n i n s t i l l a i r a t between -10 and -15°C produced an order o f magnitude l e s s charging than drops f r o z e n i n an a i r s t r e a m f l o w i n g a t 11 ms Examination o f the i c e p a r t i c l e s under a microscope a t s i m i l a r temperatures. suggested t h a t t h i s e f f e c t was due t o a i r escaping from the ice a t low f r e e z i n g r a t e s and smaller a i r bubbles being formed a t h i g h f r e e z i n g r a t e s . Evidence was found f o r the enhancement o f e l e c t r i f i c a t i o n a t h i g h m e l t i n g r a t e s which DRAKE a t t r i b u t e d t o the onset o f vigorous convection i n the meltwater. The e f f e c t o f carbon d i o x i d e on m e l t i n g e l e c t i f i c a t i o n was a l s o discussed. The e l e c t r i f i c a t i o n due t o m e l t i n g p r e c i p i t a t i o n under i d e a l -3 c o n d i t i o n s i n a thundercloud was estimated as 4 C km which can be _3 compared t o 8 C km found by SIMPSON and ROBINSON ( l 9 4 l ) . I t was suggested t h a t the importance o f m e l t i n g i c e i n thundercloud e l e c t r i f i c a t i o n cannot be e s t a b l i s h e d u n t i l more i n f o r m a t i o n i s a v a i l a b l e on the nature o f the s o l i d p r e c i p i t a t i o n , the environment i n which i t melted and t h e l o c a t i o n and magnitude o f the lower p o s i t i v e charge. CONTENTS FOREWORD i ABSTRACT ii CHAPTER I THE IMPORTANCE OF MELTING ICE IN CLOUD ELECTRIFICATION 1.1 Introduction 1 1.2 The thunderstorm 1 1.3 The e l e c t r i c charge d i s t r i b u t i o n i n thunderstorms 4 1.4 The lower p o s i t i v e charge 5 1.5 Theories of t h e f o r m a t i o n o f t h e lower p o s i t i v e charge 7 Laboratory assessment o f the t h e o r i e s of t h e f o r m a t i o n of the lower p o s i t i v e charge 10 1.6 CHAPTER 2 PREVIOUS STUDIES OF MELTING ICE ELECTRIFICATION 2.1 Experiments With blocks o f i c e 12 2.2 The m e l t i n g o f f r o z e n water drops 12 2.3 The b u b b l e - b u r s t i n g theory of m e l t i n g e l e c t r i f i c a t i o n 13 2.4 Factors i n f l u e n c i n g the charging o f m e l t i n g n a t u r a l ice p a r t i c l e s . 20 CHAPTER 3 THE DESIGN OF A WIND TUNNEL FOR THE FREE FLIGHT OF SMALL ICE SPHERES 3.1 The importance o f a f r e e support system 21 3.2 The problem o f turbulence 21 3.3 Laminar f l o w wind t u n n e l s 24 3.4 V e l o c i t y w e l l systems 26 3.5 The design o f t h e support tube 28 CHAPTER 4 THE CONSTRUCTION AND INSTRUMENTATION OF THE WIND .TUNNEL 4.1 The adaption of the c o l d room 32 4.2 The wind t u n n e l 33 4.3 Measurement o f e l e c t r i c charge 35 4.4 The measurement o f temperature and h u m i d i t y 38 4.5 The measurement o f a i r speed CHAPTER 5 THE PREPARATION OF ARTIFICIAL CLQUDWATER 5*1 The source o f i m p u r i t i e s i n h a i l 42 5.2 Measurement o f i m p u r i t i e s i n c l o u d and r a i n w a t e r 45 5.3 The p r e p a r a t i o n of a r t i f i c i a l cloudwater CHAPTER 6 L "> FREE FLIGHT EXPERIMENTS ON MELTING AND EVAPORATING ICE PARTICLES 6.1 Experimental procedure 50 6.2 The behaviour of the support system 51 6»3 The e l e c t r i f i c a t i o n o f m e l t i n g i c e 53 CHAPTER 7 EXPERIMENTS WITH MELTING ICE SPHERES HANGING.ON PLATINUM WIRES 7.1 The support of m e l t i n g i c e spheres 55 7.2 The experimental procedure 56 7.3 The i c e p a r t i c l e s 58 7.4 The a n a l y s i s o f t h e m e l t i n g experiments 60 CHAPTER 8 THE EFFECT OF MELTING RATE AND FREEZING TEMPERATURE ON MELTING ELECTRIFICATION 8.1 M e l t i n g r a t e and the environment 64 8.2 The e f f e c t o f m e l t i n g r a t e on e l e c t r i f i c a t i o n 65 8.3 The e f f e c t of the support 67 8.4 Freezing r a t e and m e l t i n g e l e c t r i f i c a t i o n 68 8.5 A.ir bubbles and m e l t i n g e l e c t r i f i c a t i o n 70 806 Comparison w i t h previous experiments 74 CHAPTER 9 THE EFFECT OF CARBON DIOXIDE ON MELTING ELECTRIFICATION 9.1 Carbon d i o x i d e and l a b o r a t o r y experiments 75 9.2 The importance o f carbon d i o x i d e i n m e l t i n g electrification 76 9.3 An experiment t o determine the e f f e c t o f atmospheric carbon d i o x i d e 77 9.4 The absorption o f carbon d i o x i d e by a water drop 79 Carbon d i o x i d e l e v e l s i n p r e v i o u s l a b o r a t o r y experiments Conclusion 80 81 9.5 9.6 CHAPTER 10 THE ELECTRICAL EFFECTS OF THE MELTING OF REAL PRECIPITATION 10.1 The l o c a t i o n o f t h e lower p o s i t i v e 10.2 S o l i d p r e c i p i t a t i o n i n thunderstorms 85 10.3 M e l t i n g i c e and t h e magnitude of t h e lower p o s i t i v e charge 89 CHAPTER 11 charge THE ELECTRIFICATION OF EVAPORATING ICE SPHERES 11.1 Previous work 93 11.2 The e l e c t r i f i c a t i o n of i c e p a r t i c l e s evaporating i n the wind t u n n e l 94 I n t e r p r e t a t i o n of the wind t u n n e l experiment 94 11.3 CHAPTER 12 CONCLUSIONS AND SUGGESTIONS FOR FURTHER WORK 12.1 The design o f a wind t u n n e l t o study the e l e c t r i f i c a t i o n of p r e c i p i t a t i o n 96 12.2 The e l e c t r i f i c a t i o n o f m e l t i n g i c e 97 12.3 The r o l e of m e l t i n g i c e i n cloud 98 APPENDIX 1 Al.l A1.2 A1.3 A1.4 A1.5 electrification MELTING ELECTRIFICATION DATA The e l e c t r i f i c a t i o n o f i c e spheres m e l t i n g on p l a t i n u m w i r e s - a r t i f i c i a l cloudwater 100 The e l e c t r i f i c a t i o n o f i c e spheres m e l t i n g on p l a t i n u m w i r e s - deionized water 102. The e l e c t r i f i c a t i o n o f i c e spheres m e l t i n g on p l a t i n u m loops - f r o z e n i n s t i l l a i r 103 The e l e c t r i f i c a t i o n o f i c e spheres m e l t i n g on p l a t i n u m loops - frozen i n a i r s t r e a m 104 F o r t r a n program used t o process the m e l t i n g e l e c t r i f i c a t i o n data 105 APPENDIX 2 THE ABSORPTION AND DESQRPTION OF CARBON DIOXIDE BY WATER A2.1 A b s o r p t i o n by a s t a t i o n a r y drop 107 A2.2 The d e s o r p t i o n o f a t h i n water l a y e r i n a c o n t a i n e r 108 A2.3 The release of carbon d i o x i d e from a bubble immersed i n an imsiturdfceid l i q u i d 109 REFERENCES 110 CHAPTER THE IMPORTANCE OF MELTING ICE Ity 1 CT.QUD ELECTRIFICATION 1.1. INTRODUCTION Many t h e o r i e s of the o r i g i n of the e l e c t r i c charges i n thunderclouds have been based on t h e o r e t i c a l and experimental work on t h e p r o p e r t i e s o f ice and water. CHAPMAN ( 1 9 5 3 ) , DRAKE (1968) and IRIBARNE and KLEMES (1970) have described experiments t o assess the importance o f some o f these c l o u d e l e c t r i f i c i a t i o n t h e o r i e s by a t t e m p t i n g t o c l o s e l y reproduce environment of p r e c i p i t a t i o n . the n a t u r a l DRAKE has shown t h a t f r o z e n water drops produce more e l e c t r i f i c a t i o n on m e l t i n g than would be expected from s t u d i e s o f blocks o f i c e . The present work attempts tocfevelop t h i s approach t o the l a b o r a t o r y study of cloud physics by t r y i n g t o estimate the importance o f m e l t i n g i c e i n convective cloud e l e c t r i f i c a t i o n . DINGER and GUNN (1946), MAGONO and KIKUCHI (1965), DRAKE (1968) and o t h e r s have r e p o r t e d f i n d i n g a p o s i t i v e charge o f approximately 1000 pC g * on t h e meltwater produced from chemically pure i c e . This e l e c t r i f i c a t i o n process i s of t h e c o r r e c t s i g n , and according t o DRAKE the c o r r e c t magnitude, t o be responsible f o r the c r e a t i o n o f the lower p o s i t i v e charge which i s o f t e n found near the 0°C l e v e l i n thunderclouds. M e l t i n g e l e c t r i f i c a t i o n may a l s o e x p l a i n why RAMSAY and CHALMERS (1960) and REITER (1965) have found t h a t p r e c i p i t a t i o n c u r r e n t changes from p o s i t i v e t o negative as steady r a i n t u r n s t o snow. I decided t o study the m e l t i n g o f small f r o z e n water d r o p s , t y p i c a l l y 4 mm i n d i a m e t e r , as they are of a s i z e o f t e n found i n convective c l o u d s . 1.2. THE THUNDERSTORM 1.2.1. One The thundercloud as a m e t e o r o l o g i c a l phenomenon o f the most comprehensive s t u d i e s o f the dynamics o f thunderclouds y e t undertaken was the American 'Thunderstorm P r o j e c t ' i n t h e l a t e 1940s. The r e p o r t o f the o b s e r v a t i o n s made i n F l o r i d a as p a r t o f t h i s p r o j e c t (BYERS and BRAHAM, 1948) has been taken as t h e basis o f a model ( 13 APR 1972 1972 n Lis,! J thunderstorm UJ CO in 4) (J) O S> \ to CO UQ to 0; E .* (J 00 UJ N <3 UJ 0 u Oo UJ 0 in 0 to to *0 u CD 4> 2. ever s i n c e . By measuring the d i s t r i b u t i o n o f r a i n f a l l and observing radar echoes BYERS and BRAHAM p i c k e d out c e l l s w i t h i n a thunderstorm system which were t y p i c a l l y 5 km across and contained an updraught and a downdraught. These c e l l s were observed t o pass t h r o u g h a w e l l d e f i n e d s e r i e s o f stages (Fig. 1,1) l a s t i n g a t o t a l o f 30 minutes t o one hour, s t a r t i n g from an a p p a r e n t l y o r d i n a r y cumulus cloud ( F i g . l a ) . Due t o a h i g h l e v e l o f v e r t i c a l i n s t a b i l i t y and a p l e n t i f u l supply o f moisture f l o w i n g i n t o t h e c l o u d , the growth becomes more r a p i d and more e x t e n s i v e then f o r an o r d i n a r y cumulus. When t h e downdraught i s s t a r t e d , t h e cloud p'asses i n t o the mature stage (Fig. the l b ) d u r i n g which most o f t h e l i g h t n i n g and p r e c i p i t a t i o n occur. Finally downdraught dominates and the cloud e n t e r s the d i s s i p a t i n g o r a n v i l stage (Fig. 1.1.c). An i m p o r t a n t f e a t u r e o f t h i s d e s c r i p t i o n o f the thundercloud i s the r o l e o f the p r e c i p i t a t i o n i n causing the downdraught which then tends to l i m i t the l i f e o f t h e c e l l . 1.2.2. C l a s s i f i c a t i o n o f thunderstorms Thunderstorms may be c l a s s i f i e d as heat or a i r mass storms and f r o n t a l storms, depending on how the i n i t i a l vigorous updraught was produced. convergence necessary t o s t a r t the Most heatthunderstorms occur i n the t r o p i c s c\-rC o v e r l a n d , e s p e c i a l l y over mountains. F r o n t a l thunderstorms^usually a s s o c i a t e d w i t h c o l d f r o n t s , and tend t o p e r s i s t f o r several hours as t h e y move w i t h t h e f r o n t , they are more f r e q u e n t near the coast and can occur over the oceans o u t s i d e the t r o p i c s ( A d m i r a l t y Weather Manual 1938). The a c t u a l size, s e v e r i t y and l i f e o f t h e storm does not depend on i t s t y p e , but r a t h e r on the t o t a l a v a i l a b l e energy, which w i l l be determined by the degree and v e r t i c a l e x t e n t o f u n s t a b l e a i r and the supply o f moisture from below the cloud. S i m i l a r l y the h e i g h t o f c l o u d base wiH be determined by t h e l o c a l m e t e o r o l o g i c a l v a r i a b l e s e s p e c i a l l y h u m i d i t y and w i l l be much g r e a t e r i n the c o o l d r y a i r o f t h e Alps than i n t h e warm moist a i r o f the t r o p i c s . Shaded Motion of s t o r m region Precipitotion /HAIL HA UPDR AUGHT Fig.1.2 A steady state convective s t o r m 77 (Browning,1964) - f \ / ir v e l o c i t y / / / Mot ion of-clou d / / •gl. 3 A schematic view in w h i c h t h e w i n d \ of a t h u n d e r s t o r m shearswith height in a n environment (Newton.1967 ) 3. 1.2.3. Severe thunderstorms There i s some evidence t h a t s e v e r e storms? o f t e n producing damaging h a i l , are a s s o c i a t e d w i t h s i n g l e c e l l s o r super c e l l s , which p e r s i s t f o r several hours. A f t e r s t u d y i n g a severe storm a t Wokingham i n 1959, BROWNING and LUDLAM (1962) d e s c r i b e d the e s s e n t i a l f e a t u r e o f the severe storm as being the s l o p i n g o f the updraught, e n a b l i n g the p r e c i p i t a t i o n t o f a l l c l e a r w i t h o u t f o r m i n g a dominating downdraught described by BYERS and BRAHAM (1948). as i n the storms New m o i s t a i r could then be drawn i n from t h e f r o n t o f the storm as i n F i g . 1.2, e n a b l i n g t h e thunderstorm t o p e r s i s t and dominate i t s environment. According t o NEWTON (1967) severe storms are most l i k e l y t o occur when there are bands o f s t r o n g winds f l o w i n g i n d i f f e r e n t d i r e c t i o n s .near the upper and lower l e v e l s o f the cloud ( F i g . 1.3). I f the storm moves w i t h the v e l o c i t y o f the a i r i n the mid-troposphere, t h e r e w i l l be a r e l a t i v e movement between the cloud and i t s environment near both i t s t o p and base. From an a n a l y s i s o f the f o r c e s i n v o l v e d NEWTON and NEWTON (1959) suggested t h a t w i t h modest v e r t i c a l motions a storm column could remain e r e c t w i t h r e l a t i v e h o r i z o n t a l motions between cloud and environment i n excess of 10 ms ^. I t i s probable t h a t w h i l e severe storms are not v e r y common, an a p p r e c i a b l e number o f thunderstorm c e l l s are i n c l i n e d t o the v e r t i c a l as the r e s u l t o f wind shear. From the D a i l y Weather Report and the A e r o l o g i c a l Record i t i s p o s s i b l e t o deduce values f o r the maximum r e l a t i v e v e l o c i t i e s between cloud and environment when thunderstorms are i n the r e g i o n o f the upper a i r wind sounding. 1-1- summarizes the r e s u l t s o f t h i s a n a l y s i s f o r the B r i t i s h d u r i n g p a r t o f the summer o f 1967. Table Isles From these few r e s u l t s i t seems t h a t an a p p r e c i a b l e f r a c t i o n o f B r i t i s h thunderstorms may have updraughts s l i g h t l y inclined to the v e r t i c a l . TABLE l . i Maxima r e l a t i v e v e l o c i t i e s between cloud and environment UP t o 10 km f o r summer storms over the B r i t i s h Relative velocity up t o 10 ms 9 from 10 t o 15 ms 1.3 Number o f thunderstorm days -1 more t h a n 15 ms Isles -1 11 -1 5 THE ELECTRICAL CHARGE DISTRIBUTION IN THUNDERSTORMS The c o n v e n t i o n a l p i c t u r e o f t h e thunderstorm having an upper p o s i t i v e and a lower n e g a t i v e charge i s supported by t h e work o f SIMPSON and SCRASE (1937) w i t h an a l t i e l e c t r o g r a p h and MALAN and SCHONLAND (1951) who measured p o t e n t i a l g r a d i e n t changes due t o l i g h t n i n g f l a s h e s . p o s i t i v e charge has o f t e n been observed near cloud A s u b s i d i a r y lower base- SIMPSON and SCRASE i n England, REYNOLDS and NEILL (1955) i n U.S.A. and KUETTNER (1950) i n t h e Alps suggest t h e n e g a t i v e charge i s l o c a l i s e d a t some temperature between -8° and -16°C depending on t h e h e i g h t o f t h e cloud base. However, measurements i n South A f r i c a by MALAN and SCHONLAND (1951) suggest t h a t the negative charge i s i n t h e f o r m of a column from the 0°C l e v e l up t o - 40°C. MALAN ( l 9 5 l ) has p o i n t e d o u t t h a t the South A f r i c a n storms were observed a t Johannesburg 1.8 km above sea l e v e l and were g e n e r a l l y i s o l a t e d cumulinimbi as opposed t o t h e E n g l i s h storms which were o f t e n of f r o n t a l o r i g i n and multicellular. However, t h e work o f OGAWA and BROOK (1969) has suggested t h a t the South A f r i c a n r e s u l t s exaggerate the v e r t i c a l e x t e n t of the negative charge because they were s i n g l e s t a t i o n ' o b s e r v a t i o n s o f e l e c t r i c f i e l d changes compared t o t h e m u l t i p l e s t a t i o n measurements o f REYNOLDS and NEILL and the v e r t i c a l dimension probed by t h e a l t i e l e c t r o g r a p h . 5. TABLE 1 .9 The magnitude and position of ttiemain charge centres i n thunderclouds Observer Positive charge SIMPSON and ROBINSON Negative height charge height 24C 6 km 20C 3 km GISH and WAIT (1950) 39G 9.5 km 39C 3 km MALAN (1952) 40C 10 km 40C 5 km (1940) T y p i c a l values o f t h e main charges i n thunderclouds are found i n 1 Table 1.2. They are of the same order as those destroyed i n s i n g l e l i g h t n i n g f l a s h e s a c c o r d i n g t o PIERCE (1955) and WORMELL (1939). 1.4 1.4.1 THE LOWER POSITIVE CHARGE The evidence f o r a lower p o s i t i v e charge SIMPSON and SCRASE (1937) found evidence f o r a l o c a l c o n c e n t r a t i o n o f p o s i t i v e charge i n t h e cloudbase o f some thunderstorms u s u a l l y i n f r o n t of the main r a i n area. T h i s lower p o s i t i v e charge has been observed by several other workers (Table 1.3) i n some b u t not a l l storms. Because of t h e nature o f t h e measurements and i t s r e l a t i v e size compared t o t h e main charge centres a lower p o s i t i v e charge may be present i n most thunderstorms but i s o n l y d e t e c t e d under favourable c o n d i t i o n s . From the r e s u l t s of SIMPSON and ROBINSON (1940) and MALAN (1952) i t would appear t h a t the s u b s i d i a r y charge i s about one q u a r t e r of t h e magnitude of t h e main charges. T a b l e t s a l s o i n d i c a t e s t h a t t h e v e r t i c a l p o s i t i o n o f t h e charge seems t o be independent o f temperature but u s u a l l y i t i s l o c a t e d i n t h e l o w e s t kilometre o f cloud. 7 Return stroke Post-return stroke > K— L [ Fig.1.4 Typical Intermediate electric field i Leader i changes at 5km ( C l a r e n c e and _ from adishorge to ground Malan,1957) Main l o c a t i o n of l o w e r p o s i t i v e c h a r g e Possible location of p o s i t i v e c h a r g e Rain sheet a n d Downdra u ght Fig.1.5 THE LOCATION OF THE LOWER POSITIVE ( W I L L I A M S , 19 5 8 ) CHARGE 6. TABLE 1.3 The l o c a t i o n of t h e lower p o s i t i v e charge POSITION S 0 ( J R C E REYNOLDS and NEILL (1955) New Mexico TEMPERATURE 1 km above cloud base -3 °C SIMPSON and ROBINSON ( l 9 4 l ) England 0.5 km " " +8 °C KUETTNER (1950) Zugspitze 0.5 km " » 0 °C MALAN (1952) Johannesburg MALAN and SCHONLAND (1951) MALAN and CLARENCE (1957)* cloud base Johannesburg " +5 °C 0.5 km below cloud base +8 °C 0.5 km +8 °C " " " Denotes t h a t t h e bottom of t h e charged r e g i o n was l o c a t e d . 1.4.2 The r o l e o f the lower p o s i t i v e charge i n the l i g h t n i n g discharge WHIPPLE (1938) suggested t h a t l i g h t n i n g i s not due t o an e x c e p t i o n a l l y l a r g e p o t e n t i a l d i f f e r e n c e between cloud and ground because i t i s p o s s i b l e t o have cloud-ground the c l o u d . l i g h t n i n g w i t h o u t p o i n t discharge under t h e a c t i v e p a r t of He a l s o t e n t a t i v e l y suggested t h a t l i g h t n i n g could be i n i t i a t e d by a b u i l d - u p of p o s i t i v e p o i n t discharge ions i n t h e base o f the c l o u d . CLARENCE and MALAN (1957) found evidence f o r t h i s process by studying the e l e c t r o s t a t i c f i e l d changes t h a t occurred before t h e f i r s t s t r o k e i n a lightning flash. Fig.1-4 shows t h e i n i t i a l breakdown stage (B) l a s t i n g up t o 10 ms which i s f o l l o w e d by an I n t e r m e d i a t e stage ( I ) l a s t i n g up t o 400 ms a f t e r which the leader and t h e r e t u r n stroke s t a r t the l i g h t n i n g proper. discharge A t h o r i z o n t a l d i s t a n c e s up t o 2 km from the discharge t h e B f i e l d changes were observed t o be negative w h i l e f o r d i s t a n c e s i n excess o f 5 km they were p o s i t i v e , and between 2 and 5 km t h e f i e l d changes were e q u a l l y l i k e l y t o be p o s i t i v e o r n e g a t i v e . initial CLARENCE and MALAN i n t e r p r e t e d t h i s breakdown as being due t o a discharge i n t h e cloud between a p o s i t i v e and a negative r e g i o n where t h e maximum f i e l d a t t h e ground due to these charges was l o c a t e d a t 2 km and 5 km from t h e discharge. Using SIMPSON's (1927) r e s u l t t h a t the maximum f i e l d a t t h e ground a t a h o r i z o n t a l d i s t a n c e D from the charge passes through a maximum when t h e 7. charge passes through a maximum when t h e charge i s a t a h e i g h t H where H = ^2 D CLARENCE and MALAN l o c a t e d t h e p o s i t i v e charge a t 1.4 km and the negative a t 3.6 km. These values agree w e l l w i t h t h e h e i g h t o f t h e cloud base and the lower r e g i o n o f t h e n e g a t i v e l y charged column found by MALAN and SCHONLAND ( l 9 5 l ) . These r e s u l t s s t r o n g l y suggest t h a t t h e lower p o s i t i v e charge plays an e s s e n t i a l p a r t i n t h e l i g h t n i n g discharge i n a t l e a s t some thunderstorms. 1.4.3 The l o c a t i o n of t h e lower p o s i t i v e charge WILLIAMS (1958) has compared t h e data i n Table 1.3 and has drawn up a model o f a thunderstorm c e l l ( F i g . 1.5) i n which the lower p o s i t i v e charge i s l o c a t e d i n t h e form o f a p r i s m 1 km wide on t h e boundary between the updraught and downdraught. He a l s o suggested t h a t t h e r e i s a r e g i o n o f p o s i t i v e charge on the r e a r side o f t h e downdraught. WILLIAMS found evidfeace f o r t h i s model by a n a l y s i n g t h e experiment o f FETERIS (1952) i n which a dense network o f ground observers r e p o r t e d the p o s i t i o n and time of occurrence o f every f l a s h t o ground from a s i n g l e c e l l whose radar echo had a maximum diameter o f 10 km. Assuming t h a t t h e lower p o s i t i v e charge was i n v o l v e d i n a l l t h e l i g h t n i n g f l a s h e s WILLIAMS used t h i s a n a l y s i s t o c o n f i r m the h o r i z o n t a l d i s t r i b u t i o n o f the lower p o s i t i v e charge i n h i s model, 1.5 1.5.1 THEORIES OF THE FORMATION OF THE LOWER POSITIVE CHARGE Melting p r e c i p i t a t i o n CHALMERS (1965) suggests t h r e e ways i n which the m e l t i n g o f s o l i d p r e c i p i t a t i o n may cause t h e charge s e p a r a t i o n necessary t o produce the lower p o s i t i v e charge. 1) The b u r s t i n g o f a i r bubbles trapped i n t h e i c e (1.5.3) 2) l a r g e snowflakes o r h a i l may m e l t t o form waterdrops which are so l a r g e t h a t t h e y break up. (1.5.4) 8, 3) when i c e and water are i n c o n t a c t the water may be p o s i t i v e l y charged, so any s p l a s h i n g , rubbing o r shaking o f f of water from t h e s u r f a c e o f a m e l t i n g p a r t i c l e w i l l cause charge s e p a r a t i o n . (1.5.5) 9 1.5.2 The evidence f o r s o l i d p r e c i p i t a t i o n i n thunderclouds While i t can probably be s t a t e d t h a t the m a j o r i t y o f thunderstorms i n temperate c l i m a t e s extend above the 0°C l e v e l and have p r e c i p i t a t i o n i n t h e ice phase, t h e r e i s a growing weight o f evidence f o r the e x i s t e n c e o f warm thunderstorms w i t h no i c e present a t a l l and whose p r e c i p i t a t i o n growth i s by t h e coalescence of water drops. FOSTER (1950), LANE-SMITH ( 1 9 6 9 ) , apd MICHNOWSKI (1963) have r e p o r t e d seeing l i g h t n i n g from clouds whose tops did not extend above the 0°C l e v e l . The A d m i r a l t y Weather Manual (1938) s t a t e s t h a t thunderstorms o f t e n occur i n Java w i t h tops below the summits of nearby mountains which are a l l l e s s than 3 km a l t i t u d e . t h a t the tops of clouds are v e r y close t o the C°C l e v e l . the This i m p l i e s However i n a l l thunderclouds where t h e lower p o s i t i v e charge has been found the cloud extended f o r s e v e r a l k i l o m e t e r s above t h e 0°C l e v e l and i t i s not p o s s i b l e to say whether t h i s charge i s present i n warm thunderstorms. 1•5•3 The a i r bubble t h e o r y o f the lower p o s i t i v e charge. The work of DINGER and GUNN (1946), MAC CREADY and PROUDFIT (1965a) and MAGONO and KIKUCHI (1965) provides s t r o n g evidence t h a t when i c e melts the meltwater acquires a p o s i t i v e charge o f the o r d e r o f 300 pC g ^ provided t h a t a i r bubbles are released from the i c e . DRAKE (1968) found t h a t when frozen water drops of 1 t o 6 mm i n diameter are melted i n an a i r s t r e a m vigorous convection may develop i n t h e meltwater and t h e e l e c t r i f i c a t i o n i s then enhanced by as much as an order o f magnitude. The p o s i t i v e l y charged m e l t i n g h a i l o r snow w i l l f a l l c l e a r o f t h e a i r which has become n e g a t i v e l y charged so producing a n e t p o s i t i v e charge below t h e 0°C l e v e l . e s t i m a t e d t h a t t h i s charging process could account f o r a p o s i t i v e DRAKE charge 9. d e n s i t y of 10 G km , which agrees w e l l w i t h t h e probable value of 8 C km c a l c u l a t e d by MASON (1957). There are several o b j e c t i o n s t o t h i s t h e o r y , the most i m p o r t a n t being t h a t i t i s v e r y s e n s i t i v e t o i o n i c i m p u r i t i e s and i t may be argued t h a t DRAKE considered water which was more pure than occurs i n n a t u r a l c l o u d s . I f t h i s c h a r g i n g process can be explained by t h e IRIBARNE and MASON (1967) theory o f b u b b l e - b u r s t i n g e l e c t r i f i c a t i o n , one would expect the spectrum of a i r bubble* sizes t h o o t r u o t u r o o f the ioo t o be an important f a c t o r . F i n a l l y i t i s not known whether v i g o r o u s c o n v e c t i o n would develop i n r e a l p r e c i p i t a t i o n f a l l i n g through a r e a l 1.5.4. atmosphere. The d r o p - s h a t t e r i n g mechanism I f l a r g e snowflakes o r h a i l s t o n e s melt t o form water drops which are l a r g e r than about 5 mm i n diameter the r e s u l t a n t raindrops w i l l break up as they gather speed under g r a v i t y . SIMPSON (1909) and CHAPMAN (1953) have found t h a t breaking water drops separate charge , w i t h the drops becoming p o s i t i v e l y and t h e a i r n e g a t i v e l y charged. The a c t u a l magnitude o f the charge depends on t h e s e v e r i t y of t h e s h a t t e r i n g process and according t o CHAPMAN can v a r y from 0.4 pC g * up t o 1000 pC g 1 where the r e l a t i v e v e l o c i t y of -1 drop and a i r s t r e a m are as much as 5 ms . CHAPMAN suggests t h a t i f t h e r e i s enough m i c r o t u r b u l e n c e i n t h e cloud t o give drops a momentary v e l o c i t y of 1 ms ^ r e l a t i v e t o t h e i r surroundings then charges of 100 pC per drop are possible. T h i s process could be important i n the t u r b u l e n t i n t e r f a c e between updraught and downdraught where WILLIAMS (1958) has l o c a t e d the lower p o s i t i v e charge i n thunderclouds. A f u r t h e r advantage of t h i s mechanism i s t h a t i t i s l e s s s e n s i t i v e t o i o n i c i m p u r i t i e s than t h e bubble b u r s t i n g t h e o r y . MATTHEWS and MASON (1964) have found t h a t when l a r g e drops are g e n t l y d i s r u p t e d i n an a i r s t r e a m , the e l e c t r i f i c a t i o n can be increased by a f a c t o r of a hundred t o 300 pC g ^ 4 by a p p l y i n g an e l e c t r i c f i e l d o f the order o f 3 x 10 V m "1 . As such a f i e l d would be expected i n a thundercloud t h i s process should be a c t i v e to some e x t e n t below the 0°C l e v e l . Cloud motion Negatively charged colu mn L o w e r p o s i t ii v e char ge \ 11 Point discharge * * .' ' "i E3 F i g .1.6 T h e point L i g h t n i n g flash t o g round Positive point d i s c h a r g e ions Rai n discharge origin ( M A L A N ,1 9 5 2 ) of the l o w e r positive charge 10* 1»5*4 The Ice-Water c o n t a c t theory 4 .. Because t h e m o b i l i t y o f protons exceeds t h a t ^ t h e h y d r o x y l ions i n i c e , and since f o r both ions t h e c o n c e n t r a t i o n i s h i g h e r i n w a t e r , t h e r e should be a tendency f o r t h e protons t o pass through t o t h e i c e more e a s i l y than the h y d r o x y l i o n s , thus making a t h i n f i l m o f meltwater n e g a t i v e l y charged. 2 TAKAHASHI (1969) found t h i s charge separation t o be about 1500 pC cm" which f o r a 4 mm i c e sphere corresponds t o 75 pC spread over t h e s u r f a c e . I f water i s shed d u r i n g t h e m e l t i n g process the m e l t i n g p a r t i c l e w i l l become p o s i t i v e l y charged. This mechanism could be i m p o r t a n t i n the e l e c t r i f i c a t i o n of m e l t i n g snowflakes, where a i r bubbles escape from a t h i n f i l m of water. 1.5.5. The p o i n t discharge t h e o r y WILLIAMS (1958) has p o i n t e d o u t t h a t t h e lower p o s i t i v e charge has been observed t o l i e i n t h e lowest k i l o m e t r e o f cloud and i t s l o c a t i o n does n o t seem t o be c o r r e l a t e d w i t h temperature. KUETTNER (1950) and REYNOLDS and NEILL (1955) l o c a t e d the charge a t o r above the 0°C l e v e l which does not a l l o w the t h e o r i e s i n v o l v i n g m e l t i n g ice t o be .a s a t i s f a c t o r y e x p l a n a t i o n , although it i s not easy t o estimate a c c u r a t e l y t h e temperature i n s i d e clouds. MALAN (1952) has suggested t h a t ions from p o i n t discharge may get caught i n t h e updraught below t h e thundercloud attachment ( F i g . 1.6) and become immobilised by t o cloud p a r t i c l e s i n t h e base o f t h e cloud. MALAN p o i n t s out t h a t most o f the l i g h t n i n g f l a s h e s t o ground i n Johannesburg seem t o take place t o t h e f r o n t o f t h e advancing storm where t h e p o i n t discharge are being caught i n t h e updraught* ions This t h e o r y has o n l y been e x p l a i n e d i n a q u a l i t a t i v e way but i t could e x p l a i n the anomaly o f t h e absence of an increase o f f i e l d measured by t h e a l t i - e l e c t r o g r a p h below thunderclouds* 1.6 Laboratory Assessment o f t h e Theories of t h e Formation o f the Lower P o s i t i v e Charge Three t h e o r i e s o f the lower p o s i t i v e charge have been o u t l i n e d , which i n v o l v e t h e e l e c t r i c surface o r bulk p r o p e r t i e s o f i c e and water. The choice 11. between these t h e o r i e s does n o t seem t o be determined by v e r i f y i n g these p a r t i c u l a r p r o p e r t i e s o f t h e water substance, b u t r a t h e r by a t t e m p t i n g to a s c e r t a i n whether the mechanisms i n which these p r o p e r t i e s are a c t i v e do i n f a c t occur i n t h e r e g i o n o f t h e lower p o s i t i v e charge. I t was t h e r e f o r e decided t o t r y and simulate as c l o s e l y as p o s s i b l e the c o n d i t i o n s present i n t h e thundercloud and a t the same time make the necessary e l e c t r i c a l measurements t o assess t h e importance o f m e l t i n g i c e i n the lower r e g i o n s of thunderclouds. 12. CHAPTER PREVIOUS STUDIES OF MELTING 2 ICE ELECTRIFICATION 9.1 EXPERIMENTS WITH BLOCKS OF ICE DINGER and GUNN (1946) melted 2-ml i c e blocks i n a warm a i r s t r e a m and found t h a t t h e meltwater acquired a p o s i t i v e charge of about 0.4 pC mg ^ i f the i c e was made from d i s t i l l e d water. The amount o f charge separated decreased r a p i d l y i f the m e l t i n g r a t e f e l l below 10 mg s ^ o r carbon d i o x i d e was d i s s o l v e d i n t h e i c e . Small q u a n t i t i e s o f i o n i c i m p u r i t i e s o f the o r d e r o f 20 mg 1 * were s u f f i c i e n t t o reduce the charging by a f a c t o r o f ten. DINGER and GUNN suggested t h a t t h e charge separation mechanism was r e l a t e d t o t h e escape o f a i r bubbles trapped i n t h e i c e and p o i n t e d o u t t h a t the r e d u c t i o n o f charging w i t h increased i m p u r i t y l e v e l s was s i m i l a r t o t h e behaviour o f t h e charge on a i r bubbles which had been i n v e s t i g a t e d by McTAGGART (1914) and ALTY (1926). MATTHEWS and MASON (1963) repeated Dinger and Gunn's experiment b u t f a i l e d t o f i n d any charging above 0.003 pC mg I n two l a t e r notes ^MATTHEWS and MASON(l9*4^^DINGER(1964) suggest t h a t t h i s n u l l r e s u l t might be caused by the presence o f a high c o n c e n t r a t i o n o f carbon d i o x i d e i n t h e l a b o r a t o r y , due t o the use o f d r y i c e . McCREADY and PROUDFIT (1965) also repeated t h e Dinger-Gunn experiment and found t h a t the m e l t w a t e r acquired 1 a p o s i t i v e charge o f about 0.02 pC mg" . ROGERS (1967) melted 15mm diameter i c e spheres, supported on an air j e t , and found t h a t t h e p a r t i a l l y melted spheres were n e g a t i v e l y charged i f water had been f l u n g o f f and p o s i t i v e l y charged o t h e r w i s e . 2.2. THE MELTING OF FROZEN WATER DROPS DRAKE (1968) c a r r i e d o u t a thorough study o f the e l e c t r i f i c a t i o n accompanying the m e l t i n g o f f r o z e n water drops over a wide range o f melting conditions. The i c e p a r t i c l e s were f r o z e n onto a 1mm loop o f 330 • o Many bubbles • No bubbles + A few bubbles Charge PC 120 o o 0° • o o 3o • • L o 0 ***** © o o<*> -•—r -V * p 10 Mass of sample IS g Fig.2.1 The e f f e c t o f air bubbles on melting electrification ( A f t e r K!KUCHI/I965a ) -t Charge -i pC mg 3*« -3 3* |t» for 4 10 -3 10-1 -I to A i r bubble c o n c e n t r a t i o n v o l u m e / volume Fig.2.2 The relationship b e t w e e n air bubble concentration and melting e l e c t r i f i c a t i o n 13. constantan w i r e amd melted i n a c o n t r o l l e d a i r s t r e a m . c o n v e c t i o n c u r r e n t s developed order o f magnitude. DRAKE found t h a t , when i n the m e l t w a t e r , the charging increased by an He also found t h a t carbon d i o x i d e o n l y i n h i b i t e d charging i f t h e r e was no convection i n t h e meltwater and t h a t h i g h c o n c e n t r a t i o n s A carbon d i o x i d e increased the c h a r g i n g . The a c t u a l amount o f charging depended on the r a t e o f heat f l o w t o the m e l t i n g i c e and on t h e f r e e z i n g temperature and p u r i t y o f the water. i m p u r i t y ions of l e s s than 2 mg 1 For water w i t h a c o n c e n t r a t i o n o f the charge separated l a y t y p i c a l l y between 1 and 2 pC mg ^. DRAKE found a good q u a l i t a t i v e argeement w i t h the amount o f e l e c t r i f i c a t i o n p r e d i c t e d by the a p p l i c a t i o n o f the IRIBARNE and MASON (1967) bubble e l e c t r i f i c a t i o n experiments melting i c e . bursting to the escape o f trapped a i r bubbles from the However, the enhancement o f e l e c t r i f i c a t i o n w i t h h i g h c o n c e n t r a t i o n s o f carbon d i o x i d e d i d not f i t t h i s t h e o r y . 