Extra evidence for liquid amorphous water in cold atmospheric clouds:
Author’s response to basic counterarguments
Anatoly N. Nevzorov
Central Aerological Observatory. Dolgoprudny 141700, Russia
Email: an-nevzorov@yandex.ru
Abstract. The current knowledge of the microphysics of cold clouds involves such peculiarities as
not explainable from today’s notions but being readily explained if basing on the conception of liquid amorphous water (A-water) with its specific properties. All worldwide measurements in icecontaining stratiform clouds using the high-sensitive TWC/LWC probe reveal permanent presence
therein of liquid fraction. That this implies its condensational equilibrium with the ice fraction, is argued against by some authors referred this phenomenon to only residual effect of ice on LWC sensor. Such explanation proves to be biased and inadequate as based on speculative estimation of this
unreal effect wittingly meant only to achieve the preset result of “zero LWC”. A comparison of basic
properties of two models of glory formation, by droplets of ordinary water and A-water, with natural
glory evinces that the true glories on cold clouds are produced by A-water droplets with n ~1.81 rather than the ordinary water.
1. Introduction
The goal of this work is to derive the confirmation of the existence of liquid amorphous water
in cold clouds from arguments of disagreement with it.
In the current knowledge of the physics of cold (with temperatures below 0оС) clouds, the
problems connected with the presence of the liquid water fraction in ice-containing clouds (ICC) remain both the least investigated and the most disputable. This concerns its nature, repeatability, and
physical role in cloud processes. The conventional notions based on Wegener – Bergeron –
Findeisen (WBF) principles consider supercooled liquid water in ICC to be only intermediate, temporary substance. Meanwhile, more and more world-wide experimental data on the liquid fraction
behavior in the ICCs furnishes increasingly more solid arguments against this conventional approach.
The problem proper of the occurrence, dynamics and properties of a liquid disperse phase in
cold, especially ice-containing clouds is one of the most important of all topical problems in cloud
microphysics. The lack of key experimental data required for its solving gives rise to speculative
conceptions and theories. In spite of the fact that such abstract reasoning builds upon the commonly
assimilated utilitarian knowledge of water properties and classical ideas of WBF in the physics of
phase-mixed clouds, it fails to explain even most frequently observed anomalies of liquid phase behavior in cold stratiform clouds.
Logically, the futility of the attempts to explain the nature of such anomalies on an aprioristic
classical basis must lead one to dismiss habitual dogmas and seek for new solutions. Our recent re-
search has revealed specific properties of liquid disperse phase in ICC that distinguish it from the
ordinary supercooled water. Namely, they as a rule are clearly indicative of an abnormally steady
coexistence of liquid and ice disperse phases. Moreover, in mixed-phase clouds most of liquid water
tends to be contained in much larger droplets (conventionally > 30 µm) than in purely water clouds
(agains < 30 µm). This is demonstrated by Fig.1.
Fig.1. Typical examples of cloud particle samples obtained in stratiform clouds at the temperatures -8...-27оС visually classified as purely ice ones, CAO, A.M. Borovikov, 1951.
Purposing the study of crystal shapes, the micro photos were made of selected fragments with
minimal contents of droplets.
Initially similar data were referred to occasional (“case study”) observations, whose results were
only considered as an exception from the general rule, applicable to very rare situations. The results
would then be explained by possible spatial isolation of each of the two phases, or by vapor super
saturation over water, e.g. in ascending or turbulent air, and even by the specific chemistry of cloud
water. The abnormally big sizes of ICC droplets, up to hundreds micrometers, were conventionally
explained in terms of their coalescence growth. Theoretical researches in this area, e.g. by Korolev et
al. (2006b, 2007), are as well concerned with specific dynamical processes, strictly time-limited by
their relaxation, and is far from being able to explain the permanent character of a mixed-phase
structure of usually quiet and long-live stratiform clouds.
2. Current state of the problem
In our aircraft measurements (Nevzorov, 1992, 2000), the large-droplet liquid fraction was
found in practically all stratiform ICCs at temperatures from 0°С down to at least –55°С (in Cirrus).
A thorough analysis of complex microphysical measurements and literary data available concerning
insufficiently investigated problems of the physics of water and clouds at T<0oC, has led us to the
following conclusion. The ICC liquid water considerably differs in its properties from the universally
known ordinary water (hereinafter water-1), and is in a specific, amorphous phase, named А-water.
Details of the analysis, as well as a discussion of the properties of А-water, its nature and its role in
the physics of cold clouds are presented in (Nevzorov, 1993, 2006b, 2009). Most importantly, free
А-water is concluded to be in stable condensation equilibrium with ice disperse phase Fig 1, being
directly condensed from on special nuclei vapor and capable of remaining in metastable liquid state
even at temperatures below -40°C. Its refractivity, as primarily specified by the value of n = 1.8÷1.9
(Nevzorov, 1992, 1993) and later n = 1.8÷1.82 for yellow light (Nevzorov, 2006a), corresponds to
Н2О substance density of about 2.1 g.cm–3 according to the Lorenz – Lorents formula (Eisenberg,
Kauzmann, 1969). Its specific evaporation heat is estimated to be approximately 5 times less than
that of water-1.
So far the conception of cloud А-water is far from being generally understood and acknowledged. Instead, there were some few publications as below whose authors, openly or by default, contest the presence of this alternative form of liquid water in cold atmospheric clouds and its role in an
explanation of a variety of abnormal, from