2.3. THE BUBBLE-BURSTING THEORY OF MELTING ELECTRIFICATION 2.3.1 The evidence f o r an a i r bubble mechanism. KIKUCHI (1965a) showed t h a t blocks o f i c e made from d e i o n i z e d water d i d not become charged on m e l t i n g unless some a i r bubbles were present i n the i c e ( F i g . 2.1). The l e v e l o f charging was t y p i c a l l y two orders of magnitude les<= than t h a t found by DRAKE ( 1 9 6 8 ) , probably because o f the d i f f e r e n t m e l t i n g conditions. KIKUCHI also found t h a t the h i g h e r t h e c o n c e n t r a t i o n o f a i r bubbles trapped i n t h e i c e , the g r e a t e r the charging ( F i g . 2.2). I f large a i r bubbles o f about 1 mm diameter were p r e s e n t , the charging was reduced, suggesting t h a t t h e spectrum o f bubble s i z e s was also i m p o r t a n t . Although KIKUCHI estimated t h e mean charge on an a i r bubble t o be 3 x 10 pC, t h i s cannot be d i r e c t l y compared w i t h t h e r e s u l t o f the experiment o f IRIBARNE and MASON (1967) who s t u d i e d bubbles l a r g e r than 160 Jim compared t o the average diameter of 50 jim i n the i c e samples. This value f o r t h e charge Al R / / / 7 / / / / / / / / / / / / / '// ///ft ©0x-0©x;x-000 X-QQ0 @ © y © © y f © © © y * © @ © U n c o v e r e d ion it © © .2.3 Water dipole Hydroxy! ion P r o t on r Impurity cation X Impurity anion Schematic i l l u s t r a t i o n of t h e double layer ( After Alty,1926) 14. on an a i r bubble i s not i n c o n s i s t e n t w i t h the IRIBARNE and MASON experiments i f one assumes the main i o n i c i m p u r i t y t o be atmospheric carbon d i o x i d e d i s s o l v e d i n the i c e . 2*3.2. The E l e c t r i c a l double l a y e r a t an a i r - w a t e r i n t e r f a c e . The s e p a r a t i o n o f charge when a i r bubbles b u r s t a t a water surface and when water drops splash o r s h a t t e r may be e x p l a i n e d by t h e r u p t u r e o f an e l e c t r i c a l double l a y e r o f p o s i t i v e and negative charges a t t h e a i r - w a t e r interface. The e x i s t e n c e o f such a double l a y e r was f i r s t suggested by HELMHOLTZ (1879)> and i t s presence confirmed by t h e work o f McTAGGART (1914) and ALTY ( 1 9 2 6 ) , who s t u d i e d the motion o f a i r bubbles i n an e l e c t r i c field. By s t u d y i n g the way i n which t h e negative charge on a i r bubbles i n pure water v a r i e d w i t h bubble s i z e and p u r i t y o f the w a t e r , ALTY developed a t h e o r y d e s c r i b i n g the form o f the charges which made up t h e double l a y e r ( F i g . 2.3). ALTY said t h a t the p o l a r water molecules were o r i e n t a t e d i n a p r e f e r r e d d i r e c t i o n a t t h e a i r - w a t e r i n t e r f a c e , w i t h the p o s i t i v e end o f the d i p o l e s pointing into the l i q u i d . These surface molecules e l e c t r o s t a t i c a l l y a t t r a c t e d negative ions and o t h e r water molecules. I n very pure water w i t h a t y p i c a l -4 --J - ] c o n d u c t i v i t y o f 10 ohm m i m p u r i t y ions w i l l be present i n c o n c e n t r a t i o n s 7 8 of 1 i n 10 and i o n i z e d water molecules i n 1 i n 10 . Most o f the surface water d i p o l e s w i l l become covered w i t h a s t r i n g o f water molecules bonded t o them by hydrogen bonds. ALTY showed t h a t t h e i m p u r i t y n e g a t i v e ions were 7 8 a t t r a c t e d t o t h e surface i n c o n c e n t r a t i o n s of about 1 i n 10 t o 10 . This l a y e r o f n e g a t i v e ions then a t t r a c t e d i m p u r i t y p o s i t i v e i o n s and protons which formed a d i f f u s e space charge and which were more r e a d i l y removed by molecular c o l l i s i o n s and a i r escaping from t h e bubble. The a i r bubbles i n ALTY's experiment were n e g a t i v e l y charge because 10% of the n e g a t i v e ions were not covered by p o s i t i v e ions ( F i g . 2.3). CHALMERS and PASQUILL (1937) measured the p o t e n t i a l d i f f e r e n c e across a w a t e r - a i r i n t e r f a c e and found t h a t t h i s c o u l d be e x p l a i n e d by 1 i n 25 of t h e water d i p o l e s being o r i e n t a t e d p e r p e n d i c u l a r t o the s u r f a c e . They Bubble film — Film drops Jet Jet T h e bursting of a 1 5 mm a i r ( After Woodcock drops bubble et al. 1 9 5 3 ) .15. suggested t h a t i n r e a l i t y the water molecules are not a l l o r i e n t a t e d i n the same d i r e c t i o n as ALTY has suggested but on average tend t o produce the e f f e c t observed. 2.3.3. The mechanism o f bubble b u r s t i n g The b u r s t i n g o f a i r bubbles a t a water s u r f a c e haa been s t u d i e d w i t h a h i g h speed cine camera by WOODCOCK e t a l (1953). who obtained a s e r i e s o f photographs s i m i l a r t o F i g . 2.4. WOODCOCK found t h a t the b u r s t i n g process was s i m i l a r f o r bubbles w i t h diameters ranging from 0.2 t o 2 mm. I n stage 1 the bubble reaches t h e surface and then forms a r a i s e d cap o r f i l m 2). (stage This f i l m b u r s t s and may e j e c t a l a r g e number o f small d r o p l e t s c a l l e d f i l m drops (stage 3 ) . A small j e t forms a t the base o f the depression and grows r a p i d l y as t h e r a i s e d l i p subsides (stage 4)» The j e t becomes unstable and on r e a c h i n g i t s maximum h e i g h t e j e c t s t y p i c a l l y f i v e drops c a l l e d j e t drops (stage 5 ) . The t o t a l time taken from stages 1 t o 5 was o f the o r d e r of 2 ms. The diameter o f the j e t drops were found t o increase w i t h bubble size from 10 ^m f o r a 100 |im bubble t o lOQjtn f o r a 1mm diameter bubble. The* time taken f o r the f i l m d r o p l e t s t o form i s g e n e r a l l y a few microseconds and MASON (1954) using a microatscope slide technique has measured the diameters t o range from 0.4 t o 1.0 urn. DAY (1964) and BLANCHARD (1963) demonstrated t h a t t h e number o f f i l m drops produced f e l l o f f r a p i d l y from 100 f o r a 2 mm diameter bubble t o 10 f o r a 1mm bubble and l e s s than 1 f o r a 300 Jim bubble. BLANCHARD (1963) estimated the charge c a r r i e d by a f i l m drop t o be 3 e l e c t r o n charges per d r o p l e t from a b u r s t i n g bubble i n seawater 3 which i s a f a c t o r o f 10 l e s s than t h e charge c a r r i e d by a j e t drop from a s i m i l a r bubble. I t can t h e r e f o r e be assumed t h a t the maincharge t r a n s f e r mechanism a s s o c i a t e d w i t h a i r bubbles r e l e a s e d i n t h e m e l t i n g o f small p r e c i p i t a t i o n p a r t i c l e s w i l l be r e l a t e d t o the e j e c t i o n o f j e t drops. 2.3.4. Charge s e p a r a t i o n accompanying the b u r s t i n g of bubbles. BLANCHARD (1963) and IRIBARNE and MASON (1967) have found t h a t t h e d r o p l e t s e j e c t e d from b u r s t i n g bubbles are g e n e r a l l y n e g a t i v e l y charged f o r water w i t h i o n i c i m p u r i t y c o n c e n t r a t i o n s less than 1 0 ~ 4 N and 9 i n Molar g A = Thickness of double loyer Negat ive charge density pC mm 10 Molar B i O-OOl 0'0» o 0-1 d - D i s t a n c e from w a t e r surface Fig.2.5 Net c h a r g e f»m density between the s u r f a c e and a depth d ?7/A Negat ive charge F-f J Posit ive ch ar§e -r Fig.2.6a. Formation of a negatively charged jet — P ure w a t e r 7> ^ ; Flg.2.6b. Formation of a neutral j e t — Less pure water 16. p o s i t i v e l y charged f o r l e s s pure water, IRIBARNE and MASON e x p l a i n e d these r e s u l t s q u a l i t a t i v e l y by s t u d y i n g the behaviour o f the double l a y e r d u r i n g the f o r m a t i o n of the j e t drops* IRIBARNE and MASQN p o s t u l a t e d t h a t the j e t was composed o f the water nearest the surface of t h e a i r bubble, which had s l i d down the edge of t h e depression t o form a j e t a t t h e centre ( F i g . 2.4)- From photographs o f the f o r m a t i o n o f these j e t s , taken by WOODCOCK e t a l (1953) and NEWITT e t a l ( 1 9 5 4 ) , they estimated t h a t the volume of the j e t was about 1% of the volume of the bubble. They were then able t o c a l c u l a t e the depth d of the surface l a y e r which was needed t o make t h e j e t o f a bubble o f r a d i u s R. (Equation 2.1). I f the surface l a y e r down t o a d e p t h d i s m a i n l y the negative h a l f o f the d • double l a y e r then the j e t w i l l be n e g a t i v e l y charged (Fig- 2.6A). However? should d be g r e a t e r than the t h i c k n e s s of the complete double l a y e r then the j e t w i l l be n e u t r a l ( F i g . 2.6B)- So the t h i c k n e s s o f the double l a y e r w i l l govern the charge s e p a r a t i o n due t o bubble b u r s t i n g and the way t h i s charging v a r i e s w i t h bubble s i z e . 2.3.5. The e f f e c t o f i m p u r i t i e s on the t h i c k n e s s of the double l a y e r - By c o n s i d e r i n g t h e r a t e o f removal of the ions o f t h e double l a y e r from the e l e c t r o s t a t i c a t t r a c t i o n o f the surface water d i p o l e s * GOUY (1910) deduced an expression f o r the i n t e g r a t e d charge d e n s i t y Q- over the d i s t a n c e from t h e s u r f a c e t o a depth x (Equation 2.2)«T = (a D7C•* exp( 4 -P<^ x) where a and £ 2.2 are constants c o n t a i n i n g the gas constant and the p e r m i t t i v i t y o f a f r e e spaceD i s the d i e l e c t r i c constant o f water T i s the a b s o l u t e temperature c i s t h e gram molar c o n c e n t r a t i o n o f i o n i c i m p u r i t y . 10 Molar \ CHARGE: pc 8x10 Molar \ / 5x10 Moor / I 20 40 io too 0 BUBBLE Fig.2.7 DIAMETER H- m C h a r g e s e p a r a t e d by t h e Iribarne and b u r s t i n g o t bubbles Mason—theory 3 00 17. I n f i g - 2.5 o* i s p l o t t e d as a f u n c t i o n o f x f o r two c o n c e n t r a t i o n s o f i m p u r i t y , 10 M corresponding t o extremely pure d e i o n i z e d water and 10 M corresponding t o a t y p i c a l cloud water c o n c e n t r a t i o n o f 6 mgl o f sodium c h l o r i d e . The t h i c k n e s s o f the double l a y e r i s t h e d i s t a n c e from the water surface a t which cr , the i n t e g r a t e d charge d e n s i t y below t h e s u r f a c e f a l l s t o zero. I t can be seen from f i g . 2.5 t h a t a f a c t o r of 100 increase i n t h e i o n i c i m p u r i t y c o n c e n t r a t i o n causes a f a c t o r of 10 decrease i n t h e t h i c k n e s s of the double l a y e r . From equation 2 . 1 t h e t h i c k n e s s of t h e s u r f a c e l a y e r d which forms the j e t o f a 200 Jim diameter bubble i s 0.3 \xm and IRIBARNE and MASON observed t h a t bubbles o f t h i s diameter e j e c t j e t drops o f t o t a l charge -3 x 1 0 ~ pC f o r 1 0 ~ M s o l u t i o n s and + 3 x 1 0 ~ pC f o r 10** M. These observations agree q u a l i t a t i v e l y w'.th t h e above t h e o r y . 1 5 2 2.3.6 5 4 4 The dependence o f the charge separated by b u r s t i n g bubbles on the water p u r i t y and bubble r a d i u s . By combining equations 2.1 and 2.2, IRIBARNE and MASON deduced a r e l a t i o n s h i p between t h e t o t a l charge on t h e j e t drops (Q) and t h e water p u r i t y and bubble r a d i u s , ( e q u a t i o n 2»3)» Q = 2.9 x 1 0 9 2 R C^" exp (-£ - 1.1 x 1 0 7 c£ R) .... 2.3 where Q i s measured i n pC. Figure 2.7 i s a graph of t h i s equation? from which i t i s c l e a r t h a t f o r any i m p u r i t y c o n c e n t r a t i o n t h e r e should be a bubble diameter a t which the charge separated i s a maximum. These maxima should a l s o tend t o occur a t s m a l l e r bubble diameters as the water becomes l e s s pure. IRIBARNE and MASON found good agreement w i t h t h i s t h e o r y down t o 200 urn, t h e s m a l l e s t bubbles t h a t they s t u d i e d . A p o s s i b l e cause f o r t h e breakdown o f equation 2.3 f o r b , t a l e s o f l e s s than TOO^i-p diameter may be t h a t the volume o f the j e t may n o t be 1% of the volume of t h e bubble. This behaviour o f very small bubbles may be very i m p o r t a n t i n e x p l a i n i n g t h e e l e c t r i f i c a t i o n of m e l t i n g i c e as i c e samples o f t e n c o n t a i n many bubbles s m a l l e r than 50 \i m. 18. 2.3.7 The r e v e r s a l o f t h e s i g n o f ch-.rae pppa,T-at.ipn w i t h very impure water. I f t h e j e t i s made up o f both components of the double l a y e r t h e n according t o the above t h e o r y the j e t drops should be uncharged. However, IRIBARNE and MASON have suggested a mode o f charge s e p a r a t i o n which w i l l e x p l a i n t h e i r own and BLANCHARD's (1963) o b s e r v a t i o n s t h a t w i t h h i g h l e v e l s of i m p u r i t y the j e t drops are p o s i t i v e l y charged w i t h t y p i c a l l y 3 x 10 pC separated per bubble. As t h e j e t breaks up necks w i l l form between the b u l g e s , which e v e n t u a l l y form the d r o p s . Water w i l l tend t o f l o w o u t o f these necks i n t o the drops which are then e j e c t e d . Now the p o s i t i v e space charge o f t h e double l a y e r w i l l tend t o be d i s t r i b u t e d along the v e r t i c a l a x i s o f t h e j e t and so w i l l tend t o move out o f the necks f a s t e r than t h e negative p a r t o f the double l a y e r which i s r e s t r i c t e d by t h e surface. IRIBARNE and MASON a p p l i e d the theory o f t h e f l o w o f water i n a c a p i l l a r y tube t o t h e o u t f l o w of p o s i t i v e charge from the neck and o b t a i n e d an upper value f o r the charge s e p a r a t i o n o f 3 x 10 pC, which agrees w e l l w i t h t h e i r observations. 2.3.8 The release o f a i r bubbles by m e l t i n g i c e • When a water drop i s f r o z e n v i r t u a l l y a l l the d i s s o l v e d a i r i s r e l e a s e d as bubbles which are then trapped i n t h e i c e . On m e l t i n g these bubbles are l i b e r a t e d from the i c e and are p a r t l y absorbed by the meltwater before b u r s t i n g a t t h e water surface. Because the s o l u b i l i t y o f a i r i n water r a p i d l y decreases w i t h f a l l i n g temperature, a high p r o p o r t i o n of t h e bubbles w i l l reach the water surface and b u r s t . The amount o f a i r which would be released by the m e l t i n g o f a 4 mm diameter water drop f r o z e n a t - 10°C 3 would be about 0.45 mm • The i c e p a r t i c l e s melted by DRAKE (1968) and the author contained a i r bubbles ranging from 10 ^m up t o 400 ^m d i a m e t e r , 9 however DRAKE d i d not f i n d any n o t i c e a b l e c o r r e l a t i o n between bubble spectrum and the degree o f charging on m e l t i n g . He e x p l a i n e d t h i s by p o i n t i n g o u t t h a t t h e a i r bubble s t r u c t u r e changed d u r i n g t h e m e l t i n g process as some bubbles coalesced and o t h e r s d i s s o l v e d . Ex p e n m e n t -9—& T h e o r y + 10 Charge i—r 10 S"o too zoo k-oo Diameter Fig. 2 . 8 Hm The c h a r g e s e p a r a t e d by t h e bursting of bubbles -4 in a 3 * 5 x 1 0 Molar solution I r i b a r n e and Mason (1967) 19. 2.3,9 n f n The a p p l i c a t i o n of the bubble ^ r f i ^ . P H t K I T - m e l t i n g i c e electrification. DRAKE found t h a t the way i n which the charge separated by m e l t i n g i c e v a r i e d w i t h the .concentration o f i o n i c i m p u r i t i e s agreed w i t h t h e IRIBARNE 4 and MASON Ibubble b u r s t i n g t h e o r y f o r concentrations l e s s than 10 Mo The l e s s pure the water, the s m a l l e r the charge gained by the m e l t w a t e r . However the t h e o r y p r e d i c t e d t h a t the m e l t w a t e r should become n e g a t i v e l y < -4 ~ charged f o r i m p u r i t y c o n c e n t r a t i o n s g r e a t e r than 10 M„ DRAKE d i d not find this. I t i s suggested by the author t h a t the reason why DRAKE f a i l e d t o f i n d a r e v e r s a l i n the s i g n of charge separated was t h a t a t h i g h i m p u r i t y c o n c e n t r a t i o n s the charging o f small a i r bubbles i s more important than t h a t o f the l a r g e r bubbles. Figure 2.8 shows the v a r i a t i o n i n the charge c a r r i e d by the e j e c t e d drops as a f u n c t i o n o f bubble diameter f o r water 4 of p u r i t y 3.5 x 1 0 ~ M. Below 100 |im diameter the IRIBARNE and MASON t h e o r y p r e d i c t s t h a t the drops e j e c t e d w i l l be negative,so i n the m e l t i n g o f i c e the meltwater would be p o s i t i v e l y charged. F u r t h e r j the negative charge c a r r i e d by the drops from a 20 jim diameter bubble should be an order o f magnitude g r e a t e r than the p o s i t i v e charges from a 300^ bubble. So even the meltwater from i c e o f g r e a t e r than 10 ^ c o n c e n t r a t i o n of ions may be p o s i t i v e l y c h a r g e d bubbles smaller than 50 jim. 9 i f t h e r e are enough The range o f a i r bubble diameters i n the samples melted by DRAKE was 10 t o 400 |*m. Another possible disagreement between experiment and t h e o r y was the enhancement of e l e c t r i f i c a t i o n which was found by DRAKE f o r i c e w i t h high c o n c e n t r a t i o n s of carbon d i o x i d e . According t o t h e double l a y e r t h e o r y the carbon d i o x i d e should have i n h i b i t e d e l e c t r i f i c a t i o n * I t w i l l be suggested l a t e r i n t h i s t h e s i s t h a t the carbon d i o x i d e probably had escaped from the a i r bubbles before they b u r s t a t the s u r f a c e o f the meltwater. 20. 2.3.10 MgHpnrj ] r P e l e c t r i f i c a t i o n ^nd the s.pgs±£um_o_£ bubble s i z e s . The range o f a i r bubble diameters trapped i n the i c e samples of DRAKE and KIKUCHI (1965) was l O ^ m t o 400 ^m. From both t h e t h e o r y and experiments of IRIBARNE and MASON i t would be expected t h a t t h e charge separated by bubbles i n d i f f e r e n t p a r t s o f the bubble diameter spectrum would vary considerably w i t h the concentration of i m p u r i t i e s . The spectrum p r o b a b l y depends on the r a t e o f f r e e z i n g of the o r i g i n a l water and the size o f t h e water drops. Water drops f r o z e n i n an a i r stream w i l l f r e e z e much f a s t e r than i n s t i l l a i r . The s i z e d i s t r i b u t i o n o f a i r bubbles i n s o l i d p r e c i p i t a t i o n w i l l be h i g h l y i n f l u e n c e d by the c o n d i t i o n s under which the i c e p a r t i c l e s grow and w i l l be d i f f e r e n t f o r opaque and c l e a r h a i l . the F i n a l l y , the way i n which i c e m e l t s may a f f e c t t h e s i z e o f the a i r bubbles a c t u a l l y b u r s t i n g a t t h e s u r f a c e , as the r a t e s a t which they d i s s o l v e o r coalesce may be a l t e r e d . 2.4 FACTORS INFLUENCING THE CHARGING OF MELTING NATURAL ICE PARTICLES L a b o r a t o r y s t u d i e s o f m e l t i n g i c e and bubble b u r s t i n g e l e c t r i f i c a t i o n have r e v e a l e d s e v e r a l p r o p e r t i e s t h a t w i l l decide the amount o f c h a r g i n g produced i n t h e r e a l atmosphere by the m e l t i n g o f n a t u r a l p r e c i p i t a t i o n particles. I f one i s t o p r e d i c t t h e amount o f e l e c t r i f i c a t i o n produced by t h i s process, not o n l y must t h e i r e f f e c t on m e l t i n g i c e e l e c t r i f i c a t i o n be known, b u t t h e e x t e n t t o which c o n d i t i o n s i n clouds w i l l encourage appreciable e l e c t r i f i c a t i o n must also be d i s c o v e r e d . The p r i n c i p l e f a c t o r s i n f l u e n c i n g m e l t i n g i c e e l e c t r i c i c a t i o n are then 1) P u r i t y o f t h e water 2) M e l t i n g r a t e 3 ) A i r bubble s i z e spectrum 4) C r y s t a l s t r u c t u r e of t h e p a r t i c l e 5) The way i n which t h e m e l t i n g takes place e.g. does c o n v e c t i o n occur i n t h e meltwater? 21. CHAPTER 3 THE DESIGN OF A WIND TUNNEL. FOR THE FREE FLIGHT OF SMALL ICE SPHERES. 3.1. THE IMPORTANCE OF A FREE SUPPORT SYSTEM Some o f t h e v a r i a b l e s which i n f l u e n c e the amount o f charging occurring when i c e melts were l i s t e d i n s e c t i o n 2.4. I f an attempt i s t o be made t o draw conclusions about t h e e l e c t r i f i c a t i o n o f m e l t i n g s o l i d p r e c i p i t a t i o n from a l a b o r a t o r y experiment, probably the most important p r o p e r t y t h a t must be r e a l i s t i c a l l y reproduced i s t h e a i r f l o w around the p a r t i c l e . This a i r f l o w w i l l not o n l y i n f l u e n c e the development of convection i n t h e m e l t w a t e r , b u t a l s o t h e m e l t i n g process. I n t h e experiment o f DRAKE (1968), the i c e p a r t i c l e s were suspended from a loop of w i r e 1 mm i n diameter and so could be supported when the a i r f l o w was g r e a t l y d i f f e r e n t from t h e i r t e r m i n a l v e l o c i t y . Also the p a r t i c l e s were not f r e e t o r o t a t e and i f they had been f r e e , t h e onset o f convection i n t h e meltwater might not have occurred u n t i l much h i g h e r temperatures o r a i r f l o w r a t e s . Furthermore, i f # the p a r t i c l e s could be supported f r e e l y i n an a i r s t r e a m , then the e f f e c t o f the e l e c t r i c a l c o n t a c t between t h e support and t h e i c e p a r t i c l e could be assessed. I t was t h e r e f o r e decided t o t r y t o develop a method o f h o l d i n g an i c e p a r t i c l e i n a v e r t i c a l a i r s t r e a m away from any s o l i d boundaries. 3.2. THE PROBLEM OF TURBULENECE 3.2.1. The e f f e c t o f t u r b u l e n c e on a supported p a r t i c l e A l l methods of f r e e l y s u p p o r t i n g o b j e c t s i n v e r t i c a l a i r - s t r e a m s are based on the p r i n c i p l e t h a t , i f a i r moves upwards w i t h a speed equal t o the t e r m i n a l sppad o f t h e o b j e c t , then the upward drag f o r c e s on t h e suspended o b j e c t w i l l balance the downward g r a v i t a t i o n a l f o r c e . The c h i e f problem i n t h e design o f usable a i r support system i s the tendency o f the o b j e c t t o d r i f t t o t h e sides o f t h e t u n n e l . An i n d i c a t i o n o f t h e d i f f i c u l t y Direction of motion x is of rot at i on Fig.3.1 A rotating p r i s m at fluid C ONCAVE > (a) + + < CONVEX + High p r e s s u r e Low p r e s s u r e R e l a t i v e mo tions of adjacent s t r e a m l i n e s + b urface of discontinuity Fig.3-2 The f o r m a t i o n of e d d i e s 22. i s t h a t as t h e t e r m i n a l v e l o c i t y o f an i c e sphere of 4mm diameter i s 1 approximately 10 ms"" , a h o r i z o n t a l d r i f t o f o n l y 1% of t h e t e r m i n a l v e l o c i t y w i l l cause the sphere t o cross a 150 mm diameter t u n n e l i n li seconds. Even i f t h e r e i s no systematic cause of h o r i z o n t a l m o t i o n , any random movement of t h i s magnitude i s l i k e l y minutes. t o r e s u l t i n a chance c o l l i s i o n w i t h the sides w i t h i n I t i s t h e r e f o r e e s s e n t i a l t o design a wind t u n n e l which possesses a very low l e v e l of t u r b u l e n c e . 3,2*2* The a p p l i c a t i o n of B e r n o u l l i s theorum t o f l o w i n t u n n e l s Although s t r i c t l y concerned w i t h i n v i s c i d f l o w , B e r n o u l l i s theorem can be used t o describe t h e c o n d i t i o n s which lead t o laminar f l o w becoming t u r b u l e n t i n r e g i o n s away from t h e sides of the t u n n e l , where i n $ e r t i a l r a t h e r than viscous f o r c e s dominate. B e r n o u l l i ' s theorem can be expressed p t p constant »....*......«».•*«.**. 3.1 where p i s the s t a t i c pressure and p ^ and as the dynamic pressure 2 = i vv p 3.2 where v i s the a i r v e l o c i t y and p the a i r d e n s i t y . Equation 3.1 o n l y holds f o r d i f f e r e n t p o i n t s on the same streamline and i n general d i f f e r e n t s t r e a m l i n e s w i l l have d i f f e r e n t values o f the c o n s t a n t , corresponding t o d i f f e r e n t energy d e n s i t i e s . 3.2.3. Flow along curved streamlines. By c o n s i d e r i n g the t r a n s v e r s e a c c e l e r a t i o n of a curved s t r e a m l i n e one can d e r i v e a s i m i l a r expression t o equation 3.1of f l u i d the r o t a t i n g with radius r . Figure 3.1 shows a prism There w i l l be a pressure g r a d i e n t due t o motion o f the f l u i d , i n order, t o balance the c e n t r i f u g a l f o r c e . can be expressed as 2 ^ * = r where This h 3.3 os ds i s the side of the prism along the p r i n c i p a l normal. This i s the j u s t i f i c a t i o n f o r the p r i n c i p l e t h a t i f t h e f l o w i s along p a r a l l e l streaml i n e s then no pressure g r a d i e n t can e x i s t across the f l o w . So a h o r i z o n t a l pressure g r a d i e n t w i l l cause a i r t o f l o w t o t h e side of the wind t u n n e l . T Boundary layer 7—7-~l—/ Fig. 3-3 /*//////////// The definition of / boundary ^ Fig.3-4 The d e v e l o p m e n t a) Fig.3 5 Blunt f / / / / layer Direction of decreasing pressure of b o u n d a r y layer separation object b) S l e n d e r Boundary layer separation a t an o b s t a c l e object 23. 3 t2*,4,JeynQulU§ tteasmn and stidy. l&m&ism I f one considers a surface of d i s c o n t i n u i t y o r an area bounding r e g i o n s of f l u i d w i t h d i f f e r e n t v e l o c i t i e s , then i t i s p o s s i b l e t o chose a frame of r e f e r e n c e such t h a t t h e f l o w on one side o f t h e boundary i s i n the opposite d i r e c t i o n t o t h e f l o w on t h e o t h e r ( f i g . 3.2). I f a k i n k develops i n t h i s surface ( F i g . 3.2a), then e q u a t i o n 3.3. p r e d i c t s t h a t the pressure a t a convex surface w i l l be h i g h e r than a t a concave s u r f a c e . This means t h a t any i r r e g u l a r i t i e s which develop i n the s t r e a m l i n e s adjacent t o t h e boundary w i l l be u n s t a b l e and w i l l (Fig. 3.2b). tend t o get b i g g e r , causing the p r o d u c t i o n o f eddies This i s t h e reason why i n any low t u r b u l e n c e system t h e a i r f l o w must be as u n i f o r m as p o s s i b l e across t h e s e c t i o n . Two places a t which non- u n i f o r m f l o w can a r i s e are a t o b s t r u c t i o n s and bends i n t h e t u n n e l . 3.2.^. ,Ed^y,iarmat;on.^t t v n n e l wails, - Boundary j a y e r s e p a r a t i o n . Boundary l a y e r s e p a r a t i o n i s the p r i n c i p a l process by which t u r b u l e n t eddies are i n t r o d u c e d i n t o a wind t u n n e l e i t h e r from t h e sides o r from o b j e c t s placed i n the a i r s t r e a m . I t i s p o s s i b l e t o take i n t o account the drag o f an o b j e c t , due t o a f l u i d motion over i t s s u r f a c e , by assuming t h a t t h e f l u i d i n c o n t a c t w i t h the o b j e c t i s moving w i t h t h e v e l o c i t y of the surface of the o b j e c t . There w i l l be a v e l o c i t y g r a d i e n t i n t h e r e g i o n of the obstacle ( F i g . 3.3) and t h e boundary l a y e r i s d e f i n e d as t h e r e g i o n of f l u i d v e l o c i t y o f the f l u i d Fig. i n which t h e i s l e s s than 99% of i t s u n d i s t u r b e d v e l o c i t y 3.4 shows a s e r i e s of v e l o c i t y p r o f i l e s a t ( a ) , ( b ) and ( c ) near a f l u i d boundary where t h e r e i s a pressure g r a d i e n t opposing the motion of the f l u i d . As t h e f l u i d f l o w s along t h e boundary i t i s r e t a r d e d by the pressure g r a d i e n t and e v e n t u a l l y at A t h e d i r e c t i o n o f t h e f l o w near the boundary i s reversed. This reversed f l o w p i l e s up a g a i n s t the f l u i d moving i n t h e o r i g i n a l d i r e c t i o n and t h e s t r e a m l i n e s associated w i t h these f l o w s leave t h e boundary. T h i s i s c a l l e d boundary l a y e r s e p a r a t i o n and i t w i l l produce a surface o f d i s c o n t i n u i t y , AB S separating regions o f " f l u i d w i t h d i f f e r e n t v e l o c i t i e s and energy d e n s i t i e s . This surface w i l l be unstable and w i l l produce a t r a i n of eddies by t h e mechanism described i n Fig.3.2. I/) If) 0) cn O 0) N ] to 4> to 0) o T5 Do 2 iO C7) 0> Q to to CD to 0) T to 0) m cn cn to 24. ,The causes of boundary l a y e r s e p a r a t i o n Boundary l a y e r s e p a r a t i o n w i l l occur wherever there are l a r g e enought adverse pressure g r a d i e n t s near a f l u i d boundary t o l e v e r s e the f l o w . I n a d i v e r g e n t s e c t i o n o f t u n n e l , the angle o f divergence has t o be l i m i t e d t o p r e v e n t s e p a r a t i o n o c c u r r i n g a t the w a l l s . Another cause i s t h e pressure g r a d i e n t set up a t sharp bends, where equation 3,3 p r e d i c t s a pressure g r a d i e n t across the f l o w due t o c e n t r i f u g a l f o r c e s , so the f l u i d a t the o u t s i d e o f the bend v \ i l l be r e t a r d e d . I f o b j e c t s are placed i n the a i r s t r .a then an adverse pressure g r a d i e n t w i l l be s e t up at t h e r e a r o f t h e o b j e c t . The b l u n t e r t h e e x t r a c t i o n , tne more l i k e l y turbulence w i l l occur ( F i g . 3.5 3 ,b). 3.3. 3.3.1. LAMINAR FLOW WIND TUNNELS P r i n c i p l e s of o p e r a t i o n One o f t h e ways o f ensuring t h a t t h e f r e e l y supported particle stays away from the w a l l s i s t o reduce the turbulence t o such a l e v e l t h a t the p a r t i c l e remains i n t h e p o s i t i o n i n which i t was placed. Tunnels o f t h i s type have been d e s c r i b e d by CHAPMAN (1953), LIST (1959), and PRUPPACHER and NEIBURGER (1968). These t u n n e l s are a l l l a r g e r than 4m i n v e r t i c a l and r e q u i r e blowers from 4 t o 15 kW power r a t i n g . They have wide extent working s e c t i o n s of about 0»2m i n diameter and a great deal o f care has been taken to ensure t h a t t h e a i r f l o w i n the working s e c t i o n i s laminar. This i s achieved by the use o f honeycombs, gauzes and c o n t r a c t i o n s . 3 3„2.» The U n i v e r s i t y of C a l i f o r n i a Cloud Tunnel U The v e r t i c a l wind t u n n e l ( F i g . 3.6) described by PRUPPACHER and NEIBURGER (1968) was b u i l t f o r the study of f r e e l y supported s o l i d and l i q u i d p r e c i p i t a t i o n p a r t i c l e s . artificial I t i s a s e c t i o n t u n n e l powered by a 15 kW vacuum pump and u t i l i z e s several common methods of reducing turbulence. The c o o l i n g i s provided by t h r e e l a r g e r e f r i g e r a t i o n u n i t s and t h e h u m i d i t y o f t h e a i r f l o w can be a l t e r e d by the h u m i d i f i e r placed upstream of t h e plenum. Although i t was o b v i o u s l y out o f t h e question t o b u i l d such a system a t Durham w i t h the l i m i t e d f i n a n c e a v a i l a b l e some 25. of t h e techniques used t o smooth t h e a i r can be a p p l i e d t o t h e c o n s t r u c t i o n o f a s m a l l e r wind t u n n e l . 3.3.3 Methods o f reducing turbulence. The f i r s t a i r smoothing s e c t i o n i n F i g . 3.6 i s t h e plenum o r s t i l l i n g oL> chamber, which a c t s as a capacitance t o damp out o s c i l l a t i o n s . The a i r then passes i n t o a s e c t i o n c o n t a i n i n g a honeycomb and a s e r i e s o f gauze screens. Honeycombs reduce eddies by f o r c i n g t h e f l u i d i n t o pipes which are a p p r e c i a b l y narrower than the t u n n e l ; they also help t o keep the f l o w p a r a l l e l . Screens reduce d i f f e r e n c e s i n t h e l o n g i t u d i n a l v e l o c i t y across the s e c t i o n by p r o v i d i n g more r e s i s t a n c e t o t h e f a s t e r moving regions of the f l u i d . The l a s t a i r s m o o t h i n g s e c t i o n i n the C a l i f o r n i a t u n n e l i s the c o n t r a c t i o n where t h e cross s e c t i o n o f the a i r f l o w i s reduced and consequently the a i r i s ' accelerated. I f t h e c o n t r a c t i o n i s designed so t h a t the f a l l i n pressure experienced by each volume o f a i r i s the same and i f t h e f i n a l v e l o c i t y i s a p p r e c i a b l y h i g h e r than t h e i n i t i a l v e l o c i t y then t h e main f a c t o r governing the o u t l e t v e l o c i t y w i l l be the pressure drop across t h e c o n t r a c t i o n and n o t the d i s t r i b u t i o n of v e l o c i t i e s a t the i n l e t . I n the C a l i f o r n i a tunnel the r a t i o cf the i n l e t area t o o u t l e t area was 7:1. 3.3.4 S u c t i o n versus blowing Because the i m p e l l e r o f a blower creates considerable t y r b u l e n c e as w e l l as h e a t i n g the a i r s t r e a m , i t may be p r e f e r a b l e t o operate t h e t u n n e l i n the s u c t i o n mode. I n the C a l i f o r n i a t u n n e l a i r i s sucked through t h e 3 -1 system by a 15kW vacuum pump d e l i v e r i n g 0.2 m s of a i r , w i t h a pressure drop across t h e pump o f the order of 0.9 atmospheres. This l a r g e pressure drop appears t o have been necessary i n order t o place a sonic t h r o a t upstream o f t h e pump i n order t o stop d i s t u r b a n c e s t r a v e l l i n g upstream from the impeller. the pipe where t h e a i r f l o w s a t supersonic speed, i s described by PRANDTL (l952)» This method of using a sonic t h r o a t , which i s a r e g i o n of The c h i e f disadvantage of t h e s u c t i o n tunnels i s t h a t they have t o be c a r e f u l l y sealed i n o r d e r t o prevent a i r from l e a k i n g i n t o t h e system. Back pressure c a p S t a b l e support t o r particle E x i t screen Shaped gauze screen f Gauze screen Honeycom b Fig.3-7 A Blanchard-type tunne 11 Air speed rl ms 7- \ / P a r t i c l e stably supported So to _L_ Distance from side m m Fig.3-ff Velocity profile for Fig.3-7 ( C o t t o n and Gokhale, 1 9 6 7 ) O 26. 3,4. VELOCITY WELL SYSTEMS 3.4.1. P r i n c i p l e of o p e r a t i o n Several wind t u n n e l s have been made which support water drops by p l a c i n g them i n a r e g i o n where t h e v e l o c i t y d i s t r i b u t i o n o f t h e a i r f l o w i s i n the form of a w e l l . This g i v e s t h e drop a p o s i t i o n o f stable e q u i l i b r i u m . These t u n n e l s f a l l i n t o two t y p e s , e i t h e r t h e drop i s supported i n a d i v e r g e n t s e c t i o n o f t u n n e l e.g. GARNER and KENDRICK (1959) o r above t h e end of t h e t u n n e l as i n BLANCHARD (1950). These types of support have t h e advantage t h a t t h e a i r f l o w does n o t have t o be as smooth as i n t h e laminar f l o w systems. 3.4.2. 'Blanchard-tvoe' t u n n e l s The e s s e n t i a l f e a t u r e s of t h i s type o f wind tunnel are shown i n f i g u r e 3.7. Tunnels o f t h i s t y p e have been b u i l t by BLANCHARD (1950) KINZER and GUNN ( 1 9 5 1 ) , KOENIG (1965) and COTTON and GOKHALE (1967). The water drop tends t o s t a y a t the edge o f the bottom of the v e l o c i t y w e l l ( f i g . 3.8). by s p e c i a l l y shaped screen and t h e e x i t screen. This w e l l i s created The back pressure cap prevents t h e drop from f l y i n g o u t of t h e system and also a s s i s t s t h e a i r t o spread out on l e a v i n g the t o p o f the t u n n e l . I t i s e s s e n t i a l t h a t the v e l o c i t y p r o f i l e does n o t produce eddies due t o t h e e x i s t e n c e o f d i f f e r e n t v e r t i c a l velocities i n a d j a c e n t regions o f the a i r . According t o B e r n o u l l i ' s theorum the s'.des of t h e w a l l are unstable unless t o spread o u t . he a i r f l o w from the t u n n e l tends I f such a p r o f i l e were c r e a t e d i n s i d e a c y l i n d r i c a l tube eddies would f o r m a t t h e sides of t h e w e l l . I t i s n o t known t o what e x t e n t the success of t h i s type o f system i s due t o a b i l i t y o f waterdrops t o d i s t o r t when acted on by shear f o r c e s . These systems have never i n t h e author's knowledge been used t o s u p p o r t s o l i d o b j e c t s which c o u l d n o t r e a c t i n the- same way as l i q u i d drops a t t h e boundary o f t h e v e l o c i t y w e l l . BLANCHARD (1957) found t h a t i c e spheres could be supported f o r o n l y a few seconds. A f u r t h e r advantage o f water- drops i s t h a t they can be e a s i l y placed a t the s t a b l e p o s i t i o n by using a hyp©*dermic s y r i n g e . Location of water drop Shaped gauze screen* Screens mini "Honeycomb 5 0 m m- Fig.3-9 Typical divergent tube support t Ffg.3-10 The tapered ( Kinzer and Gu nn ) tube Fig/311 The air Jet ( Rog*rs,1967) 27. Wind t u n n e l s i n which the watersrop i s supported i n s i d e a d i v e r g e n t tube ( F i g . 3 . 9 ) , which contains a v e l o c i t y w e l l , have been b u i l t by GARNER and KENDRICK (1959) and IRIBARNE and KLEMES (1970), This method o f support has the advantage t h a t t h e water drop does n o t have t o be c a r e f u l l y placed i n the p o s i t i o n o f s t a b l e e q u i l i b r i u m ? bat can be allowed t o f a l l down the a x i s o f the d i v e r g e n t s e c t i o n and f i n d i t s own s t a b l e p o s i t i o n - Both t h e "Blanchardtype* and d i v e r g e n t tube supports have t u n n e l sections o f about 150 mm i n diameter and supported drops from 2mm up t o t h e maximum drop diameters o f about 6mnw 3.4.4 A i r l e t s and tapered tubes The t h i r d type o f f r e e support system does not r e q u i r e a h i g h l y smoothed a i r f l o w and u s u a l l y c o n s i s t s o f an a i r s t r e a m which i s o f a s i m i l a r diameter t o supported p a r t i c l e . Examples of t h i s method are the tapered tube o f KINZER and GUNN (1951) and t h e a i r j e t used by ROGERS (1967)* The tapered tube ( F i g . 3.10) i s s i m i l a r t o t h e rotameter method of measuring a i r f l o w r a t e , t h e water drop being kept away from the sides by t h e a i r r u s h i n g past* its axis. Great care must be taken t o make the tube symmetrical about ROGERS (1967) found t h a t water drops h i t the sides on f r e e z i n g and i t i s d o u b t f u l i f a non-symmetrical p a r t i c l e could be kept away from the sides of the tube* The p r i n c i p l e o f t h e a i r j e t i s not w e l l understood, b u t ROGERS found t h a t t h e nozzle diameter had t o be a f a c t o r o f 5 s m a l l e r t h a n t h e diameter of t h e supported i c e sphere. The j e t can support i r r e g u l a r o b j e c t s b u t n o t water drops and ROGERS found t h a t i c e spheres l a r g e r than 6mm i n diameter could be supported i n d e f i n i t e l y . He a l s o suggested t h a t s m a l l e r spheres could be supported i f the nozzle diameter were reduced. The a u t h o r t r i e d reducing t h e size o f t h e nozzle down t o 0.5 mm but found t h a t i t was n e a r l y impossible t o l o c a t e t h e a i r j e t and then place a small i c e sphere i n i t w i t h o u t a s o p h i s t i c a t e d alignment system. 5 V eloc ity pro t i l t Air Forces d u e to Y / » B e r n o u l l i s tthhceoorruum m \ / \7AVj 7/ v def l e c t e d by sphere R e s u l t a n t force on s p h e r e /a 'A (A) Fig.312 (B) Possible mechanisms for the air j e t Momentum system force (A) (A) Bernoulli force A LOW o UNIFORM VELOCITY ( B) Momentum to r c e ( B) FLOW GRADIENT Bernoulli LOW HIGH force i H»GH V e l o c i t y profile 1*5 I n c r e a s i n g p r e s s u r e velocity- Fig.313 D e f o r m a t i o n of w a t e r drops F i g . 314 Water drops a v e l o c i ty in well 28. 3.5. 3.5.1. THE DESIGN OF THE SUPPORT TUBE The gh^'.ce o f the type of support I n t h e preceding s e c t i o n t h r e e types of f r e e support system were discussed? namely t h e laminar f l o w , v e l o c i t y w e l l and the a i r j e t methods. The choice o f a system i s r e s t r i c t e d by the volume o f a i r i n the c o l d room and the l i m i t e d c o o l i n g capacity a v a i l a b l e . D u r i n g any s e n s i t i v e e l e c t r i c a l measurements the r e f r i g e r a t i n g compressor would have t o be switched o f f as i t caused t h e c o l d room t o v i b r a t e . The o p e r a t i o n o f the wind t u n n e l would cause appreciable UACW* due t o t h e compression o f a i r a t the blower"and t h e h e a t i n g o f the a i r i n the working system. So i f the temperature o f t h e a i r i n t h e r e g i o n o f the p a r t i c l e i s t o be k e p t c o n s t a n t over a 10minutes p e r i o d the e q u i v a l e n t o* zold room volume should n o t be c i r c u l a t e d f a s t e r t h a n about every t h r e e minutes. laminar f l o w wind t u n n e l s have had a diameter o f a t l e a s t 150 mm which Previous would mean t h a t a i r e q u i v a l e n t t o the volume o f the c o l d room woould be c i r c u l a t e d 1 every 18 s i f the a i r speed i n t h e working s e c t i o n was 10 m s " . KINZER and GUNN (1951) b u i l t a v e l o c i t y w e l l system w i t h a diameter o f 30 mm which suggests t h a t such systems can be more r e a d i l y designed w i t h small diameters than t h e low t u r b a t e n c e tunnels« Although a i r j e t s provide more s t a b l e support f o r ice spheres l a r g e r than 6 mm, i t i s c l e a r t h a t the f l o w round r e a l stones i s f a r c l o s e r t o t h a t i n v e l o c i t y w e l l systems. I n the hail- circumstances t h i s l a s t system seems t o be the best compromise. 3.5.2. Problems o f s u p p o r t i n g s o l i d particles. A l l the v e l o c i t y w e l l systems have been designed t o support water r a t h e r t h a n i c e spheres. drops BLANCHARD (1957) found t h a t ice spheres could be supported i n h i s wind t u n n e l f o r o n l y few seconds, whereas waterdrops could be supported i n d e f i n i t e l y p r o v i d i f t g t h a t - t h e r e , was no e v a p o r a t i o n . The a i r j e t w i l l however support s o l i d p a r t i c l e s . The mechanism of the a i r j e t i s sometimes e x p l a i n e d by B e r n o u l l i ' s theorem by saying t h a t because the v e l o c i t y a t t h e a x i s o f the j e t i s (greater than a t the edges, the a i r pressure i s l e a s t a t t h e c e n t r e (Fig.3.12) T h i s n e g l e c t s the f a c t t h a t the p a r t i c l e i s o f s i m i l a r s i z e t o the j e t and 29. the v e r t i c a l v e l o c i t y i n the centre beneath i t i s probably zero. An a l t e r n a t i v e e x p l a n a t i o n i s described i n F i g . 3.12B, i n which the a i r j e t i s d e f l e c t e d by the sphere and the change i n momentum of t h e a i r causes a f o r c e t o push the p a r t i c l e towards the centre o f the j e t . A. simple a p p l i c a t i o n o f B e r n o u l l i ' s theorem cannot be used t o e x p l a i n the v e l o c i t y w e l l systems as the f o r c e on the supported water drop should be d i r e c t e d towards the w a l l s o f the w e l l , where the a i r v e l o c i t y i s h i g h e r . However i t i s p o s s i b l e t o e x p l a i n why l i q u i d drops can be supported w h i l e s o l i d o b j e c t s cannot* by assuming t h a t the drop may be deformed by the f o r c e s a c t i n g on i t . I n a u n i f o r m a i r f l o w a water drop w i l l tend t o be deformed by the d i f f e r e n c e i n pressures a t the side and the bottom (SPILHAUS* 1947), see f i g u r e 3.13 A,B. According t o MASON (1957) t h i s deformation i s very small f o r diameters l e s s than 1mm. I f the drop i s i n a r e g i o n where the v e r t i c a l a i r speed increases across the d r o p , then the pressure d i s t r i b u t i o n w i l l be more complex, but i f one a p p l i e s B e r n o u l l i ' s theorem t o the a i r f l o w i n g over the s u r f a c e the d i s t r i b u t i o n i s probably s i m i l a r t o F i g . 3.13C. This pressure d i s t r i b u t i o n w i l l tend to cause a deformation which w i l l be i n c l i n e d to the v e r t i c a l ( F i g . 3.14). This w i l l have the e f f e c t of i n c r e a s i n g the f o r c e due t o the d e f l e c t i o n o f the a i r ( F i g . 14) and should help the water drop t o be kept wway from t h e boundary of the a i r f l o w . A solid particle w i l l not deform and so w i l l be e j e c t e d from the w e l l by the B e r n o u l l i f o r c e s (Fig. 3.14A). 3.5.3. P r e l i m i n a r y design c o n s i d e r a t i o n s In o r d e r t o l i m i t the r a t e a t which the cold room was heated up, the diameter o f t h e t u n n e l i n the r e g i o n where the p a r t i c l e would be supported (the working s e c t i o n ) , was r e s t r i c t e d t o 40 mm. A ssuming a maximum v e l o c i t y 1 i n t h i s s e c t i o n o f 10 ms" a volume o f a i r corresponding t o the c o l d room volume would be c i r c u l a t e d every 5 minutes. the As t h e blower a v a i l a b l e heated a i r by about 10°C, the a i r had t o be sucked through the t u n n e l r a t h e r than blown. This l i m i t e d the p o s s i b l e designs t o a d i v e r g e n t tube s i m i l a r to t h a t b u i l t by GARNER and LANE ( l 9 5 9 ) r a t h e r than the open t o p type used F i g . 3-15 The divergent tube working section -AI u m i n i u m Stable Most support probable of cone region location —\ particle Gauze cones 0 L Air flow j 30. BLANCHARD (1950). I n f a c t a t t h i s stage of t h e design t h e author was unaware of GARNER and LANE's work. 3.5,4, S t a b i l i t y i n t h e v e r t i c a l d i r e c t i o n I n a d i v e r g e n t tube wind t u n n e l t h e a i r speed f a l l s o f f towards t h e t o p of t h e tube so a t some h e i g h t i n the tube t h e p a r t i c l e i s supported by a i r f l o w i n g a t i t s t e r m i n a l speed. The degree o f s t a b i l i t y i s governed by the r e s t o r i n g f o r c e onthe p a r t i c l e which increases w i t h t h e angle o f divergence. However a l i m i t t o t h i s angle i s s e t by the p o s s i b i l i t y o f t h e f o r m a t i o n o f eddies due t o boundary l a y e r s e p a r a t i o n a t t h e d i v e r g e n t w a l l s . POPE and HARPER (1966) quoted t h e l a r g e s t angle between t h e tw> w a l l s f o r laminar f l o w as 8 ° , b u t say t h a t angles up t o 45° can be t o l e r a t e d provided t h e f l o w i s c a r e f u l l y guided round the c o r n e r . the I t was decided t o make t h e angle between w a l l s 12° i n order t o increase t h e damping and to study methods o f guiding the a i r into the divergent section. A f t e r experiments w i t h various flow-shaping devices i t was found t h a t two c o n c e n t r i c gauze conelets seemed to s t a b i l i z e the motion o f small p l a s t i c t n e spheres. The gauze used was 1 brass 'minimesh made by t h e Expanded Metal Company and had an open area o f 75$ and a s t r a n d t h i c k n e s s o f 0.13 mm. This design was very s i m i l a r t o t h e working s e c t i o n t h a t was f i n a l l y used ( F i g . 3.15). 3.5.$ S t a f r i U t Y jn a h o r i z o n t a l plane The d i v e r g e n t tube was i n s t a l l e d above a smoothing s e c t i o n c o n s i s t i n g of a honeycomb and a gauze screen and was connected t o a small 150 W blower. I n i t i a l l y t h i s p i l o t t u n n e l was operated a t room temperature and p l a s t i c i n e b a l l s were used t o t e s t v a r i o u s m o d i f i c a t i o n s aimed a t i n c r e a s i n g the s t a b i l i t y of the p a r t i c l e . The problem o f keeping t h e p a r t i c l e away from the w a l l s was o n l y p a r t l y solved and attempts t o create a v e l o c i t y w e l l i n the c e n t r e o f t h e tube by p l a c i n g screens below the gauze flow-shaping cones did n o t stop t h e b a l l s from r a t t l i n g around the bottom o f t h e support t u b e . However, i t was found t h a t i f t h e gauze cones were a l i g n e d so t h a t t h e i r sides were p a r a l l e l t o the upper aluminium cone, then t h e b a l l s tended t o hover around the t o p of the gauze cones. The b a l l could be dropped from t h e 31. top of the aluminium cone and would stay i n the shaded r e g i o n of F i g . 3.16. The p a r t i c l e showed a d e f i n i t e preference f o r s t a y i n g i n the h e a v i l y shaded r e g i o n shown i n the diagram. A t t h i s stage the main d i f f i c u l t y i n improving the system was t h a t t h e a i r f l o w e n t e r i n g the working s e c t i o n was probably not very smooth. So i t was decided t o b u i l d a more permanent wind t u n n e l i n s i d e the c o l d room. 3.5.6. A i r smoothing i n t h e main wind t u n n e l The a i r was f i r s t passed through a 150 mm long honeycomb w i t h a 10 mm g r i d . The next stage was a mesh screen w i t h holes 1.5 mm x 1.0 mm and f i n a l l y the t u n n e l was c o n t r a c t e d from a diameter o f 75 mm t o 30 mm. operated i n t h e sucking mode. The blower was also I d e a l l y s e v e r a l screens should have been placed between the honeycomb and t h e f i n a l screen but t h e r e was not enough space. U n f o r t u n a t e l y the t u n n e l had 2 r i g h t - a n g l e bends j u s t upstream of the honeycomb and these should have been replaced w i t h a s e t t l i n g chamber i f the turbulence i n the working s e c t i o n were t o be reduced 3.5.7 The performance Ice further. o f the support system spheres from 2 t o 5 mm diameter were supported i n a very s i m i l a r way t o the p l a s t i c i n e b a l l s . A f t e r about 10 t o 30 minutes f l i g h t they would crash i n t o t h e w i r e s vh i c h supported the gauze cones and so g e t caught. They would go very near t h e sides every 2 t o 3 minutes and i t i s probable t h a t they made c o n t a c t w i t h the w a l l s i n the 5 seconds t h a t elapsed before they moved away. The motion was d i s t i n c t l y d i f f e r e n t from t h a t i n t h e e a r l y attempts at keeping the b a l l s away from the sides o f the t u n n e l and t h e r e was a very marked tendency t o hover around the t o p o f the gauze cones. 1> 0) \ s \ s s Q UJ S s UJ IQ D 32. CHAPTER 4 THE CONSTRUCTION AND INSTRUMENTATION OF THE WIND TUNNEL 4.1. THE ADAPTATION OF THE COLD ROOM 4.1.1 The p r e p a r a t o r y of the c o l d room To study the support o f i c e spheres» t h e t u n n e l was placed i n s i d e a c o l d room. The c o l d room a v a i l a b l e was f o r m e r l y a butcher's c o l d s t o r e , powered by a 300 W compressor, which was capable o f h o l d i n g a temperature o f 30°C 3 below the ambient temperature. and the i n s u l a t i o n c o n s i s t e d polystyrene The t o t a l volume of the cold room was 4m o f 113 mm of cork and 55 mm o f expanded ( F i g . 4.1). The w a l l s and f l o o r were h e a v i l y engrained w i t h d i r t so the room was e x t e n s i v e l y r e f i t t e d . and used as a foundation A new concrete f l o o r was l a i d f o r a f a l s e f l o o r made of 15 mm plywood l y i n g on a wooden frame which was f i l l e d w i t h expanded polystyrene ( F i g , 4.1 )* The plywood f l o o r was then covered w i t h a 6 mm rubber sheet which made a watert i g h t j o i n t w i t h t h e w a l l s t o prevent water seepage during d e f r o s t i n g . The surfaces o f t h e i n s i d e w a l l s and roof were removed w i t h sandpaper and were f i n a l l y cleaned w i t h d e t e r g e n t t o remove a l l traces of grease and f a t . F i n a l l y the i n s i d e o f t h e c o l d room was covered w i t h 3 coats of polyurethane p a i n t which formed an i n e r t seal t o the w a l l s . A new d e f r o s t i n g t r a y capable of h o l d i n g about 20 l i t r e s of water was f i t t e d below the c o o l i n g coils. 4.1.2 The window Because o f t h e l i m i t e d space a v i l a b l e i n s i d e t h e cold room t h e experiments were performed from the outside , using a double glazed window f i t t e d w i t h glove ports'. As the window would be an important heat l o s s i t was made as small as p o s s i b l e . source o f The window was placed on the i n s i d e w a l l s t o enable the o p e r a t o r t o reach as f a r i n t o t h e c o l d room as possible ( F i g . 4.2).. PROBERT and HUB (1968) suggest t h a t 12 mm i s the optimum thickness of about 30°C. o f a double glazed window f o r a temperature d i f f e r e n c e I f the gap i s g r e a t e r convection tends t o b u i l d up, reducing t h e advantage o f the e x t r a t h i c k n e s s . 12.5 mm perspex w i t h a s i m i l a r thickness The two panes were made o f of a i r gap. The windows were Brass Tubt J L — Flfxible Tube lh Fl o w m e t e r 60W Lamp M i rror Perspex H u m i di t y tube Hatch measurement Faraday T o Wowed Working cage section Aluminium cones Thermocouple i Gauze Heater f Fig.4.3 screen A b s o l u t e filter Steel wool Vertical Honeycomb filter s e c t i o n of wind tunnel probe 33, sealed w i t h perspex cement and p a i n t and never misted upon t h e i n s i d e , a l t h o u g h on very c o l d days condensation sometimes formed on:theuouter pane. The glove p o r t s were never f i t t e d w i t h gloves as these would r e s t r i c t the o p e r a t o r ' s ease o f movement and as most o p e r a t i o n s o n l y took a few seconds no a p p r e c i a b l e heat l o s s was caused. When n o t i n use the glove p o r t s were f i l l e d w i t h expanded p o l y s t y r e n e stoppers* 4.1.3 E l e c t r i c a l connections t o t h e c o l d room I t soom became apparent t h a t a l a r g e number o f wires would have t o pass i n t o t h e c o l d room t o enable the wind t u n n e l t o be instrumented. I n the e a r l y stages o f experiments when t h e c i r c u i t y would have t o be c o n s t a n t l y m o d i f i e d t h e r e was an obvious need f o r i n t e r c o n n e c t i n g plugboards on t h e i n s i d e and o u t s i d e o f t h e c o l d room. s i x t e e n 4 mm sockets. sockets. These were b u i l t and f i t t e d w i t h The i n s i d e board was also equipped w i t h mains Two 12-way cables and several mains and c o a x i a l leads were r u n through the w a l l s ; these were a l l used i n the next two years. 4.2. THE WIND TUNNEL 4.2.1. L i m i t a t i o n s on d e s i g n due t o the cold room U n f o r t u n a t e l y the window was f i t t e d t o the c o l d room before t h e wind t u n n e l was designed and i t soom became apparent t h a t t h e window was mounted too low. I d e a l l y as l a r g e a length of s t r a i g h t p i p i n g as p o s s i b l e was r e q u i r e d upstream of the working s e c t i o n , but t h i s was l i m i t e d t o about 0-6 m by the h e i g h t o f the c o l d room f l o o r and windows. This s t r a i g h t s e c t i o n c o n t a i n e d a honeycomb, a gauze screen and a c o n t r a c t i o n but a bend had t o be made i n t h e t u n n e l t o enable a heater t o be placed i n the a i r stream. The blower had t o be mounted a t ground l e v e l t o minimize v i b r a t i o n s so another bend was r e q u i r e d downstream o f t h e working s e c t i o n . The wind tunnel as f i n a l l y b u i l t was about 7 m i n t o t a l l e n g t h and i n c l u d e d two 180° bends ( F i g . 4.3). 4.2.2 The blower The blower used was a Siemens 0.7 kW 3-phase blower capable o f a maximum volume f l o w r a t e o f 35 fts and a maximum pressure drop across he blower e q u i v a l e n t t o 1.1m of water. The blower was used t o suck 0) 1/1 U1 to 0) (1) DO \ in N or S 1 t I 0) 0) CT t- 34. a i r t h r o u g h t h e working s e c t i o n a t a maximum a i r v e l o c i t y o f 20 ms * i n t h e 31 mm diameter s e c t i o n , which corresponds t o 20i s the 1 o f a i r . The a i r l e a v i n g blower was heated by about 10°C depending on t h e a i r f l o w r a t e , so t h e o u t l e t from t h e blower was d i r e c t e d over t h e c o o l i n g c o i l s t o h e l p m a i n t a i n the of temperature of t h e c o l d room. The blower was b o l t e d t o t h e c o n c r e t e cap a b r i c k p i l l a r and t h e v i b r a t i o n produced was n e g l i g i b l e . For s a f e t y reasons t h e blower was l o c a t e d o u t s i d e the c o l d room but i t was found t h a t provided t h e pipes were w e l l lagged t h e heat losses were small compared to t h e compression h e a t i n g o f t h e blower. &»2sl^ ftlrflgw c o n t r o l - The a i r f l o w was r e g u l a t e d by a b u t t e r f l y valve l o c a t e d i n a bypass p i p e which met the main t u n n e l a t the i n l e t t o t h e blower ( F i g . 4#4) The valve was connected t o an e l e c t r i c motor and c o u l d be operated from the main c o n t r o l panel o r a t the valve i t s e l f . This method proved adequate and t h e a i r v e l o c i t y could be r e g u l a t e d t o b e t t e r than 0.5 ms *• 4.2.4.. The wind t u n n e l l a y o u t The l a y o u t o f the wind t u n n e l i s shown i n f i g u r e s 4.3 and 4.4. was o n l y space f o r two a i r f l o w smoothing of square tubes o f 10 mm side and a t o t a l screen. section. stages, the honeycomb which c o n s i s t e d , l e n g t h o f 150 mm, and a minimesh The h e a t e r , which was a h e a t i n g element from a water b o i l e r 3 Could A l l t h e brass s e c t i o n s between the h e a t e r and the working s e c t i o n were lagged w i t h a 50 W h e a t i n g t a p e , which thermal time constant o f t h e system. reduced The a i r i n t h e working s e c t i o n could then be r a i s e d from -8°G t o + 10°G i n about 4 minutes. The p a r t i c l e i n the\ working s e c t i o n was viewed by the use o f a 50 mm diameter m i r r o r which also served t o s h i e l d %he i c e from t h e d i r e c t r a d i a t i o n o f t h e 60 W lamp which was used t o i l l u m i n a t e t h e working section. f I t was n o t p o s s i b l e t o place any screens downwind o f the working be operated a t up t o 200 watts* the There The..heating e f f e c t o f t h e lamp was found t o be l e s s t h a n 0.2°C« The i c e spheres used i n t h e f r e e f l i g h t experiment were i n s e r t e d i n t o t h e t u n n e l t h r o u g h t h e hatchway which was placed j u s t below t h e m i r r o r . 35. 4.2.5. C o n s t r u c t i o n d e t a i l s To enable as many as p o s s i b l e of the p a r t s t o be interchangeable most o f t h e s e c t i o n s were made from 75 mm diameter t u b i n g f i t t e d w i t h 110 mm f l a n g e s w i t h standard holes f o r the securing b o l t s . The whole t u n n e l was b u i l t around a 'Handyangle' frame which was b o l t e d t o the f l o o r o f the cold room. of The t u n n e l sections were connected t o the frame by means o f sheets aluminium f i t t e d w i t h a 75 mm hole and b o l t h o l e s t o match the f l a n g e s . The Faraday cage was made from sheets o f aluminium. The f l e x i b l e t u b i n g was manufactured from neoprene impregnated f i b r e g l a s s on top o f a galvanized screen s p r i n g and the maximum leakage quoted by the manufactuers was 0.1% of the volume f l o w r a t e per metre o f pipe under c o n d i t i o n s t y p i c a l o f i t s use i n the wind t u n n e l . The f l e x i b l e t u b i n g was c a r e f u l l y sealed t o the brass flanges by means o f P-V.C. tape and adhesive and some s e c t i o n s were f i t t e d w i t h rubber gaskets t o reduce the leakage. 4.3, MEASUREMENT OF ELECTRIC CHARGE 4.3.1 The p r i n c i p l e o f measurement• The two aluminium cones ( F i g . 4.3) i n s i d e the Faraday cage were i n s u l a t e d from e a r t h a t both ends and were connected by means o f a low noise c o a x i a l cable t o a v i b r a t i n g reed e l e c t r o m e t e r (V.R.E), I f there i s a charge separation process i n s i d e the upper cone w i t h one sign being r e t a i n e d on an ice p a r t i c l e i n t h e cone and the opposite s i g n being c a r r i e d away i n the airstreamj the Cones w i l l a c t as a Faraday p a i l and a charge equal t o t h a t c a r r i e d by the i c e p a r t i c l e w i l l b e induced onto the o u t s i d e of the cones 12 and w i l l f l o w t o e a r t h through the 10 meter. ohm i n p u t r e s i s t o r o f t h e e l e c t r o - The e l e c t r o m e t e r w i l l t h e r e f o r e measure the charge s e p a r a t i o n c u r r e n t i f t h e value o f the imput r e s i s t o r i s known. The main a m p l i f i e r of t h e V.R.E. was c a l i b r a t e d by a p p l y i n g an a c c u r a t e l y known voltage t o i t s i n p u t stage. The i n p u t r e s i s t o r was checked t o + 10% by passing a known c u r r e n t through i t and n o t i n g the voltage i n d i c a t e d by t h e o u t p u t meter on the V.R.E. the The background noise l e v e l was found t o depend l a r g e l y on design o f the i n s u l a t i o n and the space charge c a r r i e d by the a i r i n the wind t u n n e l . 7 a uze 1 3 Absol ute 3 filter 3 3 7 Brass tube Fig.4.6 The space charge filter Pe r s p e x n A) An early f o r m 1 of 1 1 S*" insulator Perspex kO mm P.T.F.E. P.T.F.E. T a p e 8) Fig4.5 The f i n a l d e s i g n The design of insulators 36, 4 * 3 , 2 * The p e r f o r m a n c e o f d i f f e r e n t t r Y P fis n f insulators The i n s u l a t o r s were d e v e l o p e d by s t u d y i n g t h e i r p e r f o r m a n c e i n t h e w i n d t u n n e l i n w h i c h t h e a i r was blown t h r o u g h t h e t u n n e l . ( F i g . 4 . 5 A ) c o n s i s t e d o f two p e r s p e x perspex spacers. The f i r s t pilot design r i n g s s e p a r a t e d by f o u r 4 mm d i a m e t e r When t h e a i r s t r e a m was h e a t e d or allowed to cool after h e a t i n g , t h e V . R . E . w o u l d r e c o r d a n o i s e l e v e l o f up t o 0 . 2 pA w h i c h was suspected t o be due t o t h e i n s u l a t o r s - these n o i s y p e r i o d s o f r e c o r d . A l a t e r design ( F i g . 4«5B) e l i m i n a t e d The c h i e f m o d i f i c a t i o n was t o move t h e away f r o m t h e a i r s t r e a m and r e p l a c e t h e p e r s p e x w i t h P . T . F . E . a t t h e t i m e t h a t t h e n o i s e may have been caused by metal water spacers I t was t h o u g h t condensing, on t h e s i d e s o f t h e t u n n e l and b e i n g f o r c e d o v e r t h e i n s u l a t i n g a i r g a p . This seems an u n l i k e l y e x p l a n a t i o n as t h e dew p o i n t o f t h e a i r was u s u a l l y l o w e r than t h e p r o b a b l e t e m p e r a t u r e of the t u n n e l w a l l s * When used i n t h e m a i n t u n n e l t h e i n s u l a t o r s were s e a l e d with P.T.F.E. tape and s i l i c o n e r u b b e r t o p r e v e n t a i r l e a k s due t o s u c t i o n t h r o u g h t h e a i r gap. A l l the surfaces detergent and hexane b e f o r e use 4 . 3 . 3 . N o i s e due t o space o f t h e i n s u l a t o r s were c a r e f u l l y c l e a n e d with t o remove any g r e a s e . charge 3 "^l Because a p p r o x i m a t e l y 0 . 0 1 m s" o f a i r passed t h r o u g h t h e t u n n e l one might expect t h a t t h e w o r k i n g s e c t i o n may behave as a crude space collector despite t h e e a r t h e d gauze s c r e e n u p w i n d . f i l t e r was p l a c e B e f o r e a space i n t h e a i r s t r e a m , t h e c u r r e n t measured c o u l d on some o c c a s i o n s charge by t h e be a t t r i b u t e d t o space c h a r g e , e . g . charge V.R.E. the noise that o c c u r r e d when t h e h e a t e r was used a f t e r a l o n g p e r i o d o f n o t b e i n g u s e d . The most d r a m a t i c e v i d e n c e f o r t h e e f f e c t o f space charge o c c u r r e d when a n e a r b y b u i l d i n g was b e i n g d e m o l i s h e d and c l o u d s o f d u s t e n t e r e d laboratory. enter When t h e c o l d room d o o r was opened and t h e d u s t a l l o w e d t o the wind t u n n e l , t h e V . R . E . r e g i s t e r e d which f e l l the a maximum c u r r e n t ' o f 0.4pA back t o z e r o a b o u t 1 0 m i n u t e s a f t e r t h e door was s h u t . space charge filter A ( F i g . 4 . 3 ) was t h e n i n s t a l l e d p e r m a n e n t l y i n the w i n d 37. tunnelT h i s c o n s i s t e d ( F i g . 4 . 6 ) o f a s t e e l wool f i l t e r f o l l o w e d by a f i b r e g l a s s a b s o l u t e f i l t e r o f t h e t y p e used by BENT (1964) as. a *pmfliter f o r a space c h a r g e c o l l e c t o r . W i t h t h i s f i l t e r i n s t a l l e d t h e r e was no s i g n i f i c a n t V . R . E . d e f l e c t i o n when t h e door o f t h e c o l d room was l e f t o p e n , so i t was assumed t h a t t h e f i l t e r w o u l d be c o m p l e t e l y e f f e c t i v e under n o r m a l operating conditions* 4»3 4«, N o f c e dye ta effects t A n o t h e r s o u r c e o f n o i s e was a s s o c i a t e d w i t h t h e p r o b e s used t o measure the temperature of the working s e c t i o n . which i s a piece o f s t i f f l e a d , r u n s up t h e c e n t r e walls. As shown i n f i g u r e 4 . 3 , t h e h w i r e s u p p o r t i n g e i t h e r a -thermocouple o r probe, thermistor o f t h e l o w e r cone w i t h o u t m a k i n g conta-ct w i t h the T h i s l e a d p e n e t r a t e s t h e F a r a d a y cage and may a c t as an a e r i a l as i s a b o u t 4m l o n g . it N o i s e due t o t h i s s o u r c e reached up t o O . l p A when t h e r m i s t o r s were used b u t l a t e r w i t h t h e r m o c o u p l e s as t h e s e n s i n g t h e n o i s e was n e g l i g i b l e . device T h i s was p r o b a b l y because o f t h e h i g h R e s i s t a n c e o f t h e t h e r m i s t o r , c i r c u i t , w h i c h was t y p i c a l l y 3 k f t as opposed t o t h e 5 t o 10 i l of the thermocouples, I t was a l s o f o u n d n e c e s s a r y t o c a r e f u l l y s c r e e n the l i g h t b u l b y t h a t was used i n t h e F a r a d a y cage w i t h a l a t e r m o d i f i c a t i o n o f the tunnel. 4.3.5. Additional sources of noise One f u r t h e r cause o f n o i s e was t h e f a i l u r e t o remove the l a y e r surrounding the d i e l e c t r i c i n low noise c o a x i a l c a b l e . 12 has a s m a l l r e s i s t a n c e compared t o t h e 10 and r e s u l t e d e.g. t u n n e l tended input resistor i n an i n t e r m i t t e n t s h o r t c i r c u i t when t h e when t h e b l o w e r was s w i t c h e d o n . not securely ft layer of the V.R.E. I f t h e spacers i n the i n s u l a t o r nose through were the level. When a l l t h e s o u r c e s o f n o i s e m e n t i o n e d above had been s u c c e s s f u l l y the background noise This c a b l e was v i b r a t e d , f i x e d , t h e i r movement when the a i r was p a s s i n g t o cause an a p p r e c i a b l e semiconducting reduced l e v e l was 0 . 0 0 2 pA t h r o u g h o u t a h e a t i n g and c o o l i n g c y c l e l a s t i n g 30 m i n u t e s . complete Heater resistor Dry bulb thermo couple 3 Scopper constanton Cotton wick Perspex Brass tube 75 i*m Eig.4.7 Humidity measuring section Cork 7 G l a s s tube Vacuum flask Mercury 0 Crushed M ETHS TANK Fig.4 8 AT ice 0°C Thermocouple reference j u n c t i o n unit 38, 4 . 4 , THE MEASUREMENT OF TEMPERATURE AND HUMIDITY 4.4.1. Temperature In the p i l o t variation measurement wind t u n n e l , temperature i n current passing was a p p l i e d a c r o s s i t . was measured by o b s e r v i n g t h r o u g h a t h e r m i s t o r when a c o n s t a n t To a v o i d h e a t i n g t h e t h e r m i s t o r , t h e voltage c u r r e n t had t o be k e p t t o a minimum w h i c h made i t d i f f i c u l t t o use t h i s method t o a signal suitable f o r r e c o r d i n g on a c h a r t r e c o r d e r . the produce As m e n t i o n e d i n s e c t i o n 4 . 3 . 4 the r e l a t i v e l y h i g h r e s i s t a n c e o f the t h e r m i s t o r tended to cause n o i s e was inserted on t h e V . R . E . o u t p u t when t h e t e m p e r a t u r e m e a s u r i n g probe i n t o t h e w o r k i n g s e c t i o n o f the wind t u n n e l - copper-constantan So l o w r e s i s t a n c e t h e r m o c o u p l e s were used w h i c h gave an E . M . F . o f a p p r o x i m a t e l y 40 (A V °C * and t h e s i g n a l was a m p l i f i e d w i t h an c i r c u i t D.C. a m p l i f e r . The t e m p e r a t u r e s of the c o l d room, t h e o u t l e t f r o m t h e b l o w e r , and 2 - o t h e r p o i n t s i n the w i n d t u n n e l were a l s o 4 . 4 . 2 . Measurement integrated measured. of h u m i d i t y The h u m i d i t y m e a s u r i n g s e c t i o n was p l a c e d downwind o f t h e w o r k i n g ( F i g . 4 . 3 ) and c a r e was t a k e n t o e n s u r e t h a t t h e r e were no l e a k s between t h e 2 p o i n t s . copper-constantan Dry b u l b and wet b u l b d e p r e s s i o n thermocouples as i n f i g u r e 4 . 7 . section i n the t u n n e l were measured using The w a t e r h e l d i n t h e p e r s p e x c o n t a i n e r c o u l d be m e l t e d by t h e h e a t e r r e s i s t a n c e and a l l l w w e d wet t h e c o t t o n w i c k w h i c h c o v e r e d one j u n c t i o n o f a d i f f e r e n t i a l mocouple. aspirated j u s t i f i e d as i n c r e a s i n g the bulb depression T h i s was presumed t o be f o r t h e r a n g e o f wind speeds u s e d . r e l a t i v e h u m i d i t y was + 3%. 4.4.3 The t h e r m o c o u p l e r e f e r e n c e The p r o b a b l e error junction Four s e p a r a t e t h e r m o c o u p l e r e f e r e n c e were c o n t a i n e d i n one u n i t f o r an a i r f l o w d i d not cause any i n c r e a s e o f wet i n the crushed ther- The v a l u e o f r e l a t i v e h u m i d i t y was r e a d o f f t h e t a b l e s p s y c h r o m e t e r i n KAYE and LABY ( 1 9 7 0 ) . to (Fig. 4.8). j u n c t i o n s were r e q u i r e d and t h e s e A vacuum f l a s k , c o n t a i n i n g i c e and t h e j u n c t i o n s , was p l a c e d i n s i d e a t a n k c o n t a i n i n g about 20 l i t r e s o f m e t h y l a t e d s p i r i t s w h i c h was h e l d about 0 ° C . This ensured rV /vWWA hir* K 7o9C m 0 O ^ A W v Hi*/ I nput Output Mi 1HP A Frequency Compensation Oflset voltage vws^ 33o Fig.49 Am pi i f i e r Basic d. c . ampl ifier c i r c u i t Amplification A,- 1 4 7 5L J.Z0O 4-7W I SbSL 1,100 / kSl s-6 a J10 51 1,200 6 00 1,100 3 4 5" I33k» 610SL / AS. — 6L0SL 8U>SL I feSi TEMPERATURE 13 [0 L ko I 60 RECORDER DEFLECTION mm FIG.4.10 TYPICAL AMPLIFIER CALIBRATION (Workfng temperature) 39. t h a t t h e i c e o n l y had t o be r e p l a c e d w e e k l y . The m e r c u r y a c t e d as b o t h a h e a t s i n k and a good t h e r m a l c o n t a c t w i t h t h e ice. 4.4.4. The t'hprmo^'P.I^, w U f ^ r g t The 5 D . C . a m p l i f i e r s a l l used s i m i l a r 'Radiospares 1 Integrated c i r c u i t s (709-OPA) w h i c h were powered by a + 15 V s t a b i l i s e d power supply-. The a m p l i f i c a t i o n c o u l d be v a r i e d by a l t e r i n g t h e v a l u e o f t h e f e e d b a c k Rp and t h e i n p u t r e s i s t o r R j N ( F i g . 4.9). a p p l i e d t o the i n p u t t o ensure t h a t current. resitor The o f f s e t v o l t a g e had t o be t h e r e was zero o u t p u t f o r zero i n p u t L a r g e v a l u e s o f f r e q u e n c y c o m p e n s a t i o n c a p a c i t o r s were used to p r e v e n t i n s t a b i l i t y caused by t h e a m p l i f i c a t i o n o f unwanted h i g h f r e q u e n c y noise. The b i g g e s t d i f f i c u l t y i n b u i l d i n g t h e 5 c i r c u i t s i n t o one r a c k mounted p a n e l was t h e e l i m i n a t i o n o f e a r t h l o o p s w h i c h caused the a m p l i f i e r s t o go o f f s c a l e . circuit as T h i s was s o l v e d by c o n n e c t i n g e v e r y e a r t h p o i n t o f t h e t o a common e a r t h and by s c r e e n i n g as much o f t h e t h e r m o c o u p l e leads possible. 4 . 4 . 5 . C a l i b r a t i o n o f the thermocouples. A. c a l i b r a t i o n j u n c t i o n c o n s i s t i n g o f a c o p p e r - c o n s t a n t a n junction in a vacuum f l a s k f i l l e d w i t h p a r a f f i n was p e r m a n e n t l y a v a i l a b l e f o r c a l i b r a t i n g the temperature through the f u l l measuring c i r c u i t s . The j u n c t i o n c o u l d be r e a d i l y h e a t e d range o f t e m p e r a t u r e s t h a t weie measured i n t h e wind tunnel. One i m p o r t a n t s o u r c e o f e r r o r i n t h i s c a l i b r a t i o n was t h a t caused by t h e c a l i b r a t i n g thermocouple having a d i f f e r e n t resistance than the measuring o thermocouple. As t h e a m p l i f e r s were s e t t o zero by s h o r t i n g o u t t h e t h e r m o c o u p l e , t h i s c o u l d cause d i f f e r e n t zero r e a d i n g s t h e r m o c o u p l e s , w h i c h w o u l d n o t be r e a d i l y d e t e c t e d . f o r t h e two A preset resistor was p l a c e d i n s e r i e s w i t h t h e c a l i b r a t i n g t h e r m o c o u p l e and b e f o r e c a l i b r a t i o n the r e s i s t a n c e adjusted. A typical of the reference t h e r m o c o u p l e j u n c t i o n was c a l i b r a t i o n c u r v e i s shown i n F i g . 4.10 c u r v e s were r e p r o d u c e a b l e . These o v e r the p e r i o d o f measurements t o + 0 . 2 ° C . <z> 4 9 VWW* L <2) UV Li U.V. X60O W £ 7 6&a6 XM* Li Fig.4-11 U.V. Block diagram of temperature measuring c l r c u l t s Bypass St a Main tunnel •^Blower 7= Pitot-stat ic tube H oneycomb Fig.4.12 ic t a p s Location of o pitot-static tube S t a g n a t i o n pressure — s - ^ S t a t i c pressure St at ic ,t ops Fig.4.13 The pitot static head unit Photo r e s i s t o r SCHHITT U . V. Lamp Fig.4.14 The run of w i n d device as a flowmeter lOpmm. 40. 4 . 4 * 6 The a u t o m a t i c r e c o r d i n g o f t e m p e r a t u r e and h u m i d i t y . F i v e t h e r m o c o u p l e a m p l i f i e r s were b u i l t o f w h i c h two were c a p a b l e o f monitoring three t h e r m o c o u p l e s each b u t gave o n l y a m e t e r o u t p u t - These were v e r y u s e f u l i n t h e e a r l y s t a g e s o f t h e e x p e r i m e n t and a l s o f o r c h e c k i n g t h a t t h e h e a t i n g e l e m e n t s had c o o l e d down. f o r the two h u m i d i t y t e m p e r a t u r e measurements The a m p l i f i e r s used and t h e w o r k i n g t e m p e r a t u r e were c o n n e c t e d t o b o t h m e t e r s and u l t r a section v i o l e t recorder channels* The r e c o r d e r g a l v a n o m e t e r s c o u l d be s w i t c h e d i n t o t h e o u t p u t c i r c u i t a m p l i f i e r s by means o f a bypass switch (Fig. 4.1l). r e p l a c e t h e g a l v a n o m e t e r w i t h an e q u i v a l e n t r e s i s t o r . This switch could The r e c o r d e r g a l v a n o m e t e r s were p r o t e c t e d a g a i n s t b o t h p o s i t i v e and n e g a t i v e over- l o a d i n g by Zener d i o d e s p l a c e d back t o back w i t h a s u i t a b l e l o a d resistor. The r e c o r d e r was used on t h e 50 mm min * s p e e d t h r o u g h o u t most o f experiments. Other channels of the the were used t o r e c o r d a i r f l o w v e l o c i t y and t h e e l e c t r i c c u r r e n t measured by t h e V . R . E . 4 . 6 . THE MEASUREMENT OF AIR SPEED 4.6.1. The p i l o t - s t a t i c t u b e A p i t o t - s t a t i c t u b e was c o n s t r u c t e d ( F i g . 4 . 1 3 ) and c a r e f u l l y p o s i t i o n e d p a r a l l e l t o t h e wind t u n n e l a t a p o i n t u p s t r e a m f r o m t h e o f t h e bypass p i p e and t h e main w i n d t u n n e l (Figs. 4.3, 4.12). junction The p r e s s u r e d i f f e r e n c e between t h e s t a t i c and s t a g n a t i o n p r e s s u r e s was measured by an i n c l i n e d w a t e r manometer. According t o the t h e o r y of the p i t o t - s t a t i c tube t h i s d i f f e r e n c e i n p r e s s u r e s s h o u l d have been p r o p o r t i o n a l t o t h e s q u a r e o f the a i r v e l o c i t y . However? when t h i s i n s t r u m e n t was c a l i b r a t e d a g a i n s t a c a l i b r a t e d r u n o f wind machine f h e p r e s s u r e . d i f f e r e n c e was f o u n d t o be d i r e c t l y p r o p o r t i o n a l t o the v e l o c i t y . if Further? the c a l i b r a t i o n t h e f l o w was r e s t r i c t e d by p l a c i n g a s l e e v e changed v a l v e i n t h e main t u n n e l . The p r e s s u r e d i f f e r e n c e was a l s o an o r d e r o f magnitude g r e a t e r than expected. A p r o b a b l e e x p l a n a t i o n f o r t h i s f a i l u r e i s t h a t t h e r e was a static p r e s s u r e g r a d i e n t down t h e t u b e i n w h i c h t h e p i t o t - s t a t i c probe was p l a c e d 41. and t h i s caused an a p p r e c i a b l e s t a t i c p r e s s u r e d i f f e r e n c e between t h e s t a t i c and s t a g n a t i o n ta.->s. T h i s was g r e a t e r t h a n t h e d i f f e r e n c e between t h e s t a t i c and s t a g n a t i o n p r e s s u r e s a t any p o i n t on t h e p r o b e . A c c o r d i n g t o t h e HaganP o i s » e u i l l e law the f l o w r a t e i s d i r e c t l y p r o p o r t i o n a l to the pressure g r a d i e n t down a t u b e f o r l a m i n a r f l o w , so one w o u l d e x p e c t t h e measured s t a t i c p r e s s u r e d i f f e r e n c e between t h e two ' t a p s t o be p r o p o r t i o n a l t o t h e air velocity. 4.6..2. The r u n o f w i n d machine as a f l o w m e t e r . A r u n o f w i n d machine w i t h vanes the e n t r y p o i n t fell was f i t t e d i n t o the wind t u n n e l near ( F i g . 4 . 3 ) The vanes chopped a l i g h t beam ( F i g . 4 . 1 4 ) w h i c h on a p h o t o r e s i s t o r p r o d u c i n g a s e r i e s o f p u l s e s w h i c h were f e d i n t o an a m p l i f i e r and a S c h m i t t t r i g g e r w h i c h was used t o produce square of a r e g u l a r h e i g h t * pulses By u s i n g a d i o d e pump c i r c u i t t o produce an o u t p u t p r o p o r t i o n a l t o t h e p u l s e r e p e t i t i o n f r e q u e n c y , t h e a i r v e l o c i t y c o u l d be r e c o r d e d on a m e t e r and u l t r a v i o l e t recorder. T h i s d e v i c e worked v e r y w e l l a t room t e m p e r a t u r e , b u t t h e r u n o f w i n d machine t e n d e d t o be u n r e l i a b l e low temperatures. T h i s f l o w m e t e r was used i n a l t e r i n g t h e a i r f l o w t o r e q u i r e d v a l u e b u t was o f l i t t l e airspeed use f o r accurate measurements. the As t h e i n t h e w o r k i n g s e c t i o n c o u l d be j u d g e d t o + 0 . 5 ms ^ by n o t i n g t h e movement o f w a t e r d r o p s n e a r t e r m i n a l v e l o c i t y i t was d e c i d e d n o t t o a t t e m p t t o remedy t h e fault. at 42. C H A P T E R 5 THE PREPARATION OF ARTICIFICAL CLOUD WATER 5.1. 5.1.1 THE SOURCE QF IMPURITIES I N HAIL I m p u r i t i e s and h a i l growth The c o n c e n t r a t i o n o f i m p u r i t i e s i n h a i l t h e c l o u d d r o p l e t s f r o m which i t was f o r m e d . i s l i k e l y t o ' be t h e I f the h a i l grew by a c c r e t i o n onto a f r o z e n water drop then t h r o u g h o u t i t s growth i t w i l l from cloud d r o p l e t s . same as i n have been f o r m e d A c c o r d i n g t o LUDLAM ( 1 9 5 0 ) even i f t h e k e r n e l o f the h a i l was f o r m e d by t h e d i r e c t c o n d e n s a t i o n o f t h e v a p o u r , g r o w t h f r o m 1mm diameter w i l l be m a i n l y by t h e a c c r e t i o n o f s u p e r c o o l e d w a t e r d r o p s . 5 . 1 . 2 The c o n t a m i n a t i o n o f c l o u d w a t e r . True a e r o s o l s a r e n o t r e a d i l y c a p t u r e d by f a l l i n g w a t e r d r o p s o r h a i l , but a c c o r d i n g t o BYERS ( 1 9 6 5 ) are c a r r i e d around i n t h e a i r s t r e a m . Particles l a r g e r t h a n a f e w m i c r o n s a r e adsorbed a t t h e s u r f a c e o f f a l l i n g p r e c i p i t a t i o n . GREENFIELD ( 1 9 5 7 ) showed t h a t p a r t i c l e s s m a l l e r t h a n l j x m e n t e r by c o a g u l a t i n g w i t h s m a l l c l o u d d r o p l e t s . condensation n u c l e i w i l l D r o p l e t s w h i c h have grown f r o m be c o n t a m i n a t e d by t h e o r i g i n a l 5 . 1 . 3 C o n d e n s a t i o n n u c l e i and c l o u d w a t e r cloudwater condensation nucleus. purity C o n d e n s a t i o n n u c l e i may be c l a s s i f i e d by s i z e Giant r a d i u s y 1H m Large r a d i u s between 0 . 2 and 1.0\im Aitken radius < into 0.2f*m. JUNGE ( 1 9 5 3 ) measured t h e n u c l e u s c o n t e n t o f t h e a i r b o t h n e a r F r a n k f u r t and on t h e Z u g s p i t z e and f o u n d t h e number o f l a r g e n u c l e i v a r i e d f r o m 7 5 x 10 8 t o 4 x 10 -3 m q , w i t h a mean o f 1.3 x 10 _3 m . As WEICKMANN i and AUFM KAMPE (1953) e s t i m a t e d t h e c o n c e n t r a t i o n o f d r o p l e t s i n F l o r i d a 8 t h u n d e r s t o r m s t o be 10 -3 m i t appears t h a t l a r g e n u c l e i are probably t h e m a i n f o r m o f a c t i v j e c o n d e n s a t i o n n u c l e i i n t h u n d e r s t o r m s as are e f f e c t i v e a t lower s u p e r s a t u r a t i o n s than Aitken n u c l e i . concentration of n u c l e i increases r a p i d l y with decreasing they Since the r a d i u s i t would 43. seem t h a t t h e most common s i z e o f a c t i v e n u c l e u s t h e l o w e r end o f t h e l a r g e n u c l e u s range i n thunderclouds l i e s i . e . 0 . 2 - 0.3 ji m r a d i u s . The a c t u a l c o n c e n t r a t i o n o f t h e c o n d e n s a t i o n n u c l e u s c l o u d w a t e r depends on t h e of f a s t e r by c o a l e s c e n c e , w h i c h w i l l not g r e a t l y a l t e r the MASON ( 1 9 5 7 ) c o n s i d e r e d t h a t d r o p l e t s w i l l l i k e l y t o grow impurity concentration. grow t o a r a d i u s o f a b o u t 20^im by however t h i s e s t i m a t e was based on p u r e l y h y d r o d y n a m i c a l considerations. SARTOR ( 1 9 7 0 ) has deduced t h e o r e t i c a l l y t h a t t h e mass g r o w t h r a t e s o f d r o p l e t s o f 10 ^ m r a d i u s w i l l even w i t h o u t c h a r g e s b e i n g p r e s e n t -1 30 kVm substance i n the s i z e t o w h i c h t h e d r o p l e t s grow by c o n d e n s a t i o n w a t e r v a p o u r , because above a c e r t a i n s i z e t h e y are condensation; at be i n c r e a s e d by an o r d e r o f m a g n i t u d e , on t h e d r o p l e t s , i f t h e p o t e n t i a l g r a d i e n t «3 . S h o u l d c h a r g e s o f 3 x 10 a p o t e n t i a l g r a d i e n t 300 kVm 3 orders of magnitude. t h e e x t r e m e case a r e 1 pG be p r e s e n t then the growth r a t e s on each l O ^ d r o p l e t in s h o u l d be enhanced by As t h e v a l u e s o f charge and p o t e n t i a l g r a d i e n t i n s l i g h t l y s m a l l e r t h a n t h e maximum v a l u e s f o u n d by GUNN ( 1 9 5 0 ) i t seems l i k e l y t h a t t h i s p r o c e s s p r o v i d e s an e x p l a n a t i o n o f why p r e c i p i t a t i o n can d e v e l o p so r a p i d l y i n a cumulonimbus c l o u d . storm c e l l In a thunder- 5km t h i c k w i t h an u p d r a u g h t o f 10 ms * c l o u d d r o p l e t s a t have o n l y 10 m i n u t e s t o d e v e l o p i n t o p r e c i p i t a t i o n , w h i l e t h e t h e base time, c a l c u l a t e d by BEST ( l 9 5 l ) t o reach lOp. m r a d i u s by p u r e l y c o n d e n s a t i o n f r o m t h e v a p o u r i s o f t h e o r d e r o f one h o u r f o r a s u p e r s a t u r a t i o n o f 0.05%. I t w o u l d t h e r e f o r e seem t h a t an u p p e r l i m i t f o r m e d by c o n d e n s a t i o n to the r a d i u s o f d r o p l e t s f r o m t h e w a p o u r i n t h u n d e r c l o u d s i s p r o b a b l y 10^1 m#. 5 . 1 . 4 The c h e m i c a l n a t u r e o f c o n d e n s a t i o n nuclei. The most e f f e c t i v e c o n d e n s a t i o n n u c l e i are s o l u b l e i n w a t e r and g e n e r a l l y hygroscopic. likely The c o m p o s i t i o n o f l a r g e n u c l e i i s n o t w e l l know^but t h e most substances are sodium c h l o r i d e f r o m t h e oceans and ammonium s u l p h a t e , w h i c h i s f o r m e d f r o m s u l p h u r d i o x i d e and ammonia f r o m t h e d e c o m p o s i t i o n o f organic matter. ojcatsJyj 44. 5 . 1 . 5 E s t i m a t i o n of the i m p u r i t y c o n c e n t r a t i o n i n c l o u d w a t e r due to gondqnsaUPP PiA&J&j.* If t h e most i m p o r t a n t n u c l e i have r a d i i between O . l and Q . 3 j i m and c l o u d d r o p l e t s grow f r o m t h e vapour phase up t o l O j i m r a d i u s to estimate 5 o f ammonium s u l p h a t e TABLE 5 . 1 . Hm n 10 10 10 20 20 20 0.1 ro mgJL ~ i,n, c l o u d w a t e r due t o pa&lgi. 5.1 the a c t u a l c o n c e n t r a t i o n o f i m p u r i t y t o t h e r a d i i o f b o t h n u c l e u s and d r o p l e t 9 is n e i t h e r of which I t would seem l i k e l y t h a t t h e range o f c o n c e n t r a t i o n o f i m p u r i t i e s i s about 2 t o 20 mgA This, i t will be seen l a t e r , w e l l w i t h t h e range o f t h e p u r e s t c l o u d w a t e r samples. t h i s analysis that 1 2.0 16.0 54,0 0,3 2.0 6.8 0,3 0.1 0.2 0.3 Impurity concentrations known a c c u r a t e l y . is Concentration of impurity 0*0 can be seen f r o m t a b l e very sensitive ( S . G . o f sodium c h l o r i d e Radius o f condensation nucleus condensate of possible 1.8). Cloud d r o p l e t r a d i u s produced by g r o w t h f r o m the vapour As i t is ( £ £ g . 5 . 1 ) t h e c o n c e n t r a t i o n o f i m p u r i t i e s , assuming a s p e c i f i c g r a v i t y of 2.0 f o r the condensation nucleus. 2.2 9 the agrees I t is clear i f e l e c t r i c f i e l d s do g r e a t l y enhance t h e coalescence c l o u d d r o p l e t s o f l e s s t h a n 10 p r a d i u s , t h e n t h u n d e r s t o r m r a i n c o n t a i n a h i g h e r l e v e l o f i m p u r i t i e s t h a n non t h u n d e r y r a i n . from should The o n l y r e l e v a n t o b s e r v a t i o n by FISHER and GAMBELL ( 1 9 6 4 ) does n o t c o n f i r m t h i s . Furthermore possible a b s o r p t i o n o f s u l p h u r d i o x i d e and n i t r o g e n p e r o x i d e by p r e c i p i t a t i o n has n o t been c o n s i d e r e d . T h i s c a l c u l a t i o n has n e g l e c t e d t h e _ e f f e c t o f t h e washout o f n u c l e i w h i c h w i l l i n cumulonimbus t h a n i n s t r a t i f o r m c l o u d s . also p r o b a b l y be l e s s is i x in ^ O co CM • Ca • • rH o CO . rH . i o o co rH . vO . o o • o CO CM • . o rH o o o • CO CO o CO m • CO • • rH CO o CM • CM 2i 0 • Thunderstorm Riin - toy.iris end of r a i n f a l l clean funnel Collection of rain in clean funnel Collection of rain in clean funnel Analysis of snov/ and ice 3 flights conductivity high a t low levels. in • 1 t i CO 1 1 0 0 . . 0 in » . vO •si- 1 in co co CM o O 03 CM O CO . ro O O . CO * 0 o CM O 1 1 1 1 . O . . O O CO . 0 . . 0 o- O rH . • O r-H r-H . O CO O r-H . O O in rH . 1 1 d O CM 1 • CM . CM 1 CO . O 1 o rH CM CO . 0 o 1 1 o • CO . 1 • » O • CO . • rH . r-H 0 • l> « 0 — •1 . O 1 CM r H . . 0 0 CM O . CM O CO CO CM CO rH CO • O CM CO . . CM O O 0 CM . O CM O 'J < o ^ < < Ukraine a: ^0 North Russia "* o rH o o o s CM CM ON s vO . o O CD MM M4 O - vO . . o CO . vO MM IUCL (rt Q. CO vO • • o < >0> CM CM • o M 8.0 1 4 >H. : CO 12.0 10.3 i 4» •P «0 m -p -P • rH-H eHrf ! , 71.8 . CM o •H •H *t rH CO c 3 - 120 o i CO o o * All types of v/eather Thermally stable air from S.VY. -3 flights All types of v/eather TOTAL ELECTRIC CONDUCTIVITY cc -X fu cc 13.0 CO c• o < O O a a •> o ±c r> <c x O Z v O q uj o N QJ H O H cc: en Q a, _u ~> O UJ 2 2 O U J N hCC U J o^ H 3 H UJ U J d . CO 50 km South of Washington D.C. New Zealand Antartica 300ml fron coast. Hawaii Q UJ x CO O C 0 < rHvO O S ON X O [H OS UJ UU CQ Q i_ ; North Russia S.E. England ' CM vO O rH KOMBAYASI ISONO 1967 REFERENCE CN LOCATION < a 50 ml S.E of San Fransisco r—t aJ < UJ x ^ uj vO H ON H H § 2: O CO to in r-H 1 —1 3 •_u L U *r X CQ vO 10 ^5 o\ r H a: rH U_i 0 45. 5.2 5.2.1 MEASUREMENTS OF IMPURITIES IN CLOUD AND RAIN-WATER Type? o f measurement There are t h r e e methods o f c o l l e c t i n g p r e c i p i t a t i o n f o r c h e m i c a l namely l) cloud analysis collection 2) c o l l e c t i o n a t t h e g r o u n d where t h e f u n n e l used a l s o collects f a l l o u t between p e r i o d s o f p r e c i p i t a t i o n . 3) c o l l e c t i o n at the ground of r a i n f a l l only. U n f o r t u n a t e l y most measurements are o f t y p e 2 and t h e r e are v e r y f e w m e a s u r e - ments made i n c l o u d s . 5 . 2 . 2 The e f f e c t s o f t h e g e o g r a p h i c a l l o c a t i o n o f the s a m p l i n g s i t e . H i g h l e v e l s o f i m p u r i t i e s i n p r e c i p i t a t i o n b o t h i n and b e l o w c l o u d s arise n e a r a source of n u c l e i . T h i s may be an i n d u s t r i a l c e n t r e , where s u l p h u r and ammonium i m p u r i t i e s p r e d o m i n a t e , o r n e a r t h e s e a , where sea i s present impurity i n abnormally large concentrations. concentrations f o u n d i n c l o u d s are salt l i k e l y t o be a more r e l i a b l e g u i d e t o t h e l e v e l s found i n thunderstorms, but i f the stratus G e n e r a l l y the will samples are t a k e n i n s l o w l y moving c l o u d s o v e r an i n d u s t r i a l a r e a t h e c o n c e n t r a t i o n i s l i k e l y t o be much h i g h e r t h a n i n a c u m u l o n i m b u s . 5.2.3 The e f f e c t s o f washout on measurements a t the around. PETRENCHUK and SELEZNEVA ( 1 9 7 0 ) have compared c l o u d measurements w i t h g r o u n d measurements o f i m p u r i t y c o n c e n t r a t i o n s parts i n p r e c i p i t a t i o n , f o r various o f t h e S o v i e t U n i o n , and deduced t h e amount o f c o n t a m i n a t i o n o c c u r r i n g d u r i n g the f a l l of the p r e c i p i t a t i o n i n the n o r t h o f Russia 5.2.4. f r o m cloud base. T h i s r a n g e s f r o m 45% t o 80% i n i n d u s t r i a l U k r a i n e . The p u r i t y o f t h u n d e r c l o u d w a t e r . A number o f r e c e n t measurements o f t h e concentration of dissolved i m p u r i t i e s i n p r e c i p i t a t i o n b o t h a t t h e g r o u n d and i n c l o u d s are i n Table 5 . 2 . I t can be seen t h a t there even f o r measurements w h i c h were s e l e c t e d contained i s a wide range f r o m 2 t o 13 mg 2. f o r being e i t h e r i n cloud c o l l e c t e d a t t h e g r o u n d u n d e r c o n d i t i o n s where washout was s m a l l * or The 46. most common i m p u r i t i e s a r e Concentrations sulphate (S0 ) , chloride ( C l ) and s o l d i u m ( N a ) . 4 w h i c h have been o b t a i n e d i n v a r i o u s types o f weather are l i a b l e t o be h e a v i l y b i a s e d by a f e w p e r i o d s o f r a i n f a l l d u r i n g i n v e r s i o n c o n d i t i o n s , where t h e t o t a l i o n i c c o n c e n t r a t i o n can be as h i g h as 100 m g £ (DROZDOVA and PETRENCHUK, 1 9 6 6 ) . From T a b l e 5 » 2 t h e minimum c o n c e n t r a t i o n o f i o n i c s u b s t a n c e s i n c l o u d w a t e r p r o b a b l y l i e s around t h e 2-0 m g i * " 1 v a l u e f o u n d by ODD IE (1962) f r o m a i r b o r n e measurements i n a c l e a n a i r m a s s and BROCAS and DELWICHE ( 1 9 6 3 ) f r o m snow i n Antarctica. An u p p e r l i m i t to the concentration b to estimate f o r thunderstorms is hard .-i b u t i s p r o b a c y about 10 mgJt which i s t h e average v a l u e f o r a l l w e a t h e r c o n d i t i o n s i n a f a i r l y l o w - p o l l u t e d a r e a such as N o r t h e r n (DROZDOVA and PETRENCHUK, 1970) and a l i t t l e Russia l e s s t h a n t h e average o f the a i r b o r n e measurements made o v e r s o u t h e r n E n g l a n d by 0 D D I E ( l 9 6 2 ) » 5*2«5 The l o w e r p o s i t i v e charge and t h e p u r i t y o f cloudwater. The c o n c e n t r a t i o n o f d i s s o l v e d s u b s t a n c e s i n t h e thunderstorm w i l l depend the nearness o f o t h e r cloud droplets will on t h e l e v e l o f a i r p o l l u t i o n n e a r t h e s o u r c e s o f a e r o s o l s such as t h e s e a . The l o w e r p o s i t i v e charge has Many o f been observed area o f low p o l l u t i o n . i n most t h u n d e r c l o u d s I f the the come f r o m a i r i s probably well mixed. several SCRASE ( 1 9 3 7 ) and SIMPSON and ROBINSON ( l 9 4 l ) t i m e s by SIMPSON and a t Kew, w h i c h i s n o t i n an l o w e r p o s i t i v e charge were f o u n d t o be p r e s e n t t h e n any mechanism e x p l a i n i n g i t s o r i g i n must n o t be t o the c o n c e n t r a t i o n o f i m p u r i t i e s * c o n s i d e r i n g b o t h the t h e o r y of t h e and r e c e n t s t o r m and f o r m near c l o u d base i n an u p d r a u g h t t h a t has t h e l o w e s t 2 km o f the a t m o s p h e r e , where t h e highly sensitive cloudwater of a Therefore, from f o r m a t i o n of i m p u r i t i e s i n cloud water measurements i t seems t h a t t h e mechanism o f t h e c h a r g e must be e f f e c t i v e i n t h e i m p u r i t y range 2 t o 10 mgH lower p o s i t i v e • Fig.5.1 The deionizing apparatus 47. 5.3. THE PREPARATION OF ARTIFICIAL CLOUD WATER The a r t i f i c i a l chemicals c l o u d w a t e r was made by a d d i n g known q u a n t i t i e s t o w a t e r w h i c h was a t l e a s t a f a c t o r o f 30 p u r e r t h a n t h e solution. The i m p u r i t i e s i n o r d i n a r y t a p w a t e r c o n s i s t i o n s such as c a l c i u m , copper These were r e d u c e d T 5'3.2,, h Ion e of ion mainly of and s o | d i u m , and a l s o g r e a s e and pure final dissolved microorganisms. t o a l o w l e v e l by a d i s t i l l a t i o n and d e i o n i z i n g u n i t . ^ i o n i z a t i o n of water. exchange r e s i n s consist o f p o r o u s beads o f an i n e r t m a t e r i a l such polystyrene fall of c o n t a i n i n g f u n c t i o n a l groups which t e n d t o absorb i o n s . The r e s i n s i n t o two b r o a d c l a s s e s , c a t i o n and a n i o n e x c h a n g e s , d e p e n d i n g on t h e i o n removed f r o m t h e s u r r o u n d i n g s o l u t i o n . o f one s i g n and i t s r e p l a c e m e n t expressed as type The p r o c e s s o f r e m o v a l o f an by a n o t h e r ion is reversible and can be as: CATION RESIN R - S0 H + Na C I R - S0 R - N H* OH" + H C l ^ = * R 3 3 Na + N C l ANION RESIN where If - NH^ C l 4- H 0 2 R i s t h e base and SO^H and NH^ OH a r e the f u n c t i o n a l groups of the resins. one r u n s a weak s o l u t i o n o f sodium c h l o r i d e t h r o u g h a c a t i o n r e s i n t h e n resultant outflow w i l l c o n t a i n h y d r o c h l o r i c a c i d and i f t h i s anion r e s i n the a c i d w i l l All t e n d t o be t u r n e d i n t o pure i o n s are n o t removed e q u a l l y and t h e e x p r e s s e d i n terms o f an exchange p o t e n t i a l i s r u n i n t o an water. s e l e c t i v i t y o f t h e r e s i n can be for a particular ion. In general m u l t i v a l e n t i o n s a r e more e a s i l y removed f r o m d i l u t e s o l u t i o n s because have h i g h e r exchange p o t e n t i a l s , _. 4+ Th > c Fe 3+ * > ^2+ Zn > .„+ NH^ > „+ K A n o t h e f t y p e o f d e i o n i s a t i o n uses mixed bed r e s i n s w h i c h a r e m i x t u r e o f c a t i o n and a n i o n r e s i n s . at e f f e c t i v e l y neutral they namely, _ 2+ Ba > the an i n t i m a t e These have t h e a d v a n t a g e o f w o r k i n g pH and a r e h i g h l y e f f i c i e n t . 48. 5.3.3 The w a t e r p u r i f i c a t i o n Figure 5 . 1 shows t h e c o m p l e t e u n i t ? w h i c h was c a p a b l e o f appoximately 1 l i t r e needed. system. o f pure w a t e r every hour w i t h v e r y l i t t l e The l a y o u t o f t h e d i s t i l l i n g R. Diawson and c o n s i s t e d column t o p r e v e n t condenser. reservoir alkaline producing of a 2 l i t r e splashing, and t h e attention a p p a r a t u s was recommended by D r . flask f i t t e d with a fractionating s t r e a m was condensed i n t h e Liebig Water c o u l d be c o n t i n u o u s l y r u n i n t o t h e f l a s k f r o m t h e w h i c h was r e f i l l e d e v e r y h a l f hour. The f l a s k c o n t a i n e d s o l u t i o n o f p o t a s s i u m permanganate w h i c h was used t o any o r g a n i c m a t t e r t o c a r b o n d i o x i d e and oxidise water. The d e i o n i s i n g columns were 0.7m l o n g and 10 mm i n t e r n a l The r e s i n s was h e l d i n p l a c e by s i n t e r e d pyrex chippings at the top. head o f w a t e r f r o m t h e small reservoir. an diameter. g l a s s p l u g s a t t h e b o t t o m and The w a t e r r a n t h r o u g h t h e system u n d e r the The f l o w r a t e f o r optimum d e i o n i z a t i o n depends on t h e volume o f r e s i n and u s i n g t h e m a n u f a c t u r e r s s p e c i f i c a t i o n t h i s worked o u t a t 900 ml p e r hour. The c a t i o n r e s i n used was m a r k e t e d by B . D . H . as A m b e r l i t e and t h e i n the use a n i o n r e s i n was A m b e r l i t e I R A - 4 0 0 . The l a t t e r c h l o r i d e f o r m and had t o be c o n v e r t e d resir was a j p p l i e d to the hydroxyl by w a s h i n g w i t h a measured volume o f I N r a d i u m h y d r o x i d e . done i n t h e a p p a r a t u s on t h e l e f t o f f i g u r e 5 . 1 . IR-120 The t r e a t e d form before T h i s was resin c o u l d t h e n be t h o r o u g h l y m i x e d w i t h d e i o n i z e d w a t e r t o remove a l l of the a l k a l i . of IRA-4O0 and 5.3.4 The m i x e d bed r e s i n was c a l l e d MB-1 and was a m i x t u r e IR-120. P u r i t y o f the deionized water. The most abundant i m p u r i t y i n t h e d e i o n i z e d which was i n e q u i l i b r i u m w i t h atmospheric removed by b u b b l i n g w i t h 0.8 t o 0 . 1 5 p mho cm concentration traces w a t e r was c a r b o n d i o x i d e carbon d i o x i d e . When t h i s n i t r o g e n the c o n d u c t i v i t y of the water f e l l T h i s l o w e r v a l u e c o r r e s p o n d s t o an o f s l i g h t l y l e s s t h a n 0 . 1 mgJC^. ionic was from 49. 5 . 3 . 5 The . , r t l f i c i a l cloudwater,. E l e c t r i c a l e f f e c t s i n v o l v i n g t h e r u p t u r e of t h e d o u b l e l a y e r a t a water surface have been f o u n d by DRAKE (1968) and IRIBARNE and MASON ( 1 9 6 7 ) t o be i n d e p e n d e n t the a c t u a l o f t h e s p e c i e s o f i o n p r e s e n t 3 and t o depend ionicj^ncentration. impurity concentrations constituents are only I t w o u l d appear f r o m t h e measurements o f i n cloudwater (Table 5.3) t h a t the p r i n c i p a l sodium $ c h l o r i d e and ammonium i o n s . So i t was d e c i d e d t o make up a r t i f i c a l c l o u d w a t e r c o n s i s t i n g o f o n l y sodium c h l o r i d e i m p u r i t i e s . L a t e r 5 i f time p e r m i t t e d ammonium s u l p h a t e ? other i m p u r i t i e s such as sodium s u l p h a t e c o u l d be u s e d » The c o n c e n t r a t i o n used was 4 . 5 mgSL ~ g i v i n g a c o n d u c t i v i t y o f 8 . 1 1 * mho cm * range o f i m p u r i t y c o n c e n t r a t i o n s pipette. w h i c h f a l l s w e l l w i t h i n the probable Approximately w e i g h e d o u t and d i s s o l v e d i n 250 m l o f d e i o n i z e d T h i s was t h e n d i l u t e d f u r t h e r by t a k i n g o u t 10 ml samples w i t h a F i n a l l y t h e w a t e r was s t o r e d d u r i n g t h e e x p e r i m e n t s Pyrex b o t t l e . in a 1 litre A l l t h e g l a s s w a r e used i n t h e p r e p a r a t i o n o f t h e c a r e f u l l y cleaned w i t h p r o p a n o l ? 1 lGmgif ). h i g h l y p u r e g r a d e , m a n u f a c t u r e d by ' a n a l a r ' w i t h a maximum i m p u r i t y l e v e l o f 0 . 1 % . 2g o f s o d i u m c h l o r i d e was water. 9 i n thunderstorm p r e c i p i t a t i o n (2 to The c h e m i c a l s used were a s p e c i a l B«DoH c a l l e d and detergent w a t e r was and t h o r o u g h l y r i n s e d i n r u n n i n g t a p w a t e r and f i n a l l y r i n s e d and l e f t t o s t a n d i n d e i o n i z e d water© 120platinum. w ire Brass h o l d e r Mould f o r freezing water drops onto a 120 \*m Platinum wire loop Mould used in t h e f r e e f l i g h t Fig.6-1 Moulds experiments for f r e e z i n g w a t e r drops wire 50. C H A P T E R FREE FLIGHT EXPERIMENTS ON 6.1. 6.1.1 Preparation of the 6 MELTING AND EVAPORATING ICE PARTICLES EXPERIMENTAL PROCEDURE ice particles. The i c e p a r t i c l e s were made by f r e e z i n g w a t e r d r o p s suspended i n i c e moulds (Fig. 6.1). These moulds c o n s i s t e d o f 3 t o 5 - mm d i a m e t e r p l a t i n u m w i r e f r o m w h i c h d r o p s were h u n g . loops o f Each hoop was c o n n e c t e d t o an a l u m i n i u m f r a m e by 2 b r a s s r o d s , one o f w h i c h was i n s u l a t e d f r o m t h e f r a m e by a p e r s p e x bush. The w i r e c o u l d be c l e a n e d by h e a t i n g t o w h i t e h e a t by an e l e c t r i c c u r r e n t f r o m an a c c u m u l a t o r . The w a t e r d r o p s were l e f t i n a r e f r i g e r a t o r t o f r e e z e a t about N u c l e a t i o n would o f t e n n o t occur f o r s e v e r a l e x p e r i m e n t s no a t t e m p t was made t o c o n t r o l the f r e e z i n g t e m p e r a t u r e . h o u r s , but i n these e a r l y t h e t i m e o f n u c l e a t i o n o r measure When r e q u i r e d , t h e i c e p a r t i c l e s were removed f r o m t h e r e f r i g e r a t o r and p l a c e d i n t h e c o l d r o o m . were t h e n e i t h e r knocked o u t o f t h e i r hoops w i t h released by e l e c t r i c a l l y h e a t i n g t h e h o o p . the i c e p a r t i c l e s t o f a l l ~15°C, a tapered rapidly The i c e samples p y r e x tube The frame was d e s i g n e d t o clear i n t o a clean evaporating or enable basin. The i c e p a r t i c l e was p u t i n t o t h e wind t u n n e l t h r o u g h t h e h a t c h ( F i g . 4.3) its and a l l o w e d t o f a l l i n t o t h e w o r k i n g s e c t i o n j where i t seen moved i n t o p o s i t i o n of e q u i l i b r i u m . tunnel The p a r t i c l e was c a r r i e d f r o m t h e b a s i n t o t h e i n t h e end o f a p y r e x tube and was sucked o u t as p l a c e d i n t h e p a r t i a l l y open h a t c h . the surfaces i n contact with to s t i c k i n the tube i f i t started was Care had t o be t a k e n t o e n s u r e t h a t a l l the i c e were b e l o w 0 ° C as t h e p a r t i c l e The i c e p a r t i c l e s were shaped from the hoops. soon as t h e t u b e tended melting. i n a s i m i l a r way t o t h e d r o p s h a n g i n g They t e n d e d t o be somewhat e l l i p s o i d a l , w i t h a d e f i n i t e t e n d e n c y t o be w i d e r a t t h e end w h i c h was i n c o n t a c t w i t h t h e support. t h e s e e x p e r i m e n t s t h e o n l y d i m e n s i o n measured was t h e maximum w i d t h . In 51. 6.1.? Prfir^tjnriQ t All n n nY 11 ^ n t . a m i n a t i o n o f t h e the glassware used i n s t o r i n g t h e pure w a t e r and m a n i p u l a t i n g t h e i c e s p h e r e s was c a r e f u l l y c l e a n e d i n p r o p a n o l and d e t e r g e n t , w i t h t a p w a t e r and d e i o n i z e d w a t e r f o r s e v e r a l made f r o m b o r o s i l i c a t e g l a s s r a t h e r would n o t d i s s o l v e ice. hours* and t h e n A l l the glassware t h a n soda g l a s s t o e n s u r e t h a t t h e s i l i c a t e s f r o m the w a l l s of the c o n t a i n e r s e v a p o r a t i n g b a s i n s and t a p e r e d rinsed • was water The t u b e s were k e p t u n d e r d e i o n i z e d w a t e r when n o t i n use and were c a r e f u l l y d r i e d w i t h warm a i r f r o m a h a i r d r i e r b e f o r e u s e . t h e r e was any d o u b t as t o t h e c l e a n l i n e s s allowed t o stand o f a c o n t a i n e r , d e i o n i z e d w a t e r was i n i t f o r a f e w h o u r s j any c o n t a m i n a t i o n was shown by an increase i n the e l e c t r i c a l c o n d u c t i v i t y o f the water. The a l u m i n i u m w o r k i n g s e c t i o n and t h e b r a s s gauzes were a l s o c l e a n e d w i t h metal p o l i s h , and r u n n i n g w a t e r , b u t c o u l d n o t be c o n s i d e r e d clean i n the detergent present investigation. 6 . 2 , THE BEHAVIOUR OF THE SUPPORT SYSTEM, 6.2.1. Solid ice spheres. The w i n d t u n n e l was c a p a b l e o f s u p p o r t i n g an i c e p a r t i c l e f o r a b o u t 30 m i n u t e s b u t e v e n t u a l l y t h e p a r t i c l e w o u l d c r a s h o n t o t h e a i r f l o w gauzes. shaping T h i s was l i k e l y t o o c c u r a t any t i m e b u t p r o b a b l y a f t e r 30 m i n u t e s i n t h e t u n n e l t h e p a r t i c l e had l o s t so much mass by e v a p o r a t i o n t h a t t e n d e d t o move up t h e w o r k i n g s e c t i o n i n t o a r e g i o n where t h e it f l o w was u n i f o r m , and as a r e s u l t be l i a b l e t o c r a s h down o n t o t h e g a u z e s . 2 or 3 minutes the less Every i c e p a r t i c l e would t e n d t o come near t h e w a l l s and p r o b a b l y t o u c h e d f o r a f e w seconds b e f o r e m o v i n g away t o h o v e r somewhere else. 6.2.2. Melting It ice spheres was i m p o s s i b l e t o s u p p o r t an i c e p a r t i c l e throughout i t s . m e l t i n g process* temperature rose from about If i n t h e ";ind t u n n e l During-the m e l t i n g experiments the air - 5 ° C t o + 7°C a t a r a t e o f a b o u t 2 . 5 ° C min 1 . 52. H o w e v e r , because t h e wet b u l b d e p r e s s i o n temperature of the foe surface would be o f t h i s o r d e r , t h e was p r o b a b l y between 0 and +2°C on i m p a c t . The r e a s o n f o r t h e p a r t i c l e s t i c k i n g t o t h e is probably that there adhesion. Whether t h e s i d e s soon a f t e r r e a c h i n g 0 ° C was a w a t e r f i l m , o v e r t h e ice surface which assisted i c e p a r t i c l e s touched the sides every few seconds, o r t h e p r e s e n c e o f t h e w a t e r f i l m made t h e p a r t i c l e s u n s t a b l e , disadvantage actual i s n o t known. A o f t h e e x p e r i m e n t a l l a y o u t was t h e d i f f i c u l t y o f j u d g i n g t h e p o s i t i o n o f a p a r t i c l e m e r e l y by l o o k i n g down i n t o t h e t u n n e l and so 2 b l a c k r i n g s were p a i n t e d round t h e c o r e t o h e l p j u d g e t h e 6.2»3 Suggestions The p r o b a b l e f o r i m p r o v i n g the support perspective. system r e a s o n f o r t h e f a i l u r e o f t h e wind t u n n e l t o keep m e l t i n g p a r t i c l e s away f r o m t h e s i d e s was t h a t t h e l e v e l o f t u r b u l e n c e was t o o high. The f l o w s h a p i n g gauzes a t t h e b o t t o m o f t h e w o r k i n g s e c t i o n were c e r t a i n l y an improvement i n h e l p i n g t h e i c e spheres t o keep away f r o m t h e w a l l s . How- ever t h e a i r v e l o c i t y seems t o g u s t b o t h i n t h e v e r t i c a l and h o r i z o n t a l directiOiis. I f the height o f the w o r k i n g s e c t i o n i n c r e a s e d t o e l i m i n a t e t h e need f o r 2 r i g h t a n g l e the turbulence c o u l d have been reduced. have been p l a c e d a t A large ( F i g . 4 . 3 ) c o u l d have been bends i n t h e t u n n e l then s e t t l i n g chamber c o u l d then t h e entrance o f t h e t u n n e l and c o n n e c t e d s e c t i o n by means o f a s p e c i a l l y shaped c o n t r a c t i o n . to the working The e f f e c t o f t h e i m p e l l e r b l a d e s o f t h e b l o w e r , t r a v e l l i n g u p s t r e a m as p r e s s u r e w a v e s , was not It appreciated and no s c r e e n s were p l a c e d downwind o f t h e w o r k i n g section. i s c l e a r t h a t t h e r e s t r i c t i o n s made on t h e d e s i g n o f t h e t u n n e l by t h e need t o avoid contamination o f the i c e samples and t o measure v e r y s m a l l c u r r e n t s make t h e d e s i g n o f a v i a b l e s u p p o r t system n e a r l y I t may have been b e t t e r wind t u n n e l r a t h e r preconditions. t o have c o n c e n t r a t e d impossible. on p r o d u c i n g a w o r k a b l e t h a n a l l o w t h e d e s i g n t o be compromised by t o o many 53. 6*2.4 Conclusions on t h e s-fcudV o f m e l t i n g e l e c t r i f i c a t i o n u s i n g w i n d tunnels A t p r e s e n t t h e r e does n o t appear t o be a w i n d t u n n e l d e s i g n w h i c h w i l l f r e e l y support small ice p a r t i c l e s ( f r o m the by PRUPPACHER and NEIBURGER ( 1 9 6 8 ) , laminar f l o w tunnel I f a s m a l l t u n n e l were b u i l t w h i c h c o u l d p e r f o r m t h i s t a s k t h e n t h i s would be a u s e f u l t o o l study o f Cloud Physics* particle However, a t u n n e l that will i n the support laboratory a melting ice t h r o u g h o u t t h e t r a n s f o r m a t i o n f r o m s o l i d t o l i q u i d would p r o b a b l y have t o be more s o p h i s t i c a t e d particles. will described than a t u n n e l which merely supports s o l i d During the m e l t i n g process the change w h i c h w i l l mean t h a t t e r m i n a l speed o f t h e t h e a i r speed w i l l have t o be particle changed. As t h e f o r c e s on a s o l i d p a r t i c l e have d i f f e r e n t e f f e c t s t h a n on m o l t e n d r o p s , w h i c h can be d e f o r m e d , i t is will support an i c e sphere w i l l 6.3. 6.3.1. quite possible not suppoit a water that a system that drop. THE ELECTRIFICATION OF MELTING ICE E l e c t r i f i c a t i o n , i n f r e e fUqfrfc* E l e c t r i c a l measurements were made on 9 i c e w h i c h were f r e e l y s u p p o r t e d melting. sides d u r i n g the e a r l y stages of The average d r y b u l b t e m p e r a t u r e a t w h i c h t h e y c r a s h e d t o the was + 4 ° C . Wet b u l b d e p r e s s i o n was n o t m e a s u r e d , b u t f r o m l a t e r the a i r a t the (Table 6 . 1 ) . level away f r o m t h e spheres o f 3 t o 5 mm d i a m e t e r surface of the sides measurements spheres was p r o b a b l y l e s s t h a n 2 . 5 ° C on i m p a c t There was no e l e c t r i f i c a t i o n above t h e + 0 . 0 0 3 pA b a c k g r o u n d f o r any o f t h e samples. This i s i n agreement w i t h l a t e r observations w i t h i c e s p h e r e s m e l t i n g on p l a t i n u m w i r e s , when t h e e l e c t r i f i c a t i o n d i d n o t commence u n t i l water o f e l e c t r i c t h e m e l t i n g was w e l l a d v a n c e d . The i c e was made f r o m c o n d u c t i v i t y 0 . 7 5 j i mho cm * i n e q u i l i b r i u m w i t h laboratory carbon d i o x i d e . 6.3.2. The m e l t i n g o f i c e p a r t i c l e s A f t e r the m e l t i n g i c e p a r t i c l e s m e l t i n g p r o c e e d e d r a p i d l y and t h e t o 120 So on t h e sides of the had c r a s h e d on t h e tunnel. s i d e s o f the i c e u s u a l l y was f u l l y m e l t e d w i t h i n The i c e c o r e c i r c u l a t e d i n t h e m e l t w a t e r d u r i n g t h e later tunnel, 90 stages 54, of m e l t i n g . A l t h o u g h the s i d e s o f t h e t u n n e l had been c a r e f u l l y cleaned, i m p u r i t i e s w o u l d c e r t a i n l y have e n t e r e d t h e m e l t w a t e r d u r i n g m e l t i n g . The charge p r o d u c e d d u r i n g t h e m e l t i n g o f a 9 i c e p a r t i c l e s made f r o m w a t e r o f cm-' c o n d u c t i v i t y 0 . 7 5 | i m h o ^ i s c o n t a i n e d i n Table 6 - 1 . The r a t e o f c h a r g i n g reached a maximum i n t h e l a s t s t a g e s o f m e l t i n g and t e n d e d t o p e r s i s t f o r a b o u t 15 seconds a f t e r t h e l a s t t r a c e s o f i c e had v a n i s h e d . TABLE 6 . 1 The charge p r o d u c e d by i c e p a r t i c l e s on the s i d e o f t h e w i n d melting tunnel. Charge Diameter Temperature o f &ir Wet B u l b D e p r e s s i o n +pC mm °C °G 5.0 3 2.2 1.5 4.3 3i 3.5 2*5 3.3 4i 4.3 2.0 4.0 4 5.2 2.0 3.1 4i 4.1 4.0 1.4 5 4.2 2.0 2*9 4 4.5 2.5 0,8 3 3.0 1.7 2.1 4 3.0 1.8 T h e r e i s no s i g n i f i c a n t r e l a t i o n between t h e d i a m e t e r s o r t h e temperatures o f c r a s h i n g , and t h e charge p r o d u c e d . The mean charge was 3.0pC w i t h a s t a n d a r d d e v i a t i o n a b o u t t h e mean o f 0 . 5 p C . d i a m e t e r o f 4mm t h i s c o r r e s p o n d s t o a r a t i o o f charge For an average t o mass o f 0 . l p C mg ( 0 . 3 esu g * ) . A 1 1 i c e samples p r o d u c e d p o s i t i v e l y charged m e l t w a t e r C pnst a n t a n R g . 7-1 W i r e l o o p s u p p o r t s u s e d by D r a k e ( 1 9 G S ) Ice core SKI Air-flow Fig.7.2 C o n v e c i i v e c u r r e n t s in a m e l t i n g ice D r a k e a n d M a s o n ( 19G6 ) Air sphere flow Platinum a) Ice Fig.7. 3 sphere Straight wire b) support Partially molten C H A P T E R 7 EXPERIMENTS WITH MET.TTNG ICE SPHERES HANGING ON PLATINUM WIRES 7.1. THE SUPPORT OF MELTING ICE SPHERES 7 . 1 . , ! P r e v i o u s methods o f DRAKE (1968) has support. shown t h a t t h e way i n w h i c h t h e m e l t i n g i c e are v e n t i l a t e d can a f f e c t t h e amount o f charge magnitude. of particles s e p a r a t e d by an o r d e r of I n t e r m s o f t h e a i r bubble t h e o r y , v e n t i l a t i o n a i d s t h e r e m o v a l t h e n e g a t i v e l y charged j e t drops f o r m e d by t h e b u r s t i n g b u b b l e s . rate of v e n t i l a t i o n also a s s i s t s the f o r m a t i o n of convection i n the thus h e l p i n g the bubbles to burst at a surface Convection i n the meltwater w i l l bubbles bursting at at the ice-water the s u r f a c e interface. meltwater, free from contamination. also a l t e r the spectrum o f s i z e s o f by r e d u c i n g t h e c l u s t e r i n g o f the bubbles C l e a r l y t h e a i r f l o w around t h e p a r t i c l e and t h e way i n w h i c h i t r e a c t s t o t h e a i r s t r e a m g r e a t l y i n f l u e n c e t h e of A high amount c h a r g i n g p r o d u c e d by t h e m e l t i n g i c e . DINGER and GUNN ( 1 9 4 6 ) and MAC CREADY and PROUDFIT (1965) m e l t e d b l o c k s of ice i n containers i n an a i r s t r e a m . They f o u n d a charge was an o r d e r o f m a g n i t u d e l e s s t h a n t h a t measured 2 t'o 6 mm d i a m e t e r separation which by DRAKE ( F i g . 7 * l ) using i c e s p h e r e s h a n g i n g f r o m 1 mm l o o p s o f c o n s t a n t a n . d i f f e r e n c e between t h e s e r e s u l t s convection i n the m e l t w a t e r . The was a t t r i b u t e d by DRAKE t o the o n s e t o f T h i s c o n v e c t i o n has been d e s c r i b e d by DRAKE and MASON ( 1 9 6 6 ) who m e l t e d f r o z e n w a t e r d r o p s suspended f r o m a mesh o f 10 jim f i b r e s . i c e core These c o n v e c t i o n c u r r e n t s ( F i g . 7 . 2 ) , and t h e i r v e l o c i t y sometimes r a n d o m l y r o t a t e d increased w i t h the increasing melting r a t e and w i n d speed b u t n e v e r exceeded a f e w cm s The w i r e l o o p s u p p o r t d i d n o t p e r m i t t h e m e l t i n g p a r t i c l e t o and t h i s may i n c r e a s e t h e m o t i o n o f t h e ice core. T h i s t y p e of rotate support a l s o a l l o w s a p a r t i c l e t o be h e l d i n an a i r s t r e a m w h i c h i s m o v i n g considerably f a s t e r or slower is than i t s t e i m i n a l speed. I f the h i g h e r t h a n t h e t e r m i n a l s p e e d , the m e l t i n g w a t e r s u r f a c e w i l l airspeed tend it, I c e sphere on w i r e l o o p C o l d gas Filter 1 I H o t gas Fig.7. 4 Melting c h a m b e r used by Drake(19G*) B rass h ol d e r Ice p a r t i c l e L I Thermocouple Gauze 7.5 screen Modified probe Insulator tunnel section used w i t h w i r e support 56. t o v i b r a t e and r i p p l e more t h a n i n n a t u r e , p o s s i b l y e n h a n c i n g c h a r g i n g . T h e r e f o r e i t was d e c i d e d t o t r y t o d e v e l o p a more r e a l i s t i c method o f support. Z&LL2 A s t r a i g h t wjrp support W a t e r d r o p s were f r o z e n o n t o a 130 Hm p l a t i n u m w i r e and p l a c e d i n the wind t u n n e l . through the m e l t i n g drop u n t i l (Fig. 7.3b). I f the airspeed ( F i g . 7.3a.) D u r i n g t h e m e l t i n g p r o c e s s t h e w i r e moved i t was t a n g e n t i a l t o t h e w a t e r surface was n e a r l y e q u a l t o t h e t e r m i n a l speed o f t h e d r o p t h e n i t would c o n t i n u e t o hang on t h e w i r e f i n a l l y f a l l i n g f l y i n g o f f between 30 and 60s a f t e r m e l t i n g was c o m p l e t e . the J u d g i n g by" speed w i t h w h i c h the p a r t i c l e l e f t t h e w i r e , the a i r s p e e d w i t h i n 1 ms ^ o f t h e t e r m i n a l speed o f t h e d r o p . t h e p a r t i c l e sometimes like a jelly or was g e n e r a l l y During the m e l t i n g process r o t a t e d about a v e r t i c a l a x i s , and always v i b r a t e d i n t h e l a t e r stages of m e l t i n g . 7 . 1 . 3 . Comparison o f t h e w i r e s u p p o r t w i t h D r a k e ' s experiment. I n t h e e x p e r i m e n t o f DRAKE ( l 9 6 8 ) , t h e m e l t i n g p a r t i c l e i s s u p p o r t e d a j e t of a i r particle. a i r , the ( F i g . 7 . 4 ) w h i c h i s o f a p p r o x i m a t e l y t h e same w i d t h as As i t i s turbulence in the l i k e l y t h a t t h i s j e t i s mixing w i t h the environmental i n t h e r e g i o n o f t h e p a r t i c l e was p r o b a b l y g r e a t e r than i n t h e p r e s e n t i n v e s t i g a t i o n ( F i g . 7 . 5 ) , where t h e a i r f l o w has been smoothed by a honeycomb, gauze and c o n t r a c t i o n s e c t i o n . t h e m e l t w a t e r i s n o t c o n s t r a i n e d by t h e to r o t a t e i n a more n a t u r a l manner. Because t h e s u r f a c e o f s u p p o r t t h e whole p a r t i c l e i s W h i l e i t m i g h t be a r g u e d free that microturbulence i s probably present i n thunderclouds, t h i s low turbulence system has t h e a d v a n t a g e o f g i v i n g t h e p a r t i c l e more d e g r e e s o f f r e e d o m t h a n p r e v i o u s methods o f 7.2. support. THE EXPERIMENTAL PROCEDURE 7 . 9 . 1 P r e p a r a t i o n o f the ice particles. The i c e p a r t i c l e s were p r e p a r e d c o u l d e a s i l y be c l e a n e d . i n s p e c i a l moulds ( F i g . 6 , 1 ) which The p l a t i n u m w i r e was s o l d e r e d t o t h e end o f a s h o r t l e n g t h o f b r a s s r o d w h i c h c o u l d be p l a c e d i n a h o l d e r f i x e d t o the Stand tor ice p a r t i c l e h o l d e r Double L am p glazed / 1 77TTTT77. v. V, V. 'a \ \ Alunn in i u m Ice r e J e a s e p r o b e \ Fig.7.7 The refrigerator window Wood V, 57. baseplate of the mould. water drop which was The wire then passed through t h e centre of the t suspended from the p l a t i n u m w i r e Jftoop. The drop was nucleated e i t h e r by i c e c r y s t a l s produced by l i q u i d n i t r o g e n , or by small c r y s t a l s on the end of clean p l a t i n u m w i r e . A f t e r n u c l e a t i o n the drop 1 was allowed t o freeze completely before being released from the mould oy h e a t i n g the w i r e loop w i t h an e l e c t r i c c u r r e n t . wire and The brass rod w i t h the i c e p a r t i c l e attached could then be removed from i t s mould w i t h tweezers and screwed i n t o the h o l d e r ( F i g . 6.1). The i c e p a r t i c l e s were f r o z e n i n a r e f r i g e r a t o r and t r a n s f e r r e d t o the c o l d room i n a perspex box t o prevent m e l t i n g . 7.2.2 Examination of the i c e p a r t i c l e s * A r e f r i g e r a t o r was m o d i f i e d t o enable the ice p a r t i c l e s t o be studied under a microscope before m e l t i n g ( F i g . 7.7). capable of m a i n t a i n i n g temperatures reach - 15°C This r e f r i g e r a t o r was down to -13°G and on cool days could and so was used t o freeze the water drops. A,n Olympus Zoom - Stereo microscope was placed on the wooden top o f the r e f r i g e r a t o r and focused on t h e i c e sample which was held i n the stand. The advantages of t h i s microscope were the l a r g e working d i s t a n c e , and the wide f i e l d of view which enabled the whole p a r t i c l e t o be s t u d i e d s i m u l t a n e o u s l y , even at the maximum m a g n i f i c a t i o n of 40x. The microscope could a l s o be w i t h a camera but i n order t o speed up the experiments only b r i e f fitted notes of bubble s i z e spectrum, degree of o p a c i t y and the presence of cracks were made. The dimensions o f the p a r t i c l e s i n 3 m u t u a l l y p e r p e n d i c u l a r d i r e c t i o n s were measured w i t h a r u l e r . As the p a r t i c l e s were n o t r e g u l a r a more accurate method o f assessing the mass was d i f f i c u l t w i t h o u t r i s k of contamination. 7.2.3. The m e l t i n g stage. In o r d e r t o increase the m e l t i n g r a t e an attempt was made t o b u i l d a h u m i d i f y i n g u n i t which would reduce the wet b u l b depression i n the working section. E a r l y experiments w i t h passing steam i n t o the t u n n e l f a i l e d Temperature °C Pi Ambient tern perature 10 Fig.7 ? The s u r f a c e t e m p e r a t u r e of a n ice sphere during freezing 58. because o f condensation and subsequent blockage due t o water f r e e z i n g i n t h e pipes l e a d i n g i n t o t h e c o l d room. A h u m i d i f i e r c o n s i s t i n g of a deep t r a y of water and a 100 W lamp bulb d i d increase the h u m i d i t y s l i g h t l y b u t w i t h the h i g h f l o w r a t e o f a i r i n t h e t u n n e l a more s o p h i s t i c a t e d device would be needed t o b r i n g t h e r e l a t i v e h u m i d i t y up t o 90%. capacity The e x t r a h e a t i n g d i d enable t h e m e l t i n g r a t e s t o be increased d e s p i t e t h e increased wet b u l b depression* A t t h e maximum m e l t i n g r a t e a t t a i n a b l e a 4 mm i c e sphere melted i n 2.5 minutes* MASON (1956) c a l c u l a t e d t h a t a 4 mm s o l i d i c e sphere would m e l t i n 3 minutes w h i l e f a l l i n g from the Q°C l e v e l i n a c l o u d , assuming a s a t u r a t e d a d i a b a t i c lapse r a t e . D u r i n g m e l t i n g t h e p a r t i c l e could be viewed through t h e m i r r o r i n t h e w i n d t u n n e l and notes were made of the s t a t e and manner of m e l t i n g - These could be synchronised w i t h t h e records of temperature and charging c u r r e n t by using t h e event marker o n t h e u l t r a v i o l e t r e c o r d e r . An idea of the airspeed was obtained by n o t i n g the path of t h e drop a f t e r i t l e f t , , the wire._ A f t e r t h e m e l t i n g run was. completed any water l e f t i n t h e working , s e c t i o n was removed w i t h t i s s u e paper f i x e d t o the end o f a piece o f w i r e * 7.2.4 Precautions fp p r e v e n t contamination o f the ice p a r t i c l e s * The w i r e fcoops i n t h e i c e moulds and t h e p l a t i n u m wire supports were cleaned before use by e l e c t r i c a l l y h e a t i n g t o white heat. experiments Between t h e wire supports were stored i n deionized water. The p i p e t t e s and t h e o t h e r glassware were cleaned i n t h e same manner as described i n Chapter 6* The tweezers were washed i n deionized water a f t e r use. A l l t h e equipment used t o manipulate t h e water and i c e specimens was s t o r e d i n a glove box t o prevent contamination by d u s t . 7f3 lf t PegcrtpUPft The p a r t i c l e s were u s u a l l y misshapen spheres due t o t h e d i s t o r t i o n o f t h e o r i g i n a l drop under g r a v i t y w h i l e hanging i n the mould. Their masses ranged from 25 t o 60 mg b u t t y p i c a l dimensions were 4*5mm x 4.5mm x 4mm and a mass o f 36 - 40 mg. opaque. Usually t h e centre o f t h e p a r t i c l e looked A f t e r being examined under t h e microscope t h e p a r t i c l e s were 59. c l a s s i f i e d i n t o 2 groups, namely m i l k y and bubbly. I n bubbly i c e t h e bubbles were g e n e r a l l y d i s t i n g u i s h a b l e w i t h c l e a r i c e v i s i b l e between them. Milky ice contained patches where the bubbles could n o t be e a s i l y r e s o l v e d and the i c e looked opaque because o f a mass o f t i n y bubbles less than 20 Jim i n diameter. In general t h e lower t h e f r e e z i n g temperature the more l i k e l y the i c e was t o be m i l k y and the bubbles s m a l l . I n the range -6 t o -9°C the i c e was r a r e l y m i l k y and u s u a l l y very c l e a r o u t s i d e the c e n t r a l bubbly area. I n t h e range -13 t o -15 C t h e i c e u s u a l l y contained a m i l k y c e n t r a l r e g i o n , or a t l e a s t a v e r y opaque are made up o f a mass o f bubbles. Large bubbles were l e s s common i n such i c e , b u t i t was e v i d e n t t h a t more a i r was trapped than i n i c e frozen a t h i g h e r temperatures. This i s c o n s i s t e n t w i t h the increase o f gas s o l u b i l i t y i n water as the temperature f a l l s . 7.3.2 The f r e e z i n g process The behaviour o f t h e water drops d u r i n g f r e e z i n g was s t u d i e d by C r e p l a c i n g one of t h e i c e moulds w i t h a constantan feoop and making a copper constantan thermocouple j u n c t i o n on the loop i n c o n t a c t w i t h the surface of t h e water drop. ( F i g . 7.8) shows t h e v a r i a t i o n i n surface temperature during the f r e e z i n g process f o r a 3-g- mm diameter water drop f r e e z i n g i n an environment a t -11°C. During t h e p e r i o d AB the temperature of t h e drop f a l l s towards t h e ambient temperature o f the cold room. At B the drop i s nucleated by an i c e c r y s t a l and t h e s u r f a c e temperature r a p i d l y r i s e s t o about -3°C and remains constant f o r about 5 minutes. This may be e x p l a i n e d by assuming t h a t i n i t i a l l y an i c e s h e l l raj. i d l y forms and the l a t e n t heat released heats the drop u n t i l the i c e - w a t e r i n t e r f a c e i s a t 0°G. H e r e a f t e r t h e r a t e of f r e e z i n g i s governed by t h e c o n d u c t i o n o f the l a t e n t heat through the i c e s h e l l and i t s r e l e a s e t o t h e environment. of the p a r t i c l e w i l l be below 0°C. Hence the s u r f a c e temperatures At a time D the i f r e e z i n g i s complete and t h e p a r t i c l e cools t o t h e ambient temperature E and f i n a l l y t o t h e wet b u l b temperature FThis experiment confirmed t h a t l i t t l e e r r o r was i n t r o d u c e d i n t o t h e measurement o f t h e f r e e z i n g temperature, provided thac n u c l e a t i o n d i d n o t occur u n t i l t h e drop had been i n the r e f r i g e r a t o r f o r 5 minutes a t -11°C 60. and longer f o r higher temperatures. A t t h i s time t h e r a t e o f c o o l i n g had 1 dropped t o 0.2°C min"* . As only 10 - 15% o f the water freezes d u r i n g t h e i n i t i a l growth phase (Equation rapid ice 7.2), the a i r bubbles s t r u c t u r e i s probably g r e a t l y i n f l u e n c e d by the r a t e o f l o s s o f heat d u r i n g the slow growth p e r i o d . This heat l o s s can be c a l c u l a t e d from t h e d u r a t i o n o f t h e slow growth phase and the supercooling of the drop T. The mass m o f t h e water f r o z e n d u r i n g the f a s t phase i s r e l a t e d t o the t o t a l mass M o f the d r o p , t h e s p e c i f i c heat s o f water and the l a t e n t heat L o f water by equation 7.1. / M •*• s AT — .. mL r: jjj a o « o » « o « « s * . 7« 1 ~ F r a c t i o n of drop frozen ( f ) 7.2 The r a t e o f heat l o s s H d u r i n g t h e slow growth phase i s r e l a t e d t o the d u r a t i o n t o f t h i s phase by equation 7.3 H = M(l - f ) L 7.3 t For the 3-£ mm drop i n F i g , 7.8 t h e heat loss as given by equation 7*3 i s 21 mW. This i s n e a r l y an order o f magnitude l e s s than from, a comparable drop f a l l i n g a t i t s t e r m i n a l speed i n a s a t u r a t e d atmosphere a t t h e same temperature ( c f . s e c t i o n 8.4). 7.4. 7.4.1 THE ANALYSIS OF THE MELTING EXPERIMENTS The c o n t r o l o f the important parameters. As has been described ice i n s e c t i o n 2*4, the e l e c t r i f i c a t i o n of m e l t i n g i s h i g h l y dependent n o t o n l y on the m e l t i n g c o n d i t i o n s , b u t also on the chemical composition o f t h e water and t h e way i n which the p a r t i c l e was f r o z e n . DRAKE (1968) has suggested t h a t m e l t i n g r a t e and water p u r i t y have t h e g r e a t e s t e f f e c t on m e l t i n g e l e c t r i f i c a t i o n , b u t e a r l y i n the present i n v e s t i g a t i o n i t became apparent t h a t t h e temperature a t which the water was f r o z e n was also i m p o r t a n t * The c h i e f d i f f i c u l t y experienced i n analysing t h e data was t h a t t h e experimental c o n d i t i o n s could not be r e g u l a t e d a t w i l l - time t h e thermostat For most o f t h e on t h e c o l d room was n o t o p e r a t i o n a l so t h e temperature of the c o l d room depended t o a l a r g e e x t e n t on the l a b o r a t o r y temperature. (D if) I* 0) CD en en (V cn < 0) 3 I o 61. This was o f importance because the m e l t i n g r a t e of the p a r t i c l e s depended l a r g e l y on t h e r e l a t i v e h u m i d i t y of the a i r . This f e l l o f f r a b i d l y w i t h increase o f the temperature heated. through which the a i r i n t h e wind t u n n e l was The f r e e z i n g temperature of the p a r t i c l e s could be c o n t r o l l e d t o + 2°C and care was taken t o nucleate t h e drops when t h e y were w i t h i n 1°C of the environmental temperature. The mass of t h e ice p a r t i c l e s could be measured t o + 25% 9 a more accurate measurement was made d i f f i c u l t by t h e need t o a v o i d c o n t a m i n a t i o n , Same and t h e i r i r r e g u l a r shape. of measurements. T h e ^ p u r i t y o f t h e water was used f o r each s e t The carbon d i o x i d e c o n c e n t r a t i o n i n t h e water would probably depend on t h e temperature a t which the i c e was melted ( c . f Chafer 9) and so d i d not have t o be c o n t r o l l e d . The maximum r a t e of performing t h e m e l t i n g experiments was 3 per day of which o n l y about 2 out of 3 could be s u c c e s s f u l , the o t h e r s being r e j e c t e d u s u a l l y because the i c e p a r t i c l e was dropped o r t h e p l a t i n u m w i r e d i d n o t pass through the c e n t r e of t h e p a r t i c l e . This l i m i t e d the number o f p a r t i c l e s studied and t h e r e f o r e made t h e a n a l y s i s o f m e l t i n g e l e c t r i f i c a t i o n i n terms of a l l the i m p o r t a n t v a r i a b l e s d i f f i c u l t . designing the experiment support system. This l i m i ^ t i o n was accepted i n i n order t o attempt t o o b t a i n a more r e a l i s t i c However, because of the d i f f i c u l t y cjj r e g u l a t i n g a l l the v a r i a b l e s the conclusions are l i m i t e d i n a way which i s o f t e n found i n outdoor s t u d i e s i n atmospheric electricity. 7.4.2. The e l e c t r i c charge produced by m e l t i n g i c e . A l l t h e 150 i c e p a r t i c l e s melted on p l a t i n u m wires gained a p o s i t i v e charge and on no occasion was negative charging observed. p a t t e r n of e l e c t r i f i c a t i o n i s shown i n F i g . 7.9. The t y p i c a l For over h a l f the m e l t i n g p e r i o d no c h a r g i n g was measured and t h e advent o f water rippling over t h e i c e surface was u s u a l l y accompanied by a small p o s i t i v e c u r r e n t o f a few fA. When t h e p a r t i c l e s t a r t e d t o hang on t h e wire and became f r e e t o move, t h e r a t e o f charging increased r a p i d l y t o a d e f i n i t e maximum. U s u a l l y t h e p a r t i c l e would then leave t h e w i r e and s t i c k t o the F i g 7.10 Charge separated Pilot by m e l t i n g 4 m m d i o m e t e r i c e particles i nvest igat ion Freezing temperature Conductivity *C -1 of w a t e r = 7 5 ^ m h o s c m Charge PC 0 4 3 2 T 4 Melting (arbitrary rate units ) T 5 6 7 62. sides of the wind t u n n e l . I f tine charging continued on t h e sides f o r more than a few seconds i t was concluded t h a t the e l e c t r i f i c a t i o n process was not complete a t the moment the p a r t i c l e l e f t t h e w i r e and the o b s e r v a t i o n was rejected* This p a t t e r n o f e l e c t r i f i c a t i o n i s very s i m i l a r t o t h a t observed by DRAKE (1968) , but no negative charge was observed e a r l y i n the m e l t i n g process. The value of the charge produced was estimated by summing the average i charge produced i n 1 minute i n t e r v a l s up t o the time a t which the c u r r e n t decayed w i t h the time constant o f the V.R.E. Values o f t h e d r y b u l b and wet bulb depression as w e l l as the temperature o f the a i r near the ice p a r t i c l e were read o f f the r e c o r d e r c h a r t and used t o c a l c u l a t e the average m e l t i n g r a t e d u r i n g t h e l a s t minute of m e l t i n g . 7.4.3 A n a l y s i s of e a r l y m e l t i n g experiments w i t h deionized water• 15 i c e p a r t i c l e s o f about 4 mm e q u i v a l e n t d i a m e t e r i o n i z e d water w i t h c o n d u c t i v i t y 0.75^mho cm made from de- ? were melted. charge produced was + 3 . 5 + 0.5 pC, which corresponds r a t i o o f + 0.11 + 0.03 ? The average t o a charge/mass pC mg ^ (0.37 esu g ^ ) ; the e r r o r s quoted standard d e v i a t i o n s about the mean. are This compares w i t h 0.4 pC mg ^ measured by DINGER and GUNN (1946) a t m e l t i n g r a t e s n e a r l y 200 times greater. DRAKE found e l e c t r i f i c a t i o n of + 0.2 pC mg * f o r i c e spheres of s i m i l a r water p u r i t y when vigorous convection d i d not develop i n the m e l t w a t e r , but t h i s increased t o + 1.0 pc mg w i t h the onset o f convection. U n f o r t u n a t e l y d u r i n g these experiments the h u m i d i t y measurements were s u b j e c t t o a systematic e r r o r * and i t was not p o s s i b l e t o quote an absolute value f o r the m e l t i n g r a t e . I n F i g . 7-. 10 the charge separated i s p l o t t e d a g a i n s t m e l t i n g r a t e f o r i c e f r o z e n between -11 and -13°C. There i s a d e f i n i t e tendency f o r t h e charging t o increase with melting rate. DRAKE d i d not measure the m e l t i n g r a t e i n absolute terms but i t i s probably t h a t these data correspond t o the lowest 63. m e l t i n g r a t e s t h a t he s t u d i e d , as the t o t a l time f o r the i c e t o melt was on average 8 minutes compared w i t h 90 seconds t o 2 minutes shown i n the ' t y p i c a l records' i n DRAKE'S paper. to to o o o to CO 00 to in 2Ly E to 6 CO to 0) 0> 0 T o o o 0) O 0 > tn 0> to oo 0> o CM 64, CHAPTER 8 THE EFFECT OF MELTING RATE AND FREEZING TEMPERATURE ON MELTING ELECTRIFICATION. 8.1. MELTING RATE AND THE ENVIRONMENT. 8.1.1 The m e l t i n g o f f a l l i n g n a t u r a l small h a i l . MASON (1956) has solved the heat t r a n s f e r equations f o r i c e spheres f a l l i n g from the 0°C l e v e l i n a c l o u d , assuming a wet a d i a b a t i c lapse r a t e . This c a l c u l a t i o n shows ( F i g * 8.1) t h a t a 4 mm diameter i c e sphere o f s p e c i f i c g r a v i t y 0.9 w i l l have completely melted by t h e time i t reaches the +10°C l e v e l , approximately 3 minutes a f t e r t h e m e l t i n g s t a r t e d . The average m e l t i n g r a t e d u r i n g t h e l a s t minute of m e l t i n g i s 14 mg min * f o r a 4 mm p a r t i c l e and 9 mg min ^ f o r a 3 mm p a r t i c l e . I f the m e l t i n g h a i l were t o f a l l out o f the cloud then t h e m e l t i n g r a t e would be reduced because t h e heat gained by condensation o f water vapour would be decreased. MASON also showed t h a t i c e p a r t i c l e s of lower d e n s i t y would melt more s l o w l y because of t h e i r lower f a l l speeds. An upper l i m i t t o t h e m e l t i n g r a t e s o f i c e p a r t i c l e s o f 4 mm diameter and l e s s can be set a t 14 mg min "'*• As the a i r i n the wind t u n n e l was n o t s a t u r a t e d i t was intended t o t r y t o a l t e r t h e a i r temperature and r e l a t i v e h u m i d i t y so t h a t the i c e p a r t i c l e s could be melted a t r e a l i s t i c m e l t i n g ra te s • 8.1.2 The m e l t i n g o f i c e p a r t i c l e s i n the wind t u n n e l . The r a t e of heat f l o w t o a m e l t i n g i c e sphere has been g i v e n by LUDLAM (1950) as Heat Flow = 4 * [«^ K ^ T - T ^ + C L D ( P - P , ^ ) j j 8.1 m where b i s the r a d i u s o f the p a r t i c l e , T i t s surface t e m p e r a t u r e , T s the d r y bulb temperature o f the a i r away from the p a r t i c l e , P, P (T ) sa "t s : are the c o n c e n t r a t i o n s o f water vapour i n the remote environment and a t the water surface r e s p e c t i v e l y . 2.56 x lO^J kg 10~ 5 2 _ 1 The l a t e n t heat of vaporization» = the d i f f u s i o n c o e f f i c i e n t of water vapour, D = 2.4 x 2 m s , t h e c o n d u c t i v i t y o f a i r ^ K - 2.5 x 1 0 " Wnf 1 1 °K~ . 65. The c o e f f i c i e n t s C, and C take i n t o account the e f f e c t of v e n t i l a t i o n on the n m heat and vapour f l o w and are given by C h = 1.6 + 0.3 C m = 1.0 + 0.23 For a 4 mm 16.3 and (Re)^" (KRAMERS, 1946) (Re)^ (pROSSLINS, 1938) sphere at t e r m i n a l speed, Reynolds number C = Re = 2400 5 = 12.2. m The d e n s i t y of w a t e r vapour P i s equal t o the s a t u r a t i o n d e n s i t y of the air a t t h e dew point P ^ ( T ^ ^ ) - may be taken as 0°C The surface temperature of the m e l t i n g sphere as t h i s i n t r o d u c e s a maximum e r r o r of 3^ i n t o the f i n a l value o f the heat f l o w . For values of dew p o i n t between 0 and -10°C the data given by KAYE and LABY (1949) f i t s the f o l l o w i n g r e l a t i o n P J sat T where T, dew dew' A ) - P and T 2 x ( T ) = (5.0 T. sat s' dew - 0.1 T , ) x K f dew' 4 3 *g m" y °C" 1 ...8.2 are measured i n °C. s So the r a t e o f heat f l o w i n t o a m e l t i n g i c e sphere f a l l i n g a t t e r m i n a l speed may be obtained f l o w = 4 Ub[c, t K T + G h a Equation 8.3 was ice by s u b s t i t u t i n g equation 8.2 i n t o 8.3. I m D (P v . (T. sat ) - P dew Rate o f heat . (0)f\ sat* 8.3 J used to evaluate the r a t e o f heat f l o w i n t o the m e l t i n g p a r t i c l e s i n t h e wind t u n n e l . between approximately The e r r o r i n the r a t e o f heat f l o w v a r i e s A0% f o r a heat f l o w r a t e of 30 mW to 25$ a t 100 mW. At low heat f l o w r a t e s the dominant e r r o r i s associated of dew p o i n t which could o n l y be estimated to ± w i t h the measurement despite an e r r o r of o n l y + l-£# i n the measurement of r e l a t i v e h u m i d i t y . At h i g h m e l t i n g r a t e s the c h i e f source of e r r o r was the measurement of the r a d i u s of the p a r t i c l e which was 8.2 8.2.1 e s t i m a t e d . t o + 10%. THE EFFECT OF MELTING RATE QN ELECTRIFICATION. Mass, c o r r e c t i o n for e v a p o r a t i o n . A t low m e l t i n g r a t e s ao appreciable f r a c t i o n of the d u r i n g the 15 minutes i t i s i n the a i r s t r e a m . melted was estimated of the t u n n e l to 0°G i n 2 stages. ice may evaporate The mass o f i c e a c t u a l l y F i r s t l y d u r i n g the i n i t i a l the t o t a l amount o f heat l o s t due slow h e a t i n g t o evaporation during Fig. 8 2 The effect of m e l t i n g r a t e on m e l t i n g e l e c t r i f i c a t i o n Artificial cloudwattr Electrification p C mg-1 b e t w e e n -10 and - 1 3 C Drops f r o z e n in still a i r x •0 6 •05 H •04 - k * x -0% * -Hf 4- * Average melting r a t e I m t « F T r 1 —r~ F 1 1 r- . -1 10 m g m i n E l e c t r f f i c a t ion p C mg" 1 Drops frozen at -11*3**5*C 04 H •o5 -j • 0<# - x * •03 « x * ol X oi X - A v e r a g e m e l t i n g rate -i 1 > r ""i $° 1 i ' 1 r IOO ? J 1 1 1 — i$o . . F i g . 8.3 The effect of melting r a t e Artificial Electrification pC m g Drops frozen in on electrification cloudwater still air 1 r at # -10*3t'5 C 1 04 •03 •oz •O) i i —i— SO r 1 r S 10 frozen at > I . 1 ISO -I rate for last minute of ~13-t*3C Electrification pC mg 1 OS .0 3 •01 f f T I 1 » T i 50 l l too —f- —r 10 IS A v e r a g e melting \ mW 20 )S A v e r a g e meltfng Drops T — i — 100 - rate 10 ? -tmW melting 66. a time t , was 4 7rbfc L D ( P .(T. ) - P . ( i T. ))1 8.4 ^ m v sat dew sat * dew «* This f o l l o w s from e q u a t i o n s 8 . 1 and 8.2 assuming t h a t the average d i f f e r e n c e i n temperature between the dew p o i n t and t h e surface of the i c e i s i T, * dew r r During the m e l t i n g process the temperature o f the surface i s approximately 0°C so the heat l o s t , i n t i m e t ^ , due to e v a p o r a t i o n i s simply Ht = 3 . 9 b t_ 2 Tl.09 *- Using equations 8.4 + 0.022 T dew and 8.5 T 1 2 8.5 dew •* the t o t a l amount of water l o s t by evaporation was c a l c u l a t e d f o r a l l the i c e p a r t i c l e s . At a melting rate corresponding t o 20 mW, 50% o f the mass evaporated and a t 100 mW only 5% evapora ted. 9«2«2t T^e results for a r t i f i c i a l glgudwflter* The charge separated by the m e l t i n g of the a r t i f i c i a l cloudwater samples was always of the same s i g n , raamely the meltwater became p o s i t i v e l y charged. I f a l l the samples which were frozen i n s t i l l a i r between -10 and -15°C were considered then there was no apparent r e l a t i o n s h i p between maximum m e l t i n g rate and charge separated. For the range -10 t o -13°G "there i s a trend towards an increase i n c h a r g i n g w i t h increased m e l t i n g r a t e ( F i g . 8 . 2 ) . the range -lOj- t o -11% If ±s taken then t h e v a r i a t i o n becomes more marked w i t h almost a f a c t o r 10 increase i n e l e c t r i f i c a t i o n between m e l t i n g r a t e s of 10 and 15 mg min * ( F i g . 8 . 2 ) . F i g . 8.3 shows s i m i l a r though less w e l l defined v a r i a t i o n s of e l e c t r i f i c a t i o n w i t h m e l t i n g r a t e f o r water drops f r o z e n a t about -10 and - 1 3 ° C . of f r e e z i n g o f t h e water drop has an i m p o r t a n t e f f e c t on m e l t i n g e l e c t r i f i - ? cation. of The probable e r r o r i n t h e r a t i o of charge to mass i s i n the region 40 t o 50% due t o an u n c e r t a i n t y i n the mass of + 25% and i n the charge of + 20%* the These r e s u l t s suggest t h a t the temperature The e r r o r i n the measurement of charge i s due t o the f a c t t h a t molten drops f a l l o f f the wire d u r i n g the l a s t stages o f e l e c t r i f i c a t i o n . Fig 8.4 The effect of the type of x • — support @ 0 @ — Electrification 30 p C m g1 20 O 0 0 10 O 0 0 t » • 1 1 1 I Freezing Conductivity Melting Drops 1 1 temperature of water rate y 1 5 m g frozen 1 in still 1 1 1 °C 10 p mho min air 1 cm 67. 8 > 2 . 3 Comparison w i t h p r e v i o u s w o r k . These r e s u l t s a g r e e q u a l i t a t i v e l y w i t h the that the e l e c t r i f i c a t i o n melting rate increased o f DRAKE (1968) by a b o u t an o r d e r o f magnitude when t h e and wind speed became s u f f i c i e n t t o cause v i g o r o u s c o n v e c t i o n in the melt water. DRAKE d i d n o t measure t h e m e l t i n g r a t e a b s o l u t e l y so a d i r e c t comparison i s not p o s s i b l e . 8.3 t h a t observations There i s the l o w e r t h e f r e e z i n g t e m p e r a t u r e some e v i d e n c e the sharper f r o m F i g s . 8.2? the t r a n s i t i o n between t h e low and h i g h e l e c t r i f i c a t i o n r e g i o n s o f the g r a p h s . (1956) has c a l c u l a t e d t h a t t h e average m e l t i n g r a t e d u r i n g the o f m e l t i n g o f a 4mm s o l i d MASON l a s t minute i c e p a r t i c l e f a l l i n g f r o m the 0°C l e v e l in a cloud -1 i s 14 mg m i n . So i t seems p o s s i b l e t h a t such a p a r t i c l e would d e v e l o p ' vigorous convection i n the meltwater ( c f F i g . 8 . 2 ) • U n f o r t u n a t e l y i t was d i f f i c u l t t o observe t h e p a r t i c l e c l e a r l y enough t o v e r i f y t h a t t h e increase i n e l e c t r i f i c a t i o n c o i n c i d e d w i t h the onset o f convection* DRAKE f o u n d t h a t t h e t o t a l / ™4 \ comparable p u r i t y (10 c h a r g i n g p r o d u c e d by m e l t i n g p a r t i c l e s o f ~1 M ; was about 0 . 4 pC mg 0 . 0 3 pC mg ^ i n t h e absence o f c o n v e c t i o n . a t h i g h m e l t i n g r a t e s and A l t h o u g h he does n o t quote a c t u a l m e l t i n g r a t e s i t seems l i k e l y f r o m t h e d e s c r i p t i o n o f the t h a t the experiment range o f m e l t i n g r a t e s was s i m i l a r t o t h a t i n t h e p r e s e n t These v a l u e s f o r the i n F i g s . 8 . 2 and 8 . 3 . r a t i o o f charge Two p o s s i b l e the investigation. t o mass are a f a c t o r o f 10 g r e a t e r reasons f o r t h i s d i f f e r e n c e are than the d i f f e r e n t methods o f s u p p o r t i n g t h e p a r t i c l e and t h e f a c t t h a t DRAKE f r o z e the water drops i n an a i r s t r e a m as opposed t o s t i l l air. 8.3 THE EFFECT OF THE SUPPORT To see w h e t h e r t h e d i f f e r e n c e i n t h e m a g n i t u d e o f c h a r g i n g was due to t h e d i f f e r e n t ways o f s u p p o r t i n g t h e i c e p a r t i c l e s 10 f r o z e n w a t e r d r o p s were m e l t e d on ij? mm d i a m e t e r l o o p s o f p l a t i n u m w i r e . These r e s u l t s compared w i t h t h o s e o f a s i m i l a r e x p e r i m e n t w i t h p a r t i c l e s on t h e w i r e s u p p o r t used i n t h e e x p e r i m e n t d e s c r i b e d i n Section 8.2. seen i n F i g . 8 . 4 t h e r e was no s i g n i f i c a n t d i f f e r e n c e between were straight As can be the 00 LP (I i£> Q ft n 10 0) O O G QO OO -J N 0) f O o Fig.8 6 Heat flow from a w a t e r drop during Heat freezing f I ow ra t e mW 200 3 m m d la ventilated at 11ms 1 l?0 ( Theory) I GO ILo HO I00 60 ( Exper imen t) 3 mm dia stagnant lo air (corrected ) — i 1 1 -12 -jo Air t e r n p e r a t u re °c 1 -% i ~& » r -4 -2 68. e l e c t r i f i c a t i o n p r o d u c e d by p a r t i c l e s on e i t h e r s u p p o r t . I n both experiments t h e m e l t i n g r a t e s were j u d g e d t o be h i g h enough f o r v i g o r o u s e l e c t r i f i c a t i o n t o have o c c u r r e d . C l e a r l y t h e d i f f e r e n t t y p e s o f s u p p o r t do n o t cause an o r d e r of magnitude d i f f e r e n c e i n e l e c t r i f i c a t i o n a l t h o u g h p o s s i b l y the higher turbulence present i n DRAKE'S e x p e r i m e n t c o u l d be i m p o r t a n t . f 8 . 4 FREEZING RATE AND MELTING ELECTRIFICATION 8*4.1 Water d r o p s f r o z e n i n s t i l l a i r - Pure water* F i g . 8 . 4 shows t h a t t h e t e m p e r a t u r e a t w h i c h t h e d r o p s were f r o z e n has a H marked e f f e c t on t h e e l e c t r i c a t i o n p r o d u c e d on m e l t i n g . The p r o b a b l e accuracy o f t h e f r e e z i n g t e m p e r a t u r e was + 1°C due to the t h e r m o m e t e r and d r o p b e i n g l o c a t e d a b o u t 30 cm a p a r t . temperatures decreasing T h e r e i s some e v i d e n c e t h a t b e l o w - 12°C t h e charge temperature. separation for freezing increases r a p i d l y with I t was n o t e d i n C h a p t e r 7 t h a t b e l o w - 12°C t h e ice becomes more l i k e l y t o be m i l k y . 8.4.2. Water d r o p s f r o z e n i n a t l l j L a i r - A r t i f i c i a l The a r t i f i c i a l c l o u d w a t e r samples water. showed a s i m i l a r v a r i a t i o n o f m e l t i n g e l e c t r i f i c a t i o n w i t h f reezing temperature r a t e was s u f f i c i e n t t o e n s u r e t h a t cloud ( F i g . 8.5) provided t h a t the s m a l l v a r i a t i o n s i n m e l t i n g r a t e were n o t important. Below a m e l t i n g r a t e o f 14 mg min ^ t h e e f f e c t o f f r e e z i n g temperature i s a l t e r e d by t h e s h a r p changes i n t h e m e l t i n g - m e l t i n g r a t e graphs 8.4.3 (cf. Fig. 8.2, The f r e e z i n g r a t e and t h e The f r e e z i n g r a t e g o v e r n e d by t h e rate electrification 8.3). environement. d u r i n g t h e main p a r t o f the f r e e z i n g p r o c e s s o f heat l o s s f r o m t h e s u r f a c e o f the p a r t i c l e . h e a t l o s s f r o m t h e f r e e z i n g w a t e r d r o p s was d e t e r m i n e d by m o n i t o r i n g d r o p t e m p e r a t u r e as d e s c r i b e d heat i n S e c t i o n 7.3<,2. is The the The v a r i a t i o n o f r a t e o f l o s s w i t h a m b i e n t t e m p e r a t u r e i s p l o t t e d i n f i g . 8 . 6 f o r 3 . 5 mm d r o p s . The d o t t e d l i n e shows a c o r r e c t e d v a l u e f o r 3 mm d r o p s assuming t h a t heat melting loss i s p r o p o r t i o n a l to the surface The h e a t loss the area* f o r p a r t i c l e s i n an a i r s t r e a m was c a l c u l a t e d f r o m e q u a t i o n 8 . 1 assuming t h a t t h e s u r f a c e t e m p e r a t u r e o f t h e sphere was a t 0 ° C . Fig.«.7 The effect Deionized Melting of freezing water rate rate on m e l t i n g electrification 1-O^mhocm ) 1 4 mg min 1 x * Frozen @ 0 Frozen Drake in in airstream still air (196S) E l e c t r i f ic a t i o n 1 pCmq s 01 O a • 20 40 6o Heat IOO flowrate during mW 120 i I4.Q freezing 160 190 69. T h i s o v e r e s t i m a t e s t h e h e a t f l o w b u t as t h e s u r f a c e t e m p e r a t u r e v a r i e s b o t h w i t h t i m e and f r e e z i n g r a t e e s t i m a t e was n o t made. i n an u n d e t e r m i n e d manner a more a c c u r a t e I t can be seen f r o m F i g . 8 . 6 t h a t a 3mm d r o p f r e e z i n g -1 i n an a i r s t r e a m moving a t 11 ms similar particle A particle in s t i l l d i s s i p a t e s 10 t i m e s as much h e a t as a a i r even i f b o t h are freezing at -12°C i n s t i l l similar particle i n an e n v i r o n m e n t a t -12°G. a i r d i s s i p a t e s as much h e a t as a i n the a i r s t r e a m at - 2 ° C . 8 . 4 . 4 . The dependence o f m a t i n g e l e c t r i f i c a t i o n on f r e e z i n g rate. The e l e c t r i f i c a t i o n s t u d i e s o f t h e m e l t i n g o f w a t e r d r o p s f r o z e n i n a i r d e s c r i b e d i n s e c t i o n s 8 . 4 . 1 and 8 . 4 . 2 have shown t h a t t h e r e f o r the c h a r g i n g t o i n c r e a s e still i s a tendency as t h e f r e e z i n g t e m p e r a t u r e i s l o w e r e d . The e l e c t r i f i c a t i o n measured i n t h e s e e x p e r i m e n t s i s an o r d e r o f m a g n i t u d e l e s s t h a n d e t e c t e d by DRAKE (1968) under s i m i l a r c o n d i t i o n s . As t h e p a r t i c l e s m e l t e d by DRAKE were f r o z e n i n an a i r s t r e a m t h e d i f f e r e n c e between t h e 2 s t u d i e s may be r e s o l v e d by s u g g e s t i n g t h a t t h e e l e c t r i f i c a t i o n was h i g h l y dependent on t h e r a t e o f f r e e z i n g o f t h e w a t e r d r o p s . The f r e e z i n g c o n d i t i o n s were t h e r e f o r e a l t e r e d t o t e s t t h i s t h e o r y . The w a t e r d r o p s were hung f r o m a l | ran l o o p o f p l a t i n u m w i r e and c o u l d be f r o z e n i n an a i r s t r e a m , u s i n g a vacuum pump. The a i r speed was 11 ms ^ and t h e a i r t e m p e r a t u r e c o u l d be m o n i t o r e d by means o f a c o p p e r - c o n s t a n t a n thermocouple. The r a t e o f heat l o s s was c a l c u l a t e d as d e s c r i b e d i n the p r e v i o u s s e c t i o n assuming t h a t t h e a i r was s a t u r a t e d . As t h e a i r was sucked f r o m t h e b o t t o m o f t h e r e f r i g e r a t o r where i t was i n e q u i l i b r i u m w i t h ice, and was n o t h e a t e d , i t seems p r o b a b l e t h a t t h e a i r was s a t u r a t e d . The e l e c t r i f i c a t i o n was f o u n d t o i n c r e a s e r a t e o f heat l o s s f r o m the f r e e z i n g d r o p . d i s s i p a t i o n there r a p i d l y w i t h the i n c r e a s i n g A t low values o f heat i s a good agreement between t h e r e s u l t s o f t h i s e x p e r i m e n t and t h e e x p e r i m e n t w i t h the d r o p s f r o z e n i n s t i l l air (Fig, 8.7). v a l u e s o f h e a t f l o w r a t e were p r o b a b l y o v e r e s t i m a t e s f o r t h e As t h e ventilated O mm I mm Frozen in still air at -6-5'C Frozen in 0 too ^oo \xm I t—i Frozen F i g . 8,B The still I mm 0 in an frozen -1 11rns water 0 airstream drops at -12C air at~12-5C Fig.g.9 Solubility (Kayc of a i r and in water Laby,196«) Sol a b i l i t y ml ml 1 • oS >\ I > I I I I 2-<? i i I-9 oi -0 OZ o T 20 - 10 Tempe ra t u r e —? ~7— 10 20 30 70. d r o p s t h e agreement may be b e t t e r t h a n i n f i g . m a j o r s o u r c e o f i m p u r i t y i s a t m o s p h e r i c C® 2 a b o u t 0 . 1 pC m g " 1 when f r o z e n i n s t i l l 8.7. F o r d e i o n i z e d w a t e r whose the e l e c t r i f i c a t i o n increases a i r a t a b o u t - 1 0 ° C t o 0 . 8 pC mg 1 from when f r o z e n i n t h e a i r s t r e a m a t t h e same t e m p e r a t u r e . A d i r e c t c o m p a r i s o n w i t h t h e r e s u l t s o f DRAKE i s d i f f i c u l t because a c t u a l s i z e , a i r s p e e d and r e l a t i v e h u m i d i t y were n o t g i v e n i n h i s T a k i n g an a v e r a g e d i a m e t e r o f 3 mm and an a i r s p e e d o f 7 ms s a t u r a t e d atmosphere and assuming a I f t h e a i r i n DRAKE's e x p e r i m e n t was n o t s a t u r a t e d then better. AIR BUBBLES AND MELTING ELECTRIFICATION K a t e r d r o p s f r o z e n i n an a i r s t r e a m a t l o w t e m p e r a t u r e s w h i t e and opaque whereas d r o p s f r o z e n i n s t i l l bubbly c e n t r e variation i s consistent with t h e r e s u l t s obtained t h e f r e e z i n g r a t e s w o u l d be i n c r e a s e d and t h e agreement would be 8.5 paper. d u r i n g f r e e z i n g i t i s p o s s i b l e t o show t h a t the of e l e c t r i f i c a t i o n w i t h f r e e z i n g r a t e a t Durham ( F i g . 8 . 7 ) . 1 the (Fig. 8.8). are c o m p l e t e l y a i r near 0°C are c l e a r w i t h a The e f f e c t o f f r e e z i n g r a t e on m e l t i n g electrifi- c a t i o n may be due t o d i f f e r e n c e s i n t h e a i r b u b b l e s t r u c t u r e o f t h e p a r t i c l e s . 8 . 5 . 1 . The e f f e c t of t h e s o l u b i l i t y o f a i r on m e l t i n g The s o l u b i l i t y o f a i r i n w a t e r i n c r e a s e s the water decreases f o r temperatures of a i r trapped i n the temperatures. electrification. r a p i d l y as the t e m p e r a t u r e o f above 0 ° C ( F i g . 8 . 9 ) j t h e t o t a l ice i s probably greater i n i c e formed a t amount lower I n the absence o f d a t a f o r s u p e r c o o l e d w a t e r t h e v a l u e s o f s o l u b i l i t y f o r temperatures b e l o w 0 ° C have t o be o b t a i n e d by e x t r a p o l a t i o n . P r o v i d e d no a i r escapes d u r i n g f r e e z i n g , t h e amount o f a i r r e l e a s e d a t s u r f a c e o f a m e l t i n g i c e sphere is proportional s o l u b i l i t i e s o f t h e a i r i n w a t e r a t 0 ° C and a t temperature. at t o the d i f f e r e n c e i n the i n i t i a l The r a t i o o f t h e volumes o f a i r r e l e a s e d i s a p p r e c i a b l y l e s s than the v a r i a t i o n 1.0. As t h i s i n t h e amount o f m e l t i n g e l e c t r i f i c a t i o n f o r water f r o z e n at s i m i l a r temperatures 8.5) supercooling by i c e f r o z e n - 1 5 , - 1 0 and - 5 ° C as deduced f r o m F i g . 8 , 9 i s 2 . 9 : 1 . 8 : variation the ( f i g . 8 . 4 and i t seems l i k e l y t h a t t h e i n c r e a s e o f m e l t i n g e l e c t r i f i c a t i o n f r e e z i n g t e m p e r a t u r e i s due t o d i f f e r e n t a i r b u b b l e s i z e spectra with as w e l l as t h e d i f f e r e n t amounts o f a i r t r a p p e d i n t h e i c e . T h i s c o n c l u s i o n Fig.fc.10 Air bubbles in water drops frozen in still air A N umber of Max i ons MHky Bubbly Cylinders 5 0 Hro bubble 100 diameter 200 400 2o 1-1 3 t o -1 5 C 12- * i 4 - 20 - 12 -1 0 to -11-5 C - 4 - 20 - 16 - IZ - - 5 to-9 C 4 - 20 drops in each sample 71. i s r e i n f o r c e d by f i g . 8 . 7 w h i c h shows t h a t dependent 8.5.2. on the r a t e the e l e c t r i f i c a t i o n i s of f r e e z i n g r a t h e r than the temperature of f r e e z i n g . A i r b u b b l e s i n w a t e r drops f r o z e n i n s t i l l Generally the drops f r o z e n i n s t i l l by a s h e l l o f c l e a r ice. air. a i r had an opaque c e n t r e surrounded The volume o f t h e c e n t r a l r e g i o n i n c r e a s e d as f r e e z i n g temperature decreased. bubbly or m i l k y . highly the The i c e samples c o u l d be c l a s s i f i e d as M i l k y samples had a r e a s w h i c h were hazy even u n d e r t h e h i g h e r m a g n i f i c a t i o n r a n g e o f the m i c r o s c o p e and e i t h e r c o n s i s t e d o f bubbles s m a l l e r than 1 0 o r areas of small c r y s t a l s . In bubbly ice the b u b b l e s were s e p a r a t e d by c l e a r i c e and f e w were s m a l l e r t h a n 40|im d i a m e t e r . Fig, 8 . 1 0 shows t h a t as t h e f r e e z i n g t e m p e r a t u r e increases the ice particles are more l i k e l y t o be b u b b l y t h a n m i l k y and i n t h e r a n g e - 5 t o - 9 ° C about 80% were b u b b l y and o n l y b% m i l k y , whereas -13 and 70% o f t h e d r o p s f r o z e n between - 1 5 ° C were m i l k y and o n l y 15% b u b b l y . The maximum s i z e o f b u b b l e s d i d n o t v a r y a p p r e c i a b l y w i t h f r e e z i n g t e m p e r a t u r e but a t h i g h e r t e m p e r a t u r e s t h e mean s i z e was n e a r e r the maximum than f o r i c e f r o z e n a t lower temperatures. The t e n d e n c y f o r c y l i n d r i c a l b u b b l e s o f a b o u t 500 ^ m i n l e n g t h t o f o r m i n c r e a s e d w i t h t h e f r e e z i n g temperature. W a t e r d r o p s f r o z e n s l o w l y were l i k e l y t o l o s e a i r during f r e e z i n g and a i r b u b b l e s have been seen b u r s t i n g t h r o u g h t h e t h i n s h e l l d u r i n g the f i r s t 8.5.3 ice few minutes o f f r e e z i n g . A i r b u b b l e s i n w a t e r d r o p s f r o z e n i n an a i r s t r e a m . Water d r o p s f r o z e n i n an a i r s t r e a m a t 11 ms ^ and b e l o w a b o u t - 9 ° C are c o m p l e t e l y opaque even u n d e r t h e m i c r o s c o p e . They c o n t a i n a l a r g e number o f b u b b l e s o f t h e maximum d i a m e t e r ? w h i c h i s i n t h e r a n g e 25 t o 40jim. There a r e a l s o a l a r g e number o f s m a l l e r b u b b l e s o f a l l down t o t h e l i m i t o f r e s o l u t i o n w h i c h was a b o u t 5 j i m. temperature increased the bubble s i z e As t h e f r e e z i n g s p e c t r u m seemed t o b r o a d e n and by - 6 ° C t h e r e were a f e w b u b b l e s o f 100 \wi and an a p p r e c i a b l e of 50 ym d i a m e t e r . As t h e sizes number f r e e z i n g r a t e d e c r e a s e d t h e d r o p s became Fig. «H The charge separated bursting air Iribarne and of bubbles Mason 10 C h a r g e / v o l ume 1 per vol u m e (1967) Molar theory impurity concentration pC m g 10 o 10 I 10 10 40 Rubble Co diameter u rn 80 I OO IZO I GO 72. more c l e a r and a d r o p f r o z e n a t about t h e p e r c e n t a g e - 6 ° C was about 15% c l e a r ice. c l e a r ice i n a drop f r o z e n at -15°C i n T h i s was stagnant air. Melting, electrification annate fruftbl&& 9t5t4 The o b s e r v e d v a r i a t i o n o f the amount o f m e l t i n g with freezing rate suggests t h a t a i r bubbles s m a l l e r than about d i a m e t e r produce a p p r e c i a b l y more charge If electrification 50jim separation than l a r g e r bubbles. l a r g e enough c o n c e n t r a t i o n s o f b u b b l e s o f 1 0 | i m and l e s s are present, t h e n t h i s s i z e range w i l l of m e l t i n g 8.5.5. electrification ice. The b u b b l e - b u r s t i n g t h e o r y o f m e l t i n g The (fig. p l a y an i m p o r t a n t p a r t i n t h e electrification. b u b b l e - b u r s t i n g t h e o r y o f IRIBARNE and MASON ( 1 9 6 7 ) p r e d i c t s 8 . 1 l ) t h a t t h e charge s e p a r a t e d p e r u n i t volume o f a i r f a l l s o f - f -5 r a p i d l y as t h e b u b b l e d i a m e t e r i n c r e a s e s . of For a 10 molar s o l u t i o n i o n i c i m p u r i t i e s c o r r e s p o n d i n g t o a c o n d u c t i v i t y of 1.0 | i mho cm * t h e c h a r g e p e r volume i n c r e a s e s by an o r d e r o f m a g n i t u d e o v e r - t h e b u b b l e d i a m e t e r range 80 t o 20 yn. electrification agreement The particle on the The measured v a r i a t i o n o f m e l t i n g w i t h f r e e z i n g r a t e and b u b b l e s t r u c t u r e i s i n q u a l i t a t i v e with this theory. volume o f a i r r e l e a s e d f r o z e n a t about by the m e l t i n g o f a 4 mm d i a m e t e r -10 C i s o f t h e o r d e r o f 1 mm • The ice charge p a r t i c l e was measured t o be about 25 pC i f t h e i c e had a -5 c o n c e n t r a t i o n o f i o n i c i m p u r i t y o f 10 11 ms * a i r s t r e a m a t -10°C. p a r t i c l e w o u l d be a b o u t 5 0 ^ m. m o l a r and w e r e . f r o z e n i n an The maximum b u b b l e d i a m e t e r i n such a As b u b b l e s o f 100^ m d i a m e t e r produce -3 as much as 500 pC mm , i f a l l t h e b u b b l e s t r a p p e d i n the t h e s u r f a c e t h e t h e o r y p r e d i c t s a f a c t o r o f 100 g r e a t e r is observed. ice reach charging than One p o s s i b l e e x p l a n a t i o n i s t h a t many o f t h e smallest will d i s s o l v e b e f o r e r e a c h i n g t h e s u r f a c e and t h e b u b b l e s i z e will be g r e a t l y a l t e r e d by t h e c o a l e s c e n c e o f b u b b l e s . bubbles spectrum Furthermore t h e p r e d i c t i o n s o f t h e t h e o r y may be i n e r r o r f o r d i a m e t e r s as l o w as 73. 2 0 j i m as t h e t h e o r y depends on t h e b u b b l e - b u r s t i n g p r o c e s s r e m a i n i n g t h e same f o r w i d e l y d i f f e r e n t s i z e s o f b u b b l e s . The IRIBARNE and MASON t h e o r y has o n l y been, c o n f i r m e d e x p e r i m e n t a l l y f o r b u b b l e d i a m e t e r s g r e a t e r t h a n 160 Rm. 8.5.6 A i r b u b b l e s i z e s and t h e r a t e of advance of t h e ice sheet. A c c o r d i n g t o BROWNSCOMBE and HALLETT ( 1 9 6 7 ) t h e s i z e s and number of bubbles f o r m e d by t h e f r e e z i n g o f w a t e r depend on t h e r a t e o f advance o f t h e i c e s h e e t and t h e e x t e n t has measured t o w h i c h p r e s s u r e can b u i l d up* the average d i a m e t e r o f bubbles of water at various f r e e z i n g rates TABLE 8 . 1 . (Table CARTE f o r m e d by f r e e z i n g (l96l) layers 8.1). The r a t e of advance o f %he i c e s h e e t and s i z e o f bubbles,, CARTE d i a m e t e r pm (l96l) g r o w t h r a t e mm min ^ 400 0.2 200 0.5 100 2*0 50 5.0 The r a t e o f advance o f t h e i c e s h e e t i n a w a t e r d r o p f r e e z i n g a t - 1 2 ° C i n an a i r s t r e a m f l o w i n g a t 11 ms ^ i s 2 » 4 mm m i n Table&L t h i s r a t e o f f r e e z i n g c o r r e s p o n d s about 90 Jim. According to t o a mean b u b b l e d i a m e t e r o f T h i s v a l u e i s 3 t o 4 t i m e s t h e mean bubble s i z e observed i n t h e f r o z e n w a t e r d r o p s b u t t h e d i f f e r e n c e may be due t o t h e up o f p r e s s u r e d u r i n g t h e f i n a l water drops f r e e z i n g i n s t i l l stages o f f r e e z i n g o f the d r o p . air a typical that the observations For speed o f t h e i c e s h e e t w o u l d ' be 0 . 2 mm m i n * c o r r e s p o n d i n g t o a b u b b l e d i a m e t e r o f 400 jim. expected build- I t would be o f GARTE w o u l d a p p l y more c l o s e l y t o f r e e z i n g o f ai w a t e r l a y e r on t h e s u r f a c e o f a hailstone. the 74. 8 . 6 COMPARISON WITH PREVIOUS EXPERIMENTS. The m a g n i t u d e o f charge s e p a r a t e d by t h e m e l t i n g o f a r t i f i c i a l cloud w a t e r was f o u n d t o be an o r d e r o f m a g n i t u d e l e s s t h a n t h a t o b s e r v e d DRAKE ( 1 9 6 8 ) . T h i s may be e x p l a i n e d by t h e d i f f e r e n t r a t e s o f f r e e z i n g o £ t h e i c e samples. n o t be o b s e r v e d Although vigorous convection i n the melt water could i t seems l i k e l y t h a t t h i s was t h e cause o f t h e d i f f e r e n c e i n e l e c t r i f i c a t i o n a t h i g h and l o w m e l t i n g r a t e s i n f i a s . 8 . 2 and 8..3 There i s .some e v i d e n c e described The suggest t h a t t h e e f f e c t s o f c o n v e c t i o n on t h e e l e c t r i f i c a t i o n i m p o r t a n t f o r melting r a t e s as l o w as 5 mg m m large t h a t the h i g h e r the f r e e z i n g r a t e ^ a t which the increase o f e l e c t r i f i c a t i o n i s apparent. enough a i r by provided the results are ice contains bubbles. I t has been shown i n s e c t i o n 8 . 3 t h a t the o b s e r v a t i o n s made u s i n g the l o o p s u p p o r t o f DRAKE do n o t d i f f e r n o t i c e a b l y f r o m t h o s e made w i t h a more natural support which p e r m i t s the p a r t i c l e t o r o t a t e . can be used So DRAKE*s observations i n assessing the importance of m e l t i n g e l e c t r i f i c a t i o n f o r i c e which has been f o r m e d a t h i g h f r e e z i n g r a t e s and w h i c h c o n t a i n s many b u b b l e s s m a l l e r t h a n 3 0 t o 40 p m d i a m e t e r . present The r e s u l t s obtained i n the i n v e s t i g a t i o n are a p p l i c a b l e t o t h e s t u d y o f i c e f r o z e n a t l o w f r e e z i n g r a t e s where an a p p r e c i a b l e contained i n bubbles l a r g e r f r a c t i o n of the trapped a i r is t h a n 40 t o 50 p m . The o b s e r v e d dependence o f m e l t i n g e l e c t r i f i c a t i o n on t h e size of a i r b u b b l e s a g r e e s q u a l i t a t i v e l y w i t h t h e IRIBARNE and MASON (1967) t h e o r y o f the e l e c t r i f i c a t i o n of b u r s t i n g bubbles at a water s u r f a c e . T h i s c o n f i r m s t h e v i e w o f DINGER and GUNN ( 1 9 4 6 ) and DRAKE ( 1 9 6 8 ) t h a t t h e e l e c t r i f i c a t i o n o f m e l t i n g i c e i s due t o t h e b u r s t i n g o f a i r bubbles. lb. C H A P T E R 9 THE EFFECT OF CARBON DIOXIDE ON MELTING ELECTRIFICATION 9.1 CARBON DIOXIDE AND LABORATORY EXPERIMENTS 9.1*1 The Matthews and Mason experiment One of t h e reasons put f o r w a r d t o e x p l a i n why MATTHEWS and MASON (1963) f a i l e d t o d e t e c t charging when i c e and snow were melted has been t h e r e g u l a r use o f d r y i c e i n the l a b o r a t o r y . A l s o i n two out o f three experiments the water was frozen i n close p r o x i m i t y t o d r y i c e . DINGER (1964) has p o i n t e d out t h a t the presence o f carbon d i o x i d e near the apparatus was s u f f i c i e n t to reduce the e l e c t r i f i c a t i o n found i n t h e Dinger-Gunn experiment (1946). However? as contamination o f t h e w a t e r and t h e a c t u a l method o f m e l t i n g also have a l a r g e e f f e c t on the charge separated? the presence o f carbon d i o x i d e may not have been t h e only cause of the MATTHEWS and MASON n u l l result. 9.1.2 The Dinaer-Gunn experiment. DINGER and GUNN (1946) found t h a t water f r o z e n i n an atmosphere o f carbon d i o x i d e produced no e l e c t r i f i c a t i o n when melted. The i c e samples had a t y p i c a l volume o f 2 ml and were melted i n t r a y s , w i t h some v e n t i l a t i o n . 9.1.3 Drake's experiment* DRAKE (1968), i n c o n t r a s t t o most o f t h e previous workers? found t h a t water f r o z e n i n the presence o f carbon d i o x i d e produced as much as +1.3 pC mg ^ on m e l t i n g . The i c e was made from small water drops and carbon d i o x i d e was bubbled t h r o u g h the water before use. However, i f vigorous convection d i d not d e v e l o p i n the m e l t w a t e r , e l e c t r i f i c a t i o n was i n h i b i t e d by the presence o f carbon d i o x i d e . 76. 9.2 THE IMPORTANCE OF CARBON DIOXIDE IN MELTING ELECTRIFICATION 9.2.1 The double l a y ^ r t h e o r y and the e f f e c t s of carbon d i o x i d e . According t o the e l e c t r i c a l double l a y e r t h e o r y o f b u b b l e - b u r s t i n g e l e c t r i f i c a t i o n , the e f f e c t o f d i s s o l v e d carbon d i o x i d e should be the same as t h a t of a s i m i l a r c o n c e n t r a t i o n o f d i s s o l v e d ions o f any species. This has been confirmed by the experiment o f IRIBARNE and MASON (1967). The reason f o r carbon d i o x i d e being more a c t i v e than most atmospheric gases i s t h a t i t i s h i g h l y s o l u b l e i n water and forms carbonic a c i d which d i s s o c i a t e s i n t o hydrogen and b i c a r b o n a t e i o n s . I f melting ice e l e c t r i f i c a t i o n i s caused by t h e release of trapped a i r bubbles, then one would expect the presence o f c arbon d i o x i d e i n the water would i n h i b i t e l e c t r i f i c a t i o n . 9.2.2 The e f f e c t o f atmospheric carbon d i o x i d e . GLUCKAUF (1944) giyes examples o f carbon d i o x i d e c o n c e n t r a t i o n a t the ground as 0.031 the - 0.035% a t Kew and 0.035 - 0.037% i n c e n t r a l London. Inside l a b o r a t o r y the concent r a t i o n s tend t o be h i g h e r and can range from 0.04 to 0.1%. 1 away from t h e ground, the c o n c e n t r a t i o n of carbon d i o x i d e seems t o be independent o f a l t i t u d e , c e r t a i n l y up t o 10 km. GLUCKAUF g i v e s an average value o f 0.025% f o r 4 t o 10 km over England and KEELING (1968) found c o n c e n t r a t i o n s o f 0.031% over Hawaii and A n t a r c t i c a between the 500 and 700 mb levels. KAYE and LABY (1970) give t h e s o l u b i l i t y of c arbon d i o x i d e i n water as loO ml of CO^ P e r m l or * water a t 15°C and 1 atmosphere. Taking the c o n c e n t r a t i o n o f atmospheric carbon d i o x i d e as 0.03% and assuming a l l the CO^ r e a c t s w i t h the w a t e r t o form carbonic a c i d , t h i s i m p l i e s a t y p i c a l e q u i l i b r i u m c o n c e n t r a t i o n o f 5 x 10 Molar o f carbonic a c i d . This value w i l l remain n e a r l y c o n s t a n t w i t h a l t i t u d e as the e f f e c t s o f decreasing pressure and temperature on the s o l u b i l i t y tend t o cancel o u t . Unless carbon d i o x i d e i s more e f f e c t i v e i n r e d u c i n g e l e c t r i f i c a t i o n than s i m i l a r c o n c e n t r a t i o n s o f o t h e r i o n i c species one would e x p e c t t h a t , i n the c o n c e n t r a t i o n found i n the atmosphere, i t would reduce the 77. e l e c t r i f i c a t i o n t o about 60% o f the value f o r p u r e s t water (IRIBARNE and MASON, 1967). The e f f e c t of dry i c e i n t h e l a b o r a t o r y may be more s e r i o u s , because o n l y a 3% c o n c e n t r a t i o n o f carbon d i o x i d e i n the a i r i s needed t o reduce the charge produced by the b u r s t i n g o f a 100 j*m r a d i u s bubble to an i n s i g n i f i c a n t l e v e l . 9.3 AN EXPERIMENT TO DETERMINE THE EFFECT OF ATMOSPHERIC CARBON DIOXIDE. 9.3.1 Experimental details Some o f the d i s s o l v e d carbon d i o x i d e was removed from d e i o n i z e d water by bubbling w i t h n i t r o g e n and a l l o w i n g the water t o stand i n a n i t r o g e n atmosphere. The c o n c e n t r a t i o n o f carbon d i o x i d e could be r e g u l a t e d by exposing the water t o t h e atmosphere.. This water was used t o make the ice spheres, which were then melted under constant c o n d i t i o n s i n the wind tunnel. Care was taken t o nucleate the water drops 4 t o 5 minutes a f t e r being placed i n the r e f r i g e r a t o r , i n order t o reduce the amount o f carbon d i o x i d e absorbed d u r i n g the c o o l i n g o f the dropo The ice sphere was then melted on a p l a t i n l u m w i r e support i n the wind t u n n e l . 903.2 The use o f e l e c t r i c c o n d u c t i v i t y measurements t o evaluate the CQ^ concentration. Carbon d i o x i d e r e a c t s w i t h water t o produce carbonic a c i d , which i s p a r t l y d i s s o c i a t e d i n t o hydrogen and bicarbonate CO + H O ^ 2 2 H i o n s , thus + C0 ^H +HC0 ~ 2 3^ *3 0 o As carbonic a c i d i s weak a c i d , Ostwald's d i l u t i o n law (Eqrw 9.1) may be used t o evaluate the v a r i a t i o n o f c o n d u c t i v i t y w i t h c o n c e n t r a t i o n o f a c i d ; K= L C L ( L -L) 9.1 2 o o where K i s the i o n i z a t i o n constant (4.5 x 10 C i s t h e c o n c e n t r a t i o n of c a r b o n i c a c i d , L at i n f i n i t e d i l u t i o n Co q g equiv 1 a t 2b C) the e q u i v a l e n t conductance and L the e q u i v a l e n t conductance a t c o n c e n t r a t i o n Equivalent conductance i s d e f i n e d as the conductance of a s o l u t i o n c o n t a i n i n g one gm e q u i v a l e n t o f s o l u t e when measured between p a r a l l e l e l e c t r o d e s which are 1 cm a p a r t and l a r g e enough i n area t o c o n t a i n the F i g.9 1 T he e f f e c t of dissolved CO^on de ion i zed conductivity water C on d a c t i v i t y 0*7 ta mho c m 1 05 ' 0-3 - o\ -i 2 4 r 6 to 3 C o n c e n t r a t i o n of c a r b o n i c x 1 C f Molar acid 6 Fig.9-2 C h a r g e on the m e l t w a t e r made f r o m w a t e r of with 4mm diameter different ice C O ^ levels Charge + PC 6 - 4 - 2- —? 1 p— o 1 o-3 0 Co n due \ «v ity p mho c m 1 4 — i — 0-6 a 7 spheres 78. the necessary volume o f s o l u t i o n . By r e w r i t i n g the Ostwald d i l u t i o n l a w and s u b s t i t u t i n g the value f o r L 2 o f 395 Hmho cm gm e q u i v " L = b - 9 x I0~ 1 quoted by MACINNES ( l 9 6 l ) ; 8 x 10" ± \ The C 9 + 7 x l Q ^ 2 9 # 2 C s p e c i f i c c o n d u c t i v i t y can be obtained by m u l t i p l y i n g t h e e q u i v a l e n t conductance by t h e c o n c e n t r a t i o n , e n a b l i n g the v a r i a t i o n o f t h e c o n d u c t i v i t y of t h e s o l u t i o n o f carbonic a c i d t o be p l o t t e d against c o n c e n t r a t i o n ( f i g . 9.1)• When n i t r o g e n was bubbled through the deionized water samples t o remove the CO^j the c o n d u c t i v i t y f e l l V ~*1 k "1 from 0.75jimho cm t o a minimum of 0.15 ^mho cm which i m p l i e s t h a t t h e c o n d u c t i v i t y due t o carbon d i o x i d e i n e q u i l i b r i u m w i t h the water was 0.6|i mho gm ^. From f i g . 9-1, the c o n c e n t r a t i o n o f carbonic a c i d was 6 x 10 ^ N which agrees w i t h t h a t c a l c u l a t e d i n s e c t i o n 9.2.2 caused by a 0.03% c o n c e n t r a t i o n o f CO^ i n the atmosphere. 9.3.3 The e f f e c t o f GO^ c o n c e n t r a t i o n s on m e l t i n g e l e c t r i f i c a t i o n . The 10 f r o z e n water drops were made f r o m water which contained from 7 x M t o l e s s t h a n 10 M carbonic a c i d . The a c t u a l value o f the lower l i m i t of the carbonic a c i d c o n c e n t r a t i o n could n o t be determined because t h e c o n c e n t r a t i o n o f metal and non metal ions was n o t known. The icewas melted s l o w l y , t h e 4 mm spheres t a k i n g about 8 minutes t o m e l t . The charge c a r r i e d by the meltwater f o r water o f d i f f e r e n t concentrations o f carbon d i o x i d e i s p l o t t e d i n f i g . 9.2. There i s l i t t l e s i g n i f i c a n t v a r i a t i o n of the charging w i t h carbon d i o x i d e c o n c e n t r a t i o n . These r e s u l t s may be compared w i t h e a r l i e r measurements made w i t h water drops which had stood f o r about an hour before f r e e z i n g and were t h e r e f o r e i n e q u i l i b r i u m w i t h atmospheric CO^ (Table 9.1)• The estimates o f CO^ c o n c e n t r a t i o n were d e r i v e d by the method o u t l i n e d i n s e c t i o n 9.4.1. 79. TABLE 9.1 E f f e c t of CO^ c o n c e n t r a t i o n on m e l t i n g e l e c t r i f i c a t i o n , Percentage o f the c o n c e n t r a t i o n o f CO, present i n e q u i l i b r i u m w i t h water a t Charge pC +15°C Number o f drops 160 3.0 ± .8 7 180 4.0 ± 1.0 8 260 4.9 + 1.0 17 Table 9.1 suggests t h a t t h e r e i s no s i g n i f i c a n t d i f f e r e n c e between the charging produced by any of t h e 3 sets o f m e l t i n g i c e spheres. However, i f carbon d i o x i d e does have an important e f f e c t on m e l t i n g e l e c t r i f i c a t i o n these r e s u l t s could be explained by carbon d i o x i d e being absorbed by a water drop d u r i n g the m e l t i n g process ( c f s e c t i o n 9.4.2). 9.4 THE ABSORPTION OF CARBON DIOXIDE BY A WATER DROP 9.4.1 Absorption by a s t a t i o n a r y drop. A review paper by LEWIS and WHITMAN (1924) shows t h a t the c h i e f cause of r e s i s t a n c e o f a water drop t o absorbing l i q u i d a t t h e surface o f t h e drop. gaseous CO^ i s a t h i n f i l m o f Inside t h i s f i l m , which i s t y p i c a l l y 3|nn t h i c k (WHITMAN, LONG and WANG 1926), t h e l i m i t i n g f a c t o r i s the d i f f u s i o n o f CO^ through a r e l a t i v e l y h i g h c o n c e n t r a t i o n of carbon d i o x i d e solution. The r a t e of m i x i n g i n s i d e the drop only l i m i t s t h e a b s o r p t i o n process by reducing the c o n c e n t r a t i o n g r a d i e n t across the surface film» By a p p l y i n g the t h e o r y o f t h e d i f f u s i o n o f gases through a f i l m o f stagnant l i q u i d (Appendix 2 ) , t h e f r a c t i o n f o f the f i n a l e q u i l i b r i u m amount-'of CO absorbed i n a water drop can be d e r i v e d . For a 4 mm diameter drop f o r t < ! 0 0 s n/2 2 t n and f o r t > 100 s 3k 0.44e x p H iooj <t-i°°)J 0> 0) 0> 0; u O u o r- 00 cn o < 4 I 5 O o o> u o O ^ O 0* tn 80. "•6 where the p e r m e a b i l i t y c o e f f i c i e n t k l 0 Q = 2.8 x 10 a f t e r the s t a r t o f a b s o r p t i o n and D i s the d i f f u s i o n ~1 ms , t i s the time coefficient. The t w o equations 9.3 and 9-4 describe d i f f e r e n t stages i n the a b s o r p t i o n o f gas. In the f i r s t s t a g e , the p e r m e a b i l i t y o f the surface l a y e r decreases as the GO^ l e v e l r i s e s , and i n the second the l a y e r i s s a t u r a t e d w i t h CC>2 and the p e r m e a b i l i t y remains constant. These r e s u l t s are p l o t t e d i n f i g . 9-3, which shows t h a t a f t e r 2.5 min the drop has absorbed 66% o f i t s e q u i l i b r i u m value of CO^, and a f t e r 7 min 90% o f the C 0 has been 2 absorbed. 9.4.2. A b s o r p t i o n by a f a l l i n g drop. Much o f the experimental work on a b s o r p t i o n by water drops has been c a r r i e d out on f a l l i n g drops e.g. by GARNER and LANE (1959), LEWIS and WHITMAN (1924) and LEWIS e t a l . (1926). A t y p i c a l value f o r the time taken f o r 90% a b s o r p t i o n f o r a f a l l i n g 4 mm diameter drop i s 5 seconds (GARNER and LANE (1959). This i s two orders o f magnitude l e s s than f o r a drop i n stagnant a i r and i s due t o the presence o f convection and the d i s t u r b e d nature o f the surface f i l m i n a f a l l i n g drop. 9.5 CARBON DIOXIDE LEVELS IN PREVIOUS LABORATORY EXPERIMENTS 9.5.1 The Dinoer-Gunn experiment. I f t h e r a t e o f a b s o r p t i o n o f GO^ i s g r e a t l y enhanced by p l a c i n g a water drop i n a s t r e a m of the gas, the r a t e o f d e s o r p t i o n o f CO^ w i l l a l s o be increased i n a v e n t i l a t e d atmosphere. Dinger-Gunn experiment The r a t e of d e s o r p t i o n i n the ( s e c t i o n 2 . l ) may be estimated by c o n s i d e r i n g a r e c t a n g u l a r shaped volume o f water, o f depth d and surface area A, placed i n a cubic c o n t a i n e r so t h a t o n l y the area A has access t o the a i r I t seems l i k e l y t h a t , because the water was s h e l t e r e d from the f a n by the s i d e s o f the small c o n t a i n e r , the surface f i l m was not d i s t u r b e d , and the GO^ was t r a n s f e r r e d across the surface by molecular d i f f u s i o n . Appendix 2.2 the value o f f i s given by From 81. I f we assume t h a t the surface f i l m i s s a t u r a t e d w i t h CO^, then k = 2.8 -6 ^ - l x 10 m s . I n t h i s experiment the depth o f i c e was about 10 mm, so i f one considers a l a y e r o f water 1 mm t h i c k on the surface o f t h e i c e t h e n , according to e q u a t i o n 9.5, the time constant d/k w i l l be about 400 seconds. As the t o t a l time f o r a l l the i c e t o m e l t was o f t h e order o f 100 seconds i t i s suggested t h a t t h e meltwater d i d c o n t a i n approximately the same amount of CO^ as t h e o r i g i n a l water from which t h e i c e was made. This experiment would t h e r e f o r e measure t h e e f f e c t o f CO^ on m e l t i n g e l e c t r i f i c a t i o n . 9.5.2 The experiment o f DRAKE. The time constant f o r t h e a b s o r p t i o n and t h e r e f o r e a l s o d e s o r p t i o n o f CO^ by a f a l l i n g drop i s l e s s than than the m e l t i n g t i m e . the b u r s t i n g bubbles 5 s, which i s over a f a c t o r o f 10 l e s s So seems probable t h a t t h e meltwater surrounding e i n DRAKE's experiment contained v e r y l i t t l e though t h e i c e was made from water w i t h a h i g h CO^ content. v e n The r a t e of loss f o f CO^ from a small a i r bubble a f t e r release from t h e i c e can be estimated (Appendix 2.3) using the f i l m t h e o r y o f gas a b s o r p t i o n ; -g 2 -1 where r i s the r a d i u s of the bubble and D = 2 x 10 ms For a t y p i c a l 2 0 ^ m bubble, 99% of t h e CO^ i s l o s t i n t h e f i r s t 0.8 s a f t e r water comes i n c o n t a c t w i t h t h e bubble. This suggests that the c o n c e n t r a t i o n of CO^ i n t h e meltwater w i l l govern t h e CO^ content of the double l a y e r a t t h e surface o f the bubble on b u r s t i n g , r a t h e r than t h e i n i t i a l gas content o f t h e bubble. As the meltwater loses most of i t s CO^ i n seconds, t h e c o n c e n t r a t i o n o f CO^ i n t h e p a r t l y molten drop i s probably very close t o t h a t due t o t h e m e l t i n g environment, and i s n o t dependent on t h e f r e e z i n g environment. 9.6 I t i s suggested CONCLUSION t h a t t h e reason f o r t h e f a i l u r e o f DRAKE t o f i n d that CO^ i n h i b i t s m e l t i n g e l e c t r i f i c a t i o n may be due t o t h e absence o f CO^ i n the meltwater of h i s samples. The apparatus o f DINGER and GUNN would 82. measure the e f f e c t of CO - The MATTHEWS and MASON n u l l r e s u l t s were obtained w i t h ice i n bulk fcr^a, where any CO^ i n t r o d u c e d d u r i n g the f o r m a t i o n o f the i c e would n o t e a s i l y leak away during m e l t i n g - I n order t o confirm t h i s t h e o r y , i c e spheres should be melted i n an atmosphere of CO^ when, according t o t h e double l a y e r t h e o r y of m e l t i n g e l e c t r i f i c a t i o n , the charging should be reduced. I t i s hoped t o c a r r y out t h i s experiment a t Durham s h o r t l y . 83. CHAPTER10 THE ELECTRICAL EFFECTS OF THE MELTING OF REAL PRECIPITATION 1Q.1 THE LOCATION OF THE LOWER POSITIVE CHARGE 10.1.1 The l o c a t i o n deduced from l a b o r a t o r y experiments. The way i n which r e a l i c e p a r t i c l e s m e l t w h i l e f a l l i n g from the 0°C l e v e l i n convective clouds i s s i m i l a r t o the behaviour o f the m e l t i n g i c e p a r t i c l e s i n the wind t u n n e l . I n both cases the temperature r i s e s d u r i n g the course o f m e l t i n g although the temperature of the a i r i n the wind t u n n e l more s l o w l y d u r i n g the f i r s t minute of m e l t i n g . increases T y p i c a l l y 40% of the i c e i s melted i n the l a s t minute of m e l t i n g i n the tunnel compared to 50% as c a l c u l a t e d by MASON (1956) f o r a 4 mm s o l i d i c e sphere f a l l i n g i n a saturated atmosphere from the 0°C l e v e l . I n the l a b o r a t o r y between 50 and 90% of a l l the charge was separated d u r i n g the l a s t minute o f m e l t i n g when the average m e l t i n g r a t e ranged from 7 to 18 mg min As MASON c a l c u l a t e d t h i s average value t o be 14 mg min ^ f o r a 4. mm p a r t i c l e m e l t i n g i n a c l o u d , i t seems t h a t most of the charge separation on such a p a r t i c l e occurs d u r i n g the l a s t minute of m e l t i n g C e r t a i n l y the l a b o r a t o r y r e s u l t s show t h a t the amount o f charging d u r i n g the f i r s t minute of m e l t i n g i s l i k e l y t o be n e g l i g i b l e ( c f . f i g . 7.9). For a 4 mm s o l i d i c e p a r t i c l e MASON estimated t h a t the l a s t 50% of the 0 raass melted below the +6i2 C l e v e l o r 1km below the 0°C l e v e l . One might t h e r e f o r e expect t h e centre o f charge s e p a r a t i o n to l i e a t about + 8°C and 1.2 km below the 0°C l e v e l . The smaller the m e l t i n g p a r t i c l e , the higher i n the cloud i t w i l l m e l t , so 2 mm p a r t i c l e w i l l have h a l f melted by 450 m below the 0°C l e v e l - However small ice p a r t i c l e s which m e l t higher i n the cloud w i l l m e l t a t a lower r a t e due t o t h e c o o l e r environment, so t h e y may c o n t r i b u t e less t o the cloud e l e c t r i f i c a t i o n . also m e l t higher i n the c l o u d ; according Graupel w i l l to MASON a 3 mm diameter graupel p e l l e t of s p e c i f i c g r a v i t y 0.3 w i l l lose the l a s t 50% of i t s mass between 300 and 600 m below the 0°C l e v e l . C l e a r l y the l o c a t i o n o f the charged Fig. 10*1 The location t of the Schonland No of and lower positive charge Malan(1951) observations -3 -Z 22 /8 2 J4 Simpson and -2 R o b i n s o n (1941) 4 3 2 -2 Reynolds and -6 -lo't -6 -\0°c Neil! ( 1 9 5 5 ) 3 2 6 2 Tempera ture ALSO Kuettner (1950) 12 out C l a r e n c e and M a l a n ( 1 9 5 7 ) of 5 0 AO # higher than+2 C observations level average + S°C 84. r e g i o n caused by m e l t i n g p r e c i p i t a t i o n depends very much on the size and density of the i c e p a r t i c l e s . 10.1.2 The e f f e c t of the downdrauaht. I f t h e m e l t i n g p a r t i c l e s are fal l i n g i n a downdraught which may be up 1 to 10 ms" (BYERS and BRAHAM, #1953) then t h e p o s i t i o n of t h e charged r e g i o n produced by the m e l t i n g i c e may be lower than i f the p a r t i c l e s melted i n t h e updraught. I n the downdraught the n e g a t i v e l y charged d r o p l e t s w i l l be c a r r i e d down below t h e 0°C l e v e l and w i l l tend t o n e u t r a l i z e t h e p o s i t i v e charge on t h e m e l t i n g p r e c i p i t a t i o n . The speeds o f t h e downdraught measured by BYERS and BRAHAM were i n t h e range 5 t o 10 ms * which i s o f the same magnitude as t h e f a l l s p e e d s o f p a r t i c l e s o f 2 t o 5 mm diameter, so t h i s e f f e c t may w e l l be i m p o r t a n t . I f t h e downdraught i s i n c l i n e d t o the v e r t i c a l t h e m e l t i n g p r e c i p i t a t i o n may f a l l c l e a r e i t h e r i n t o t h e updraught or i n t o a r e l a t i v e l y motionless p a r t o f the cloud. 10.1.3 The measured l o c a t i o n o f the lower p o s i t i v e charge. A summary o f some experiments i n l o c a t i n g t h e lower p o s i t i v e charge i n thunderclouds i s o u t l i n e d i n Table 1.3. The mean temperatures a t which the charge was found v a r i e d from -3 t o +8°C. A d i r e c t comparison o f these r e s u l t s i s d i f f i c u l t because o f the d i f f e r e n t methods o f measurement and because the v a r i a t i o n of temperature w i t h a l t i t u d e was u s u a l l y i n f e r r e d from d i s t a n t radiosonde measurements and an estimate of t h e h e i g h t o f cloud base. These temperature measurements are l i k e l y t o be about 2°C too high according to BYERS and BRAHAM (1949) i f the charge r e g i o n i s l o c a t e d i n t h e downdraught and 2°C too low i f i n t h e updraught. F i g . 10.1 shows t h e d i s t r i b u t i o n o f l o c a t i o n s of t h e charge found by 3 observers who published i n d i v i d u a l as w e l l as mean values. The r e s u l t s o f SCHONLAND and MALAN ( l 9 5 l ) p o i n t towards a charge d i s t r i b u t i o n which can occur a t any l e v e l near and below the 0°C l e v e l and perhaps i s best explained by r i s i n g p o i n t discharge ions caught i n the updraught (MALAN. (1952).) The r e s u l t s of REYNOLDS and NEILL (1955) c e r t a i n l y do not j u s t i f y p l a c i n g the mean l o c a t i o n o f t h e charge a t -3°C as i n Table 1.3. KUETTNER (1950) has provided 85. perhaps the most r e l i a b l e estimate o f t h e p o s i t i o n o f the charge by studying the sign o f t h e p o t e n t i a l g r a d i e n t i n the c e n t r e o f p i e c f i p i t a t i o n o r l i g h t n i n g a c t i v i t y i n thunderclouds on t h e Zugspitze. On 50 occasions the charge was l o c a t e d above t h e +8°C l e v e l and on 12 above t h e +2°C l e v e l . I t i s p o s s i b l e t h a t t h e mountain may have a f f e c t e d the thunderstorm but these r e s u l t s p o i n t t o a t h e o r y o f e l e c t r i f i c a t i o n t h a t does not i n v o l v e the m e l t i n g o f i c e . CLARENCE and AAA LAN (1957) o n l y quote average r e s u l t s f o r the l o c a t i o n of the lower p o s i t i v e 10.14 charge. Conclusion From t h e previous s e c t i o n i t appears t h a t i t i s not p o s s i b l e t o s t a t e a l o c a t i o n f o r t h e lower p o s i t i v e charge o r even be sure t h a t t h e r e i s o n l y one type o f lower p o s i t i v e charge. I t may be t h a t the South A f r i c a n measurements have described a cloud o f p o i n t discharge ions whereas the European and American o b s e r v a t i o n s have described a charge c a r r i e d by the precipitation. C l e a r l y i t i s not p o s s i b l e t o say t h a t t h e measured l o c a t i o n of t h e charge precludes o r supports a m e l t i n g i c e theory. I f m e l t i n g i c e i s r e s p o n s i b l e then t h e l o c a t i o n o f t h e charge w i l l depend on the mean d e n s i t y and diameter of the m e l t i n g p a r t i c l e s . The motion of the a i r i n the r e g i o n o f t h e p r e c i p i t a t i o n may also be important and t h e mechanism should be more a c t i v e a t the edge o f the downdraught or i n t h e updraught. This l o c a t i o n agrees w i t h t h e p o s i t i o n o f t h e lower p o s i t i v e charge deduced by WILLIAMS (1958) from a study o f l i g h t n i n g f l a s h e s t o ground. 10.2 SOLID PRECIPITATION IN THUNDERSTORMS 10.2.1 C l a s s i f i c a t i o n of s o l i d p r e c i p i t a t i o n . , There i s some confusion i n t h e l i t e r a t u r e concerning t h e c l a s s i f i c a t i o n of s o l i d p r e c i p i t a t i o n and i n p a r t i c u l a r the word g r a u p e l . The Japanese e.g. NAKAYA and TERADA (1935) , d e s c r i b e graupel as having a mean s p e c i f i c g r a v i t y o f 0.13 agreeing w i t h t h e American ARENBERG ( l 9 4 l ) who gives a value o f 0.2 WEICKMANN(1953) and KEUTTNER (1950) r e f e r t o graupel as having a s p e c i f i c g r a v i t y o f about 0.6 and LIST (1965) suggests an 86. upper value o f 0.8. As LIST's s t u d i e s o f t h e s t r u c t u r e o f i c e p a r t i c l e s were a main p a r t o f h i s work h i s c l a s s i f i c a t i o n w i l l be used i n t h i s t h e s i s . Snow p e l l e t s These are l i g h t and opaque e i t h e r roughly c o n i c a l o r s p h e r i c a l p a r t i c l e s o f s p e c i f i c g r a v i t y 0„1 t o 0.3. They are formed according t o ARENBERG (1941) and NAKAYA and TERADA (1935) by the a c c r e t i o n of cloud d r o p l e t s onto a f a l l i n g snow c r y s t a l . Graupel Graupel p e l l e t s are white and opaque and r o u g h l y s p h e r i c a l i n shape w i t h s p e c i f i c g r a v i t y up t o 0.8 and diameters up t o 5mm. They d i f f e r from snow p e l l e t s i n having an i c e framework i n which a c r y s t a l l i n e s t r u c t u r e can be i d e n t i f i e d . WEICKMAN (1953), from h i s experiences on Mount Hohenpeissenberg considers t h a t the f o l l o w i n g d e s c r i p t i o n o f LITTLE (1940) describes them w e l l . " A l l the stones (average diameter some 5 mm) examined showed a d e f i n i t e c r y s t a l l i n e s t r u c t u r e , being i n the form o f a s e c t o r o f a sphere, t h e angle subtended approximate a t the c e n t r e being 90°. I t was not p o s s i b l e t o i d e n t i f y the form o f the i n d i v i d u a l c r y s t a l s , but they r a d i a t e d out from the apex of the s tone g i v i n g a s t r e a k y appearance at the s p h e r i c a l face as i f t h e stone were composed o f a bundle o f f i b r e s " . Graupel can e i t h e r be formed on a c r y s t a l o r a f r o z e n cloud d r o p l e t . Small h a i l LIST (1965) describes small h a i l as being semi-transparent p a r t i c l e s o f s i m i l a r size t o graupel but w i t h a more rounded appearance and a s p e c i f i c g r a v i t y o f 0.8 t o Q.,99. They may c o n s i s t p a r t l y o f l i q u i d water and grow from graupel by the i n t a k e of water* i n t o t h e a i r c a p i l l a r i e s of the i c e framework. Hailstones H a i l s t o n e s g e n e r a l l y have a layered c o n s t r u c t i o n and are l a r g e r than small h a i l . They may take a v a r i e t y o f shapes sometimes w i t h lobes. 10.2.?. Observations o f s o l i d p r e c i p i t a t i o n i n thunderclouds. There are very few o b s ervations of p r e c i p i t a t i o n p a r t i c l e s which were made i n thunderclouds and t h e d e s c r i p t i o n s t h a t are a v a i l a b l e were u s u a l l y made as a s u b s i d i a r y p a r t of an e l e c t r i c a l o r dynamical study. The o b s e r v a t i o n s f a l l i n t o two types> those made from mountain were immersed i n t h u n d e r c l o u d s , and a i r c r a f t o b s e r v a t i o n s . s t a t i o n s which 87. WEICKMANN (1953) observed t h a t graupel was t h e most common form o f s o l i d p r e c i p i t a t i o n i n thunderclouds. KUETTNER (1950) noted t h a t graupel was present i n 60% o f t h e thunderstorms on the Zugspitze , small h a i l i n 20%5 l i q u i d p r e c i p i t a t i o n i n 20% and h a i l i n o n l y 10% of the stormso was present i n 70% of the storms. Snow KUETTNER concluded t h a t h a i l was r e l a t i v e l y r a r e and was by no means necessary f o r the production of l i g h t n i n g . BYERS and BRAHAM (1953) found t h a t snow and snow p e l l e t s were the most common form' o f s o l i d p r e c i p i t a t i o n above the 0°G l e v e l i n summer thunderstorms over Ohio. However, graupel and small h a i l below 3 mm diameter were p r a c t i c a l l y u n i d e n t i f i a b l e but i n o n l y 10% o f the storms could the p r e c i p i t a t i o n be classed as h a l l . BRAHAM (1963) found t h a t t h e most common s o l i d p r e c i p i t a - t i o n i n c o n v e c t i v e clouds over M i s s o u r i was graupel which gave the appearance of having grown by t h e r i m i n g o f cloud d r o p l e t s . The average s p e c i f i c of the graupel was 0.88 and a l l the 110 graupel p e l l e t s c o l l e c t e d g r a v i t i e s g r e a t e r than 0.7. gravity BRAHAM gravity had s p e c i f i c also found c l e a r i c e p e l l e t s o f s p e c i f i c 0.9 u s u a l l y near t h e t o p s of updraughts. WEICKMANN and AUFM KAMPE (1953) found t h a t the l i q u i d water content of -3 cumulonimbi v a r i e s from 1 t o 6 g m . The a c t u a l value w i l l depend on t h e p a r t of the cloud s t u d i e d and the temperature of cloud base and the amount of a i r e n t r a i n e d by the updraught. From t h e o b s e r v a t i o n s o f KUETTNER, WEICKMANN and AUFM KAMPE and BYERS and BRAHAM i t seems t h a t t h e most common form o f s o l i d p r e c i p i fca'-ion i n thunderclouds i s smaller than 5 mm diameter and can be c l a s s i f i e d as graupel o r snow. ice w i l l depend on the The d e n s i t y and s t r u c t u r e o f the c o n d i t i o n s under which i t i s formed and may be d i f f e r e n t i n thunderstorm w i t h d i f f e r e n t cloud base h e i g h t s , updraught speeds and l i q u i d water contents* 10 2°3 0 The e f f e c t of growth c o n d i t i o n s on the s t r u c t u r e o f so+id p r e c i p i t a t i o n I f t h e r a t e a t which supercooled water drops a r r i v e a t an i c e surface i s g r e a t e r than t h e r a t e a t which t h e water i s f r o z e n then water w i l l be present on the surface and t h e growth can be said t o be wet. The t r a n s i t i o n from wet t o d r y growth has been s t u d i e d by LUDLAM (1950) 88. by c a l c u l a t i n g the heat balance a t the i c e s u r f a c e . He deduced t h e temperature a t which the growth becomes wet f o r d i f f e r e n t sized p a r t i c l e s i n c l o u d s w i t h bases a t 10 and 20°C. 4 mm diameter i c e spheres w i l l grow in t h e d r y phase a t h e i g h t s above t h e -10°C l e v e l i n both clouds w h i l e p a r t i c l e s o f 10 mm diameter can grow by wet growth up t o t h e -25°C l e v e l . I t seems u n l i k e l y t h a t a p a r t i c l e o f 4 mm diameter w i l l have grown by wet growth i n a cumulonimbus provided t h a t the growth d i d n o t s t a r t on top o f a f r o z e n water d r o p l e t . One might expect a p a r t i c l e o f l e s s than 4 mm t o have a l i q u i d l a y e r i f i t was surrounded by enough cloud d r o p l e t s as i t f e l l towards the 0°C l e v e l . 10.2.4 A i r bubbles i n n a t u r a l s o l i d p r e c i p i t a t i o n . Air bubbles can e i t h e r be formed by the r e l e a s e of d i s s o l v e d a i r a t an advancing ice-water i n t e r f a c e o r can o r i g i n a t e i n the spaces between i n d i v i d u a l cloud d r o p l e t s which f r o z e on impact w i t h the growing p a r t i c l e . Wet growth The r a t e o f advance o f t h e i c e i s governed by the r a t e of l o s s o f heat t o the environment. For a 4 mm diameter p a r t i c l e f a l l i n g at t e r m i n a l speed a t -10°C t h e heat l o s s as computed from e q u a t i o n 8.1 i s approximately 170 mW, corresponding t o a r a t e o f advance o f t h e i c e sheet of 2.4 mm min ^. CARTE (1961) found t h a t t h i s r a t e o f f r e e z i n g bubbles o f about 80 ^m diameter. produced At -20°C t h e mean bubble diameter would be about 50 ^m. As t h e a i r would be f r e e t o escape from t h e surface the c o n c e n t r a t i o n o f a i r bubbles may be g r e a t l y reduced. Dry growth. The a i r bubbles released by the freezing o f i n d i v i d u a l supercooled cloud d r o p l e t s are l i k e l y t o be a few \xn as t y p i c a l cloud d r o p l e t s i n cumulonimbus clouds have diameters i n t h e range 20 t o 40 urn. (wEICKMANN, %1953)% A more i m p o r t a n t source of trapped a i r bubbles i s probably t h e gaps between a d j a c e n t f r o z e n d r o p l e t s * MACKLIN (1962) e x p l a i n s the f o r m a t i o n of rime of s p e c i f i c g r a v i t y l e s s than 0.5 as being due t o d i f f e r e n t degrees o f close packing o f f r o z e n water d r o p l e t s . BftOWNSCOMBE and HALLETT ( l 9 6 7 ) suggest t h a t t h e i n c r e a s i n g d e n s i t i e s o f rime o f s p e c i f i c g r a v i t y g r e a t e r than about 0.6 can be explained by the 89. i n c r e a s i n g deformation of t h e c l o u d d r o p l e t s on impact. L i g h t e r rime w i l l be formed when the d r o p l e t s freeze before they have had time t o spread out over t h e s u r f a c e . The a i r bubbles trapped i n rime of s p e c i f i c g r a v i t y l e s s than 0.6 will probably be i n the diameter range 2 t o 200|Am assuming a range of cloud d r o p l e t diameters of 5 t o 40 jim. At very low d e n s i t i e s the gaps between frozen d r o p l e t s w i l l t e n d t o be i n t e r c o n n e c t e d . Ice o f h i g h e r d e n s i t y probably contains smaller a i r bubbles trapped between the f r o z e n d r o p l e t s due t o the e f f e c t of d e f o r m a t i o n on the d r o p l e t s * As the f r e e z i n g r a t e w i l l be l e s s the bubbles trapped i n s i d e t h e d r o p l e t s may become l a r g e r and as the growth becomes more l i k e wet growth the bubble size w i l l increase as adjacent d r o p l e t s coalesce before f r e e z i n g . 1Q.3 MELTING ICE AND THE MAGNITUDE.OF THE POWER POSITIVE CHARGEa The charge separated by m e l t i n g ice has been shown to depend on the s i z e of the a i r b u b b l e s 9 the m e l t i n g r a t e and the p u r i t y of the i c e . A l l these p r o p e r t i e s would be expected storms* t o have a range of values f o r d i f f e r e n t thunder- A f i g u r e f o r t h e magnitude o f charge t h a t can be produced by m e l t i n g i c e under p e r f e c t c o n d i t i o n s can however be obtained*. 10.3*1 Electriffica-frion under i d e a l circumstances. We w i l l assume t h a t the ice present i n t h e thundercloud contains a l a r g e number of bubbles s m a l l e r than 50 jim diameter and has been formed a t high enough f r e e z i n g r a t e s t o e l i m i n a t e an a p p r e c i a b l e l o s s o f a i i d u r i n g f r e e z i n g . The range of c o n c e n t r a t i o n s of i m p u r i t i e s i n cloudwater has been estimated in chapter 5 as 2 t o 20 mg 1 ^ C e r t a i n l y the l e v e l cannot be l e s s than t h a t due t o an e q u i l i b r i u m c o n c e n t r a t i o n of atmospheric from water i n e q u i l i b r i u m w i t h atmospheric carbon dioxideo Ice made carbon d i o x i d e and c o n t a i n i n g an a d d i t i o n a l i o n i c i m p u r i t y c o n c e n t r a t i o n of no more than 0°2 mg 1 * was found to produce 0.8 pC mg ^ o f e l e c t r i f i c a t i o n a t the maximum m e l t i n g r a t e s l i k e l y to be found i n the atmosphere ( f i g 8.7 )• This corresponds t o a charge -3 d e n s i t y of 0o8 G km i f the m e l t i n g p r e c i p i t a t i o n i s present i n a -3 ~3 c o n c e n t r a t i o n o f 1 gm . I n p r e c i p i t a t i o n of 5 gm t h i s corresponds t o 90. 3 4 C km" o SIMPSON and ROBINSON ( l 9 4 l ) estimated t h a t the lower p o s i t i v e charge o f -4 C could be considered as being l o c a t e d i n a r e g i o n 500 m i n -.3 radius. This corresponds t o a charge d e n s i t y o f 8 C km o 4 DRAKE (1968) found t h a t the charge separated by m e l t i n g a 10 Molar 1 sodium c h l o r i d e s o l u t i o n (5.8 mg 1 ) a t high m e l t i n g r a t e s was 0.4 p C mg -3 which would produce a charge d e n s i t y o f 0.4 C km f o r a concentration o f -3 -3 -3 m e l t i n g p r e c i p i t a t i o n o f 1 gm and 2 C km for 5 g m p u r i t y o f the water i s probably r e a l i s t i c e s p e c i a l l y as the measurements 1 . This value of made by SIMPSON and ROBINSON were made a t Kew which was not an area o f low pollution. TABLE 10,1 p r e d i c t e d by l a b o r a t o r y experiments Concentration of i o n i c i m p u r i t i e s 10" 5 4 1 M ( 0,6 mg l " ) concentration of melting precipitation -3 1 gm c »3 5 gm 1 1 0 ~ M ( 6 mg l " ) Charge Density 0.8 C km 4.0 C km 1 gm 0-4 C km 5 gm 2.0 C km SIMPSON and ROBINSON ( l 9 4 l ) 10 3o2 o 8 C km The e f f e c t of the nature o f the p r e c i p i t a t i o n . As has been discussed i n s e c t i o n 8.1 the d e n s i t y o f a s o l i d precipit- a t i o n p a r t i c l e a f f e c t s the m e l t i n g r a t e o f the i c e as denser p a r t i c l e s f a l l f a s t e r and reach warmer l e v e l s before f i n a l l y m e l t i n g . . also m e l t slower f o r the same reason. and Smaller p a r t i c l e s There w i l l be a l i m i t i n g d e n s i t y s i z e below which the m e l t i n g r a t e i s i n s u f f i c i e n t t o s u s t a i n the enhanced meltwater. separation e l e c t r i f i c a t i o n associated w i t h vigorous convection i n the Such p a r t i c l e s w i l l produce an order o f magnitude less charge than p a r t i c l e s w i t h higher m e l t i n g r a t e s and w i l l n o t c o n t r i b u t e sign i f IcantLy t o the lower p o s i t i v e charge. DRAKE (1968) suggests a minimum diameter of 1 mm f o r f r o z e n water drops .as these w i l l m e l t a f t e r f a l l i n g 500 m from the 0°C l e v e l according -3 t o DRAKE and MASON (1966). -3 Fig.10 2 The effect on of melting Electrification water purity ice e l e c t r i f i c a t i o n R a n g e of impurity clouds concentration ( Na pC mg in CI) 20 2 } ® Range e I e c t r t f ica tion r 0 10 Molar DATA concentration of i m p u r i t y Drake(196%) Particles frozen Convection in in airstream meltwater of ions 91. MASON (1956) has c a l c u l a t e d t h a t 3 mm diameter p a r t i c l e s o f s p e c i f i c g r a v i t y 0.3 w i l l m e l t i n a s i m i l a r d i s t a n c e - Snowflakes have f a l l speeds less than 1 ms ^ and are u n l i k e l y t o m e l t a t a high enough r a t e t o charge s i g n i f i c a n t l y by t h i s process. H a i l and small h a i l which are o f t e n made o f c l e a r o r m i l k y i c e w i t h most o f t h e a i r trapped i n bubbles l a r g e r than 50 ^m diameter are on the basis o f t h e work d e s c r i b e d i n chapter 8, u n l i k e l y t o c o n t r i b u t e to t h e charging process* significantly Opaque i c e c o n t a i n i n g many bubbles smaller than 40p m diamter would however be expected t o produce e l e c t r i f i c a t i o n up t o 0.4 "I -J. pC mg i f made o f water w i t h an i m p u r i t y c o n c e n t r a t i o n o f about 5 mg 1 In chapter 5 an e s t i m a t e f o r t h e range o f i m p u r i t y c o n c e n t r a t i o n s i n thunderclouds was given as 2 t o 20 mg 1 ^. Under t h e i d e a l c o n d i t i o n s discussed i n s e c t i o n 10<3»1 t h i s corresponds t o a range i n e l e c t r i f i c a t i o n o f 0*2 t o 0*5 pC mg ^ ( f i g . 10*2) The o b s e r v a t i o n s d e s c r i b e d i n chapter 8- c o n f i r m the magnitude ~5 of c h a r g i n g observed by DRAKE f o r water of i m p u r i t y c o n c e n t r a t i o n 10 M. 10.3.3 The e f f e c t o f the e l e c t r i c f i e l d due t o t h e negative charge c e n t r e . MATTHEWS and MASON (1964) observed t h a t water drops s h a t t e r i n g i n an electric field can produce as much as a f a c t o r o f 100 more charge s e p a r a t i o n in an e l e c t r i c f i e l d than i n t h e absence of t h e f i e l d * 4 -1 about 3 x 10 V m field The f i e l d s used were which i s a p p r e c i a b l y l e s s than the expected breakdown i n thunderclouds. BLANCHARD (1963) s t u d i e d t h e e l e c t r i f i c a t i o n produced by b u r s t i n g bubbles i n an e l e c t r i c f i e l d * The charge on t h e j e t drops from a 200pm 3 -1 diameter bubble could be reversed by a f i e l d o f about 3 x 10 V m f o r H a 10 M sodium c h l o r i d e s o l u t i o n . However? from t h e t h e o r y o f IRIBARNE and MASON (1967) and the c o n c l u s i o n s reached i n chapter 8 i t seems u n l i k e l y t h a t 200 \im bubbles w i l l p l a y an i m p o r t a n t p a r t i n m e l t i n g e l e c t r i f i c a t i o n f o r water o f t h i s p u r i t y . the As BLANCHARD observed t h a t i n d u c t i o n charging f e l l o f f r a p i d l y w i t h decreasing j e t drop size and hence bubble diameter* t h i s mechanism w i l l n o t be so e f f e c t i v e i n a l t e r i n g the charge separated by bubbles o f about 20 jim diameter i n Charged causing region the field 0 Earth Fig.10-3 of the Schematic bubble view of the e f f e c t on a n i n d u c t i o n of charging orientation mechanism 92. An i n d u c t i o n mechanism would also be i n f l u e n c e d by t h e way i n which the b u r s t i n g bubbles were d i s t r i b u t e d over the s u r f a c e of t h e m e l t i n g p a r t i c l e ( F i g . 10.3). I f the bubbles b u r s t a t a l l p o i n t s on t h e surface w i t h equal frequency, then an i n d u c t i o n mechanism would be i n e f f e c t i v e as the sign of charge produced a t t h e bottom o f a m e l t i n g p a r t i c l e would be opposite t o t h a t obtained a t t h e t o p . DRAKE and MASON (1966) have observed t h a t a i r bubbles o f l e s s than 100 y. m diameter tended t o go t o the bottom of m e l t i n g ice spheres whereas l a r g e r bubbles g e n e r a l l y went t o the t o p . I f the f i e l d i n t h e r e g i o n of t h e m e l t i n g h a i l were due t o t h e negative charge centre above, then the i n d u c t i o n charging would then increase the m e l t i n g e l e c t r i f i c a t i o n by g i v i n g the e j e c t e d j e t drops from t h e small bubbles more negative charge. The magnitude of t h i s e f f e c t i s unknown f o r bubbles l e s s < than lOOp. m diamtero 93. C H A P T E R 11 THE ELECTRIFICATION OF EVAPORATING ICE SPHERES 1 1 o l PREVIOUS WORK LATHAM and MASON ( l 9 6 l ) have shown t h a t i c e possesses a t h e r m o e l e c t r i c p r o p e r t y which causes the warmer end o f a piece o f i c e t o be n e g a t i v e l y charged. When an i c e specimen evaporates> i t s surface temperature i s u s u a l l y lower than the i n t e r i o r and one would expect the surface t o acquire a p o s i t i v e charge. As t h i s surface i s l o s t by e v a p o r a t i o n the remaining ice should acquire a net negative charge. LATHAM and STOW (1965) evaporated an i c e s h e l l surrounding a copper sphere and found a good q u a l i t a t i v e agreement w i t h the p r e d i c t i o n s o f the Latham and Mason temperature g r a d i e n t theory. I n a l a t e r paper LATHAM and STOW (1966) showed t h a t the p r o b a b i l i t y o f a charged molecule l e a v i n g the -57 ice surface was 10 times l e s s than f o r an uncharged molecule. The charging a t t r i b u t e d t o evaporation could be explained i f the charged molecule l e f t t h e ' s u r f a c e i n the centre o f a c l u s t e r o f about 1000 n e u t r a l molecules. CROSS and SPEARE (1969) monitored the e l e c t r i c ch arging o f a p o l y c r y s t a l l i n e i c e specimen due t o evaporation i n vacuo and showed the e l e c t r i f i c a t i o n t o be n e g l i g i b l e compared t o t h a t found by LATHAM and —2 STOW (1965). The l a r g e s t c u r r e n t recorded was -0.0011 fA mm evaporation r a t e o f 45 j i g s ^ and a temperature 0.3°C mm w i t h an g r a d i e n t i n the surface of The mean value o f c u r r e n t f o r evaporation ratec between 35 and 70 pgs ^ and temperature g r a d i e n t s o f 0.3 t o 0.6°C mm ^ was - 0.004 fA -2 -1 mm o For an e v a p o r a t i o n r a t e of 54 JJ qs the r e s u l t s of the Latham and Stow experiment p r e d i c t a charging c u r r e n t o f - 38 fA f o r the sample used 3 2 by Cross and Speare (3.5 x 10 mm ) . The l a r g e s t c u r r e n t observed by Cross and Speare a t t h i s e v a p o r a t i o n r a t e was -7 fA and the mean value -2.7 f A . Cross and Speare also found t h a t p o l y c r y s t a l l i n e i c e evaporating i n vacuo i s c h a r a c t e r i z e d by the development o f a f i b r o u s o r whiskery surface. They suggest t h a t t h e presence o f an a i r s t r e a m w i l l f r a c t u r e these whiskers 0> CD 0> CD O CO o4 0> uJ O 1 94. and cause them t o be c a r r i e d away* They also suggest t h a t these fragments w i l l be charged by a temperature g r a d i e n t mechanism i n a s i m i l a r way t o t h a t proposed by LATHAM (1963) f o r the e l e c t r i f i c a t i o n of f r o s t d e p o s i t s . 11.2 THE ELECTRIFICATION OF E E PARTICLES EVAPORATING IN THE WIND TUNNEL Ice spheres o f about 4 mm diameter were f r o z e n onto 120 ^m p l a t i n u m w i r e s and allowed t o evaporate i n t h e wind t u n n e l . The i c e was made f r o m a r t i f i c i a l - i cloudwater o f sodium c h l o r i d e content 4,5 mg 1 ' •> The d r y b u l b temperature of t h e a i r was about 0°C and t h e r e l a t i v e h u m i d i t y ranged from 50 t o 70%* The wet b u l b depression was s u f f i c i e n t t o prevent the i c e m e l t i n g . The values o f e l e c t r i f i c a t i o n d e s c r i b e d i n f i g . 11*1 are averages over a 2 min 12 period of t h e c u r r e n t o u t p u t from t h e V.R.E. which was used w i t h a 10 fl . input r e s i s t o r . The maximum average c u r r e n t was + 3 fA and themean + 0.1 f A . The average r a t e o f e v a p o r a t i o n was computed by equation 8.5 t o be 27 \ig s 1 corresponding t o a r a t e o f heat l o s s o f 68 mW. As the surface area o f t h e 2 ice spheres was about 50 mm , t h e maximum c u r r e n t d e n s i t y corresponds t o ~2 -2 + 0.06 fA mm and t h e mean t o + 0*002 fA mm . These values are o f t h e same order as the background section of the tunnel- c u r r e n t s w i t h no i c e present i n t h e working No c o r r e l a t i o n i s apparent between r a t e o f evaporation and t h e V o R o E o reading. 11,3 INTERPRETATION OF THE WIND TUNNEL EXPERIMENT The wind t u n n e l experiment has enabled the e l e c t r i f i c a t i o n of simulated s o l i d p r e c i p i t a t i o n p a r t i c l e s t o be studied i n c o n d i t i o n s which are probably s i m i l a r t o t h e environment o f e v a p o r a t i n g graupel and small h a i l i n the a atmosphere. The amount o f charging i s c l e a r l y o f l i t t l e importance i n cloud e l e c t r i f i c a t i o n ? as even a t the maximum charging r a t e , the p a r t i c l e would take 50 min t o a t t a i n a charge e q u i v a l e n t t o t h a t due t o i t s m e l t i n g ™X ""X D (0»3 pC mg o r 1 esu g ) • The values o f the temperature g r a d i e n t s expected are l i k e l y t o be 1 c o n s i d e r a b l y l e s s than t h e 9°C mm" value estimated by LATHAM and STOW (1965) f o r t h e i c e s h e l l on t h e copper sphere used i n t h e i r experiments. 95. MASON (1956) has c a l c u l a t e d the theimal r e l a x a t i o n time o f a 4mm diameter ice sphere f a l l i n g a t t e r m i n a l speed t o be 7s. I t seems l i k e l y t h a t such a p r e c i p i t a t i o n p a r t i c l e would soon reach a c o n s t a n t temperature w h i l e evaporating i n an i s o t h e r m a l atmosphere. I f the e v a p o r a t i n g p a r t i c l e i s f a l l i n g i n a r e a l atmosphere where the temperature increases as t h e p a r t i c l e f a l l s , t h e o u t e r surface w i l l be warmer than t h e c e n t r e . i s f a l l i n g a t 7 ms I f the p a r t i c l e through an atmosphere w i t h t h e d r y a d i a b a t i c lapse r a t e of 10°C km ^ the increase i n temperature o f t h e environment d u r i n g a p e r i o d equal t o t h e r e l a x a t i o n time o f the p a r t i c l e w i l l be 0.5°C« Assuming t h i s i s the temperature d i f f e r e n c e between the centre and the surface o f a 4 mm diameter p a r t i c l e , t h e mean temperature g r a d i e n t w i l l be approximately 0.25°C mm * o r a f a c t o r of 30 l e s s than i n the Latham and Stow experiment. One would a l s o expect the s i g n o f t h e charge s e p a r a t i o n t o be opposite to t h a t found by Latham and Stow and the e v a p o r a t i n g p a r t i c l e t o become p o s i t i v e l y chargedo A temperature g r a d i e n t should a l s o develop i n t h e whiskers o f i c e formed d u r i n g t h e e v a p o r a t i o n , due t o a g r e a t e r e v a p o r a t i o n rate o c c u r r i n g a t t h e t i p s o f the whiskers than near t h e surface of the particle. This gradient would be o f the same s i g n as i n the Latham and Stow experiment. I t i s suggested t h a t the one reason f o r t h e low l e v e l of charging produced by t h e e v a p o r a t i o n of the small ice spheres was t h e low temperature g r a d i e n t s i n the i c e samples. This c o n d i t i o n i s l i k e l y t o be found i n t h e evaporation o f p a r t i c l e s s m a l l e r than 10 mm diameter i n the r e a l atmosphere. While i t i s not know whether whiskers d i d develop on the surface d u r i n g e v a p o r a t i o n , i f t h e y d i d f o r m , then presumably t h e temperature g r a d i e n t s i n them were i n s u f f i c i e n t t o produce a measureable e l e c t r i f i c a t i o n . 96. C H A P T E R 12 CONCLUSIONS AND SUGGESTIONS FOR FURTHER WORK 12.1 THE DESIGN OF A WIND TUNNEL TO STUDY THE ELECTRIFICATION OF PRECIPITATION The design o f t h e wind t u n n e l which supported small i c e spheres has enabled some o f the problems associated w i t h t h i s type of research t o be studied. The design o f a windtunnel which w i l l support both s o l i d and l i q u i d p a r t i c l e s i s c l e a r l y more d i f f i c u l t than a system which w i l l support only water drops $ as the way i n which these p a r t i c l e s r e a c t t o pressure g r a d i e n t s and shear f o r c e s i s d i f f e r e n t . As no small wind t u n n e l appears t o have been designed which w i l l support a p a r t i c l e throughout i t s m e l t i n g p e r i o d , the a d d i t i o n a l c o n s t r a i n t s t o design caused by the need t o measure small e l e c t r i c c u r r e n t s and t o keep the p a r t i c l e s very clean make the design o f such a t u n n e l even more d i f f i c u l t . Even w i t h a wind tunnel working s e c t i o n as small as 40 mm diameter the r a t e of f l o w of a i r was so g r e a t t h a t the a i r i n the cold room of volume 3 o 4m was heated t o about 2 C a f t e r a m e l t i n g r u n l a s t i n g 1G min. This l i m i t e d t h e r a t e o f p e r f o r m i n g experiments t o one (.-very 3 hours? as the cold room temperature had t o be r e s t o r e d t o below f r e e z i n g . Stringent precautions to avoid c o n t a m i n a t i o n a l s o slow down t h e e x p e r i m e n t a t i o n and some r e s u l t s were r e j e c t e d because o f p o s s i b l e c o n t a m i n a t i o n . I n the present work? on average o n l y 2 experiments per day gave useable r e s u l t s . These problems would a r i s e w i t h almost any system of s u p p o r t i n g i c e p a r t i c l e s i n a t u n n e l . Another problem a s s o c i a t e d w i t h . t h e h i g h f l o w r a t e o f a i r i s t h e d i f f i c u l t y i n r e g u l a t i n g the r e l a t i v e h u m i d i t y i f the a i r i s heated c o n s i d e r a b l y t o enable t h e i c e p a r t i c l e s t o m e l t . The h u m i d i f i c a t i o n o f a i r f l o w i n g a t -1 the r a t e o f 10 1 s was found t o r e q u i r e more s o p h i s t i c a t e d than a heated t r a y o f water. a commerical h u m i d i f y i n g u n i t . equipment Probably the b e s t method would be t o use Clearly, trying t oattain realistic c o n d i t i o n s by f l y i n g or s u p p o r t i n g p a r t i c l e s i n a r e l a t i v e l y laminar 97o f l o w environment does severely l i m i t t h e v e r s a t i l i t y o f the apparatus and the c o n c l u s i o n s t h a t can be drawn from such experiments- The d i f f i c u l t y of measuring t h e mass o f i r r e g u l a r i c e p a r t i c l e s 9 which a l s o had t o be kept very clean? i n t r o d u c e d an e r r o r o f about 30% i n t o the f i n a l value of t h e charge t o mass r a t i o . T h i s e r r o r n e c e s s i t a t e s a l a r g e number o f experiments t o deduce the e f f e c t of environmental c o n d i t i o n s on the m e l t i n g e l e c t r i f i c a t i o n . Furthermore t h e slow r a t e o f e x p e r i m e n t a t i o n w i t h a l a r g e wind t u n n e l can be a great hindrance t o g e t t i n g meaningful r e s u l t s i n the time a v a i l a b l e . I t may w e l l be t h a t these disadvantages of a l a r g e tunnel capable o f f r e e l y f l y i n g a m e l t i n g p a r t i c l e make such a system of l e s s use than t h e more simple and v e r s a t i l e system used by CRAKE ( l 9 6 8 ) o 1 2 . 2 THE ELECTRIFICATION OF MELTING ICE The e l e c t r i f i c a t i o n o f m e l t i n g i c e has been shown t o be h i g h l y on the r a t e a t which t h e i c e was formed i n i t i a l l y . dependent Water drops f r o z e n i n s t i l l a i r were found t o produce an o r d e r of magnitude l e s s c h a r g i n g on m e l t i n g than drops f r o z e n i n an a i r s t r e a m f l o w i n g a t 11 ms ^. The d i s t r i b u t i o n and sizes o f t h e bubbles were found t o be d i f f e r e n t f o r the drops f r o z e n i n moving and s t i l l a i r * I t appeared t h a t a t low f r e e z i n g r a t e s l e s s a i r was trapped because the a i r could escape w h i l s t the i c e s h e l l was s t i l l thin. Ice f r o z e n i n t h e a i r s t r e a m below about -8°C contained no a i r bubbles g r e a t e r than 50 \im diamter? whereas i f the i c e were formed I n s t i l l a i r the l a r g e s t bubbles were u s u a l l y from 100 t o 200jim i n diameter. The o b s e r v a t i o n s t h a t a l a r g e number of small bubbles of diameter l e s s than 50|Am w i l l produce c o n s i d e r a b l y more e l e c t r i f i c a t i o n than a s m a l l e r number of l a r g e r bubbles agrees w e l l w i t h the IRIBARNE and MASON (1967) theory o f the e l e c t r i f i c a t i o n o f b u r s t i n g a i r bubbles. Evidence was found t h a t carbon d i o x i d e was r a p i d l y absorbed by a m e l t i n g water drop f a l l i n g i n a i r and i t was suggested t h a t the d i f f e r e n t r e s u l t s o f the e f f e c t o f CO^ on m e l t i n g e l e c t r i f i c a t i o n noted by DRAKE (1968) and DINGER and GUNN (1946) can be e x p l a i n e d by t h e way i n which 98. C0 escaped from the i c e d u r i n g m e l t i n g . A r a p i d increase o f an order o f magnitude i n m e l t i n g e l e c t r i f i c a t i o n over a small range of m e l t i n g r a t e s was observed, and t h i s may be the same as t h a t observed by DRAKE t o be due to t h e onset o f vigorous c o n v e c t i o n i n the meltwater. I t was shown t h a t t h i s increased e l e c t r i f i c a t i o n could occur a t m e l t i n g r a t e s l i k e l y t o be found i n the atmosphere. No s i g n i f i c a n t d i f f e r e n c e was noted between the e l e c t r i f i c a t i o n o f ice melted on s t r a i g h t 100 Jim p l a t i n u m wires and 1.5 mm loops o f w i r e . As the loop support i s e a s i e r to use t h i s i s probably the best type of support. 2 F u r t h e r work on the e l e c t r i f i c a t i o n o f m e l t i n g ice should i n c l u d e an e v a l u a t i o n o f the e f f e c t s o f e l e c t r i c f i e l d s . The e f f e c t o f CO^ on the e l e c t r i f i c a t i o n should be reexamined i n order t o see whether i t s bejaviour i s c o n s i s t e n t w i t h a b u r s t i n g bubble mechanism. Work on the e l e c t r i f i c a t i o n produced by the b u r s t i n g o f bubbles o f less than ICO^im diamter would enable the IRIBARNE and MASON t h e o r y t o be checked f o r t h e range o f bubbles l i k e l y t o be found i n small s o l i d p r e c i p i t a t i o n p a r t i c l e s . sizes The present work, and t h a t o f DRAKE, s t r o n g l y suggest a bubble b u r s t i n g mechanism f o r the f o r m a t i o n of the p o s i t i v e charge on the meltwater. 12.3 THE ROLE OF MELTING ICE IN CLOUD EIECTRIFICATION Using the i n f o r m a t i o n gained i n the present i n v e s t i g a t i o n and the work o f DRAKE (1968), the e f f e c t o f some o f the important v a r i a b l e s i n f l u e n c i n g m e l t i n g e l e c t r i f i c a t i o n can be assessed. I t has been shown t h a t p r e c i p i t a t i o n p a r t i c l e s o f approximately s p e c i f i c g r a v i t y 0.9 and diameter 4 mm m e l t i n g i n a cloud w i l l probably d i s p l a y the enhanced e l e c t r i f i c a t i o n which Drake associated w i t h vigorous convection i n the meltwater. I t was found t h a t the volume of a i r and the s i z e o f the a i r bubbles trapped i n t h e i c e could i n f l u e n c e the e l e c t r i f i c a t i o n by an o r d e r o f magnitude. formed i n s t i l l Ice which was m i l k y i n appearance and which was a i r produced t e n times l e s s charging than completely opaque i c e formed i n an a i r s t r e a m . a i r bubble I t i s t h e r e f o r e suggested t h a t the s t r u c t u r e o f the i c e i s v e r y i m p o r t a n t i n i n f l u e n c i n g the 99. the amount of e l e c t r i f i c a t i o n produced by t h i s mechanism, and t h a t i c e formed by d r y growth may be more e f f e c t i v e than i c e formed by wet growth. The m e l t i n g r a t e and p a r t i c l e size can i n f l u e n c e the- development of -enhanced e l e c t r i f i c a t i o n which may be associated w i t h v i g o r o u s convection i n the meltwater. The m e l t i n g r a t e depends on the speed o f the downdraught and the d e n s i t y o f the p a r t i c l e s , as w e l l as the size of t h e p a r t i c l e s and the a c t u a l lapse r a t e o f the temperature i n t h e c l o u d . The e f f e c t o f i m p u r i t i e s i n the cloudwater may be l e s s than the e f f e c t of the a i r bubble s t r u c t u r e and m e l t i n g r a t e s , according t o the experiments described i n Chapter 8. I f t h e c o n t r i b u t i o n of the m e l t i n g i c e t o the e l e c t r i c a l s t r u c t u r e o f a thunderstorm i s t o be assessed, then more i n f o r m a t i o n i s needed of the a c t u a l m e l t i n g i c e p a r t i c l e s and the m e l t i n g environment. I t was p o i n t e d out i n Chapter 10 t h a t the amount of i n f o r m a t i o n o f the l o c a t i o n , magnitude and frequency of occurrence of the lower p o s i t i v e charge i s very s m a l l . I t i s n o t even p o s s i b l e t o say t h a t t h e r e i s only one type of lower p o s i t i v e charge. Certainly there i s i n s u f f i c i e n t i n f o r m a t i o n t o r u l e out a m e l t i n g i c e o r i g i n , but on the evidence a v a i l a b l e i t was suggested t h a t such a mechanism could o n l y e x p l a i n the charge under t h e best circumstances p o s s i b l e , unless the mechanism was more e f f e c t i v e i n the presence of e l e c t r i c fields. The process of m e l t i n g e l e c t r i f i c a t i o n and t h e c o n d i t i o n s t h a t might cause i t t o be an e f f e c t i v e means o f charge p r o d u c t i o n i n clouds are r e l a t i v e l y well'understood. However i t i s not p o s s i b l e t o decide on the mechanism f o r t h e f o r m a t i o n of the lower p o s i t i v e charge u n t i l more i n f o r m a t i o n i s a v a i l a b l e on t h e magnitude and p o s i t i o n of the c h a r g e 9 on the nature of the p r e c i p i t a t i o n and the evironmental c o n d i t i o n s associated w i t h t h e charge. This l a b o r a t o r y i n v e s t i g a t i o n has suggested several p r o p e r t i e s of clouds which may w e l l i n f l u e n c e the cloud e l e c t r i fication. These p r o p e r t i e s must now be studied i n d e t a i l i f the physics of the lower p o s i t i v e charge i s t o be understood. 100, APPENDIX 1 WIR,^ A l . l THE ELECTRIFICATION OF ICE SPHERES MET.TTNG ON, PI,A,nM Ice f r o z e n i n stagnant a i r ARTIFICIAL CLOUD WATER - 4.5 mg l " 1 sodium c h l o r i d e . C o n d u c t i v i t y 8.4 jimho cm * No Dry Bulb Temperature °c 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 12.5 10.0 10.1 10.6 11.6 11.3 11.4 9.8 10.4 10,1 8.7 11.5 9.2 10.6 10.9 9.8 11.0 11.2 12.0 9.8 9.8 8.9 8.8 11.6 9.6 10.0 11.2 9.5 6.6 8.8 10.4 9.3 9.8 11.2 8.4 10.0 10.1 10.5 10.0 10.9 10.4 10,4 9.0 9.6 10.6 Dew Point Melting Heat Initial Mass Mass Melted - °c mW mg mg 64 32 32 32 48 32 32 32 36 32 32 32 40 48 40 41 48 36 60 48 48 36 40 48 40 36 48 48 40 32 40 32 32 40 24 64 48 40 36. 48* 48 36 40 40 36 56 25 24 22 35 21 19 21 26 27 22 25 34 35 36 43 43 17 20 23 45 32 38 39 34 33 43 37 36 29 34 29 29 35 20 56 45 38 34 44 41 28 18 35 31 5.7 5.8 6.5 7.8 7.9 8.4 9.1 7.3 7.0 4.b 6.2 6.3 4.5 7.4 3.9 3.7 4.1 9.5 9.2 8.5 3.8 3.8 2.8 6.4 4.6 3.5 4.5 6.4 2.6 3.5 4.5 3.5 3.7 4.7 4.5 4.4 2.5 2.0 2.2 3.1 4.6 5.9 7-9 3.5 4.5 96 49 43 34 47 38 27 31 44 63 32 60 68 42 86 75 85 21 26 20 85 58 73 66 83 73 83 44 50 60 74 72 69 81 44 80 92 101 84 99 73 53 18 75 69 101 No 47 48 49 50 51 52 53 54 55 56 57 58 59 60 Dry bulb Temperature Dew point °C -°C Melting Heat mW 10.1 10.4 10*4 10.5 11.6 11.6 .14.0 11.1 12.6 10.6 13.1 11.2 14.9 11.9 3.8 3.9 2.5 2.9 1-8 1.6 2.7 1.6 2.0 2.7 1.9 2.7 1.7 2.1 81 80 95 96 105 118 142 112 125 99 136 93 141 106 No Freezing Temp Cha rge - °C 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 12 12. 11.5 13 12.5 13 12.5 12 11.5 11.5 12 11.5 11.5 13 12 11.8 11.5 14.5 14 10.5 10 10 10.5 13 12 10.5 11.5 14 13 11 11 12.5 11.5 11 11.5 11 + pC 4.5 0.2 0 0.2 2*0 1.3 0.7 0.2. 0.1 0,1 Ool 0.2 0.4 0.8 0.6 2.2 0.7 1.0 0 0.1 0.8 0.1 0.9 2.4 1.3 4.2 2.0 3.1 2.3 0.3 0.5 1.3 0.5 1.3 0.»9 0,1 Initial Mass Mass Melted mg mg 48 40 40 48 48 40 48 48 40 48 40 36 36 32 43 36 38 45 46 39 46 46 38 44 38 33 35 31 Charge/mass pC mg * 0.08 0.008 0 0.009 0o058 0*060 0.038 0.009 0.004 0o004 0.005 0..008 0.012 0o023 0.016 0.051 0.016 0.057 0 0.004 0.018 0.003 0.024 0.062 0.038 0.129 0.047 0.106 0.063 0.008 0.017 0.038 0.017 0.045 0.026 0.005 ! A 3 APR 1972 MOTION [BRA! 102. No Charge Freezing Temp 37 38 39 40 41 42 43 44 4b 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 - ° c" +C 13 10.5 11 12 10 11 12 14 14.5 10o5 12 11.5 14o5 12 11 11.5 14o5 13 15 14.5 11 11 10.5 10 3.1 1.3 Charge/ma: pC mg P 0.055 0.029 0.031 1.2 0.4 1.6 0.7 1.2. 1.6 1.0 1.0 2.2 1.7 4.1 1.0 1.5 0.7 3.4 2.6 4.4 lo4 1.3 0.012 0,036 0.017 0.043 0.088 0.02.8 0.032 0.051 0.048 0.109 0.022 0.032 0.018 0.074 0.056 0.114 0.031 0,034 0.027 0.031 0.033 0.9 1.1 1.0 A 1 . 2 THE ELECTRIFICATION OF ICE SPHERES MELTING ON PLATINUM WIRES Ice frozen i n stagnant a i r . E E IONIZED WATER No Dry Bulb Temperature C 5 61 62 63 65 66 67 68 69 70 71 72 73 74 75 13.0 13.7 14.0 14.1 1^3 13.2 13.5 12.0 13.6 13.7 15.0 13.8 13.2 14.7 14.0 Conductivity Dew Point 1 . 0 pmho -1 cm -°C Melting Heat mW Initial Mass mg Mass Melted mg 1.2 3.3 2.0 2.5 2.4 0„8 2.5 1.4 2.5 2.5 2.6 2.5 2.2 3.2 2.8 138 119 154 138 141 157 131 125 126 121 154 140 130 137 133 40 36 48 40 40 48 40 46 32 32 48 48 46 40 46 39 34 46, 38 38 47 38 45 30 31 46 46 44 38 44 103. No 61 62. 63 64 65 66 67 68 69 70 71 72 73 74 75 Freezing Temperature Cha rge Charge/mass -°C +pC pC mg ^ 12 9 9.5 11.5 14 10.5 12 13 7.5 50 6.5 6.8 14.5 12.5 13.0 5.7 3.9 3.2 4.6 11.1 3.8 7.6 8.2 2.9 1.1 1.2 2.2 4.0 3.8 4.5 0,15 0.12 C.069 0.12 0.29 0.08 0„20 0.18 0..10 0.036 0.026 0,»05 0.09 0.10 0.10 A l . 3 THE ELECTRIFICATION OF ICE SPHERES MELTING ON PLATINUM LOOPS NO 76 77 78 79 80 81 82 83 84 Dry Bulb Temperature C Dew Point 12.5 14.0 12.3 14.2 13.7 13,2 13.5 13.7 12.0 No 76 77 78 79 80 81 82 83 84 - C Melting Heat mW Initial mass mg Mass Melted mg 1.0 2o4 2.5 4.7 1.1 1.7 1.5 1.3 2.0 115 100 90 94 127 118 109 99 81 24 18 18 21 27 24 18 14 14 24 17 17 19 27 23 18 14 14 Freezing Temperature Charge Charge/mass -°C +pC pC mg ^ 11 9 8.5 10 11.5 11.5 7 4 8 5.0 0„8 1.2 2.0 5.0 4.4 2.0 0„1 3.9 0.21 0.046 0.07 0.11 0.19 0>19 0.11 0.007 0.29 104. A1.4 THE ELECTRIFICATION OF ICE SPHERES MELTING ON PLATINUM I POPS DEIONIZED WATER Conductivity 1 . 0 mho cm" 1 Drops frozen i n an a i r stream moving at 11 ms No 85 86 87 88 89 90 91 92 93 94 95 Dry Bulb Temperature ~C 12.0 11.0 14.5 11.8 14.0 12.0 12.8 13.1 12.7 13.1 11.2 NO 85 86 87 88 89 90 91 92 93 94 95 Dew Point - C Melting Heat mW Initial Mass mg Mass Melted mg 2.0 1.5 4.5 6.2 1.3 2.5 2.0 2.0 1.2 2.0 1.3 86 81 82 48 108 82 87 89 98 95 85 18 18 14 16 18 18 14 14 18 18 18 17 17 13 13 18 17 13 13 18 17 18 Freezing Temperature -°C Cha rge +pC 12o0 12.5 5.2 12.3 8.5 3.5 11.5 6.6 2.4 5.3 12.5 11.2 13.5 6.9 12.2 12.0 2.9 15.3 12.5 0.4 4.6 11.1 Charge/mass pC mg 0.65 0.77 0,54 0.94 0.68 0.17 0.14 0o93 0.023 0,27 0.63 Melting heat is defined as the heat f l o w rate to the melting sphere which causes the ice to melt and i s corrected f o r the loss of heat due to evaporation using equation 8 . 1 „ The value of mass melted melting heat and charge/mass were worked out on the computer using the program outlined i n A l . 5 . 9 NoU.M.AoC. IoB.M. 360 105. A l . 5 FORTRAN PROGRAM USED TO PROCESS THE WELTING ELECTRIFICATION DATA DIMENSION TW (lOO) , HTM (lOO), TIME (lOO), TIMM (lOO), AMASS (lOO), Q (lOO), TDEW (100), RAD (lOO) , HMELT (lOO), TF (lOO) lo FORMAT (12 F 5.1) 2. FORMAT (8 x, 'TEMPW , 2x, HT. MELT', 2x, 'TIMM', 2x, 'HT,EVAP' , 2x, 1 , 1 'TIME • , 4x, 'INMASS , 2x, 'CHARGE', 2x, 'FRACTM' , 2.x, 'MASS MLT*, 1 1 2x, 'RATE', 4x, 'QPM , 5x, 'RAD', 6x, 'TDEW , 3 , 'TEMPF') X 3. FORMAT (2x, 13, 14 F 8.3) READ (5,1) (TW(I), HTM(I), TIME ( I ) , TIMM ( i ) , AMASS ( i ) , Q ( l ) , I =1,36) READ (5,1) (TDEW ( i ) , RAD ( i ) , TF ( I ) , I = 1,36) WRITE (6,2) DO 10 I = 1,36 HT MELT ( I ) = 3 . 9 * RAD ( I ) * (TW ( I ) j p l . 3 4 - 1.09 0.022 TDEW ( I ) - TDEW ( l ) J t * . 2 . HTE = 3.9 + RAD ( I ) ^ (.U0( ^ TDEW ( i ) + 0.022 TDEW ( 1 ) ^ 2 . ) A = H MELT (I)-Jf 8. ^ T I M M ( I ) B = HTE j|LTIMM ( I ) C = 3 . 9 ^ RAD ( I ) % ( . 5 5 ^ 7 DEW ( I ) + .005 Jjf TDEW ( l ) # ^ 2 . ) D - C *(TIME ( I ) - TIMM ( I ) ) FRACTM = A / (A+B+D) AMELT = FRACTM AMASS ( I ) RATE - AMELT/TIMM ( i ) QPM - Q ( I ) / AMELT 10. WRITE (6,3) I , TW(I), H MELT ( i ) , TIMM ( i ) , HTE, TIME ( I ) , AMASS ( i ) , Q ( I ) , FRACTM, AMELT, RATE, QPM, RAD ( i ) , TDEW ( I ) , TF ( i ) STOP END In the above program the names of the variables are as follows I index number of the ice p a r t i c l e TW average dry bulb temperature during l a s t minute of melting °C 106 HTM melting heat mW TIME Time p a r t i c l e was evaporating min. TIMM Time p a r t i c l e was melting min. (This is defined by the time between the moment when the a i r temperature has been raised halfway between 0°C and i t s f i n a l value at the end of melting and the end of the melting process). AMASS The i n i t i a l mass of the p a r t i c l e as deduced from i t s dimensions mg<» Q The charge on the meltwater at the end of melting pG (This was calculated by integrating the current over the melting period using the U»Vo chart record). TDEW Modulus of the dew point temperature of the a i r i n the tunnel during the l a s t minute of melting.. °C RAD Mean radius of the p a r t i c l e mm TF Modulus of the temperature of the freezing environment FRACTM Fraction of the ice actually meltedo AMELT Mass of ice actually melted mg QPM Charge/mass melted pC mg 107 APPENDIX 2 THE ABSORPTION AND DESQRPTION OF A2.1 CARBON DIOXIDE BY WATER Absorption by a stationary drop. The chief cause of resistance to the d i f f u s i o n of CO^ i n t o a water drop i n stagnant a i r i s the t h i n surface f i l m of l i q u i d . This f i l m has a permeability which r a p i d l y decreases a f t e r the i n i t i a l exposure to CO^ due to the increasing saturation of the layer. permeability remains constant. When the f i l m is saturated the The rate of absorption can be related to the concentration gradient i n the surface f i l m by |~ = k A (Cg - C ) .......... x A2.1 where W i s the volume of gas absorbed, A the surface area, k the permeability c o e f f i c i e n t and C the concentration of CO^. The subscript 1 r e f e r s to the l i q u i d remote from the f i l m and g to the g a s / l i q i d boundary. u RIDEAL and DAVIES (l963) show, by solving the d i f f u s i o n equation f o r a stagnant l i q u i d of i n f i n i t e e x t e n t , that the permeability c o e f f i c i e n t is related to the d i f f u s i o n c o e f f i c i e n t D by k = / D .......... A2.2 7 TTt provided that the f i l m i s not saturated. A f t e r the f i l m becomes saturated at a time t k - / #JD ^s By i n t e g r a t i n g A2.1 with respect to time and s u b s t i t u t i n g f o r k we have , f o r a water drop of radius r , W= t \ 2 fair? (Cg-C^ PD" j dt . . . . . . . . . A2.3 A f t e r a time t , the f r a c t i o n f of the amount of C0 absorbed at 2 e q u i l i b r i u m may be w r i t t e n as W f = . —— {4VTCg/3) a ~ | [ C g - C,) ftz>\ dt . . . A 2 . 4 108 I f we assume t h a t once the CO^ has passed through the surface f i l m i t i s r a p i d l y d i s t r i b u t e d throughout the drop then C = f Cg t = f/sj J a r 1 izf. d t A 2 . 5 This equation has a s o l u t i o n : < 1 2 n f - V " - - ' ° - (;> (I)" which converges r a p i d l y i f t « value of t = ^ r 72 t n / 2 2 6 - «- 2 2 . but tends to i n f i n i t y if t > 5- . The corresponds to the time when the permeability has reached a minimum value due to the saturation of the layer and may be designated as t . s WHITIMAN et al (1926) quote the permeability c o e f f i c i e n t f o r t > t as 2.8 x 10 1 ms , which approximately corresponds to a saturation time t of s 100s. For t ^ 100 s t = 100s, and k f f can be expressed i n terms of f-^QQj the value of f at 1 Q 0 , the permeability c o e f f i c i e n t f o r t = f l Q 0 + 3 k l00 r / 100 ( l - f ) dT A2.7 J o where T = t -100. 3 D i f f e r e n t i a t i n g A2.7 and w r i t i n g a = - k^00 df a a (i-f) A dT 2 , b This has the s o l u t i o n f = 1 - (l-f 1 0 0 ) exp (-a(t-lOO)) For a 4 mm diameter water drop A2.6 gives f^oO A2.9 = s ^^^ations A2.6 and A2.9 are p l o t t e d i n f i g . 9.3. A2.2 The desorption of a t h i n water layer i n a container. The desorption of a t h i n water layer on the surface of a block of ice i n a container can be treated i n a s i m i l a r way to the absorption of gas by a water drop, provided that the process is by molecular d i f f u s i o n 109 through an undisturbed surface f i l m . I f the surface f i l m has been present f o r longer than 100 then i t can be said to be saturated and the permeability can be taken as constant. S For a layer of area A and depth d , f may be w r i t t e n i n a similar way to equation A2.5: / f k A ( l - f ) dt / k Ad J ( l - f ) dt A2.10 J d The s o l u t i o n of A2.10 w i l l be f = 1 - exp - ( k t / d ) A2.ll The time constant of the desorption of a layer d due to i t s formation from Co^ saturated ice w i l l be d / k . WHITMAN A2.3 F r a 1 mm layer with kjs 0 2.8 x 10 ^ ms 1 et a l . (1926) , the time constant w i l l be approximately 400 . s The release of carbon epoxide from a bubble immersed i n an unsaturated liquid. I f one assumes t h a t the gas w i l l d i f f u s e through the bulk l i q u i d f a s t e r than through the surface f i l m , and i f the concentration of GO^ i n the water is n e g l i g i b l e compared to that i n the bubble, the volume of CO^ removed from the bubble i s Q = I k A Cg dt A2.12 where A i s the surface area of the bubble and Cg the concentration of CO inside the bubble. The f r a c t i o n f of the i n t i a l concentration Co of Co, >2 in the bubble i s given i n a s i m i l a r way to A2.5 as f = 3 /I Co.47Tr rI rD 3 J i r 2 4 t7t r r Co f dt A2.13 t D i f f e r e n t i a t i n g both sides of A2-13 by t we have 4E dt = 2 3 - r r ^ v | D - .f TTi f t which may be expressed as d£ = 3 3 /; D 5 f r \ J Trt I n t e g r a t i n g equation A2.14 we have dt A2.14 REFERENCE ALTY 9 The o r i g i n of the e l e c t r i c charge on small p a r t i c l e s i n water Proc. Roy. Soc. A , H2> 235-51 T. ARENBERG, D . 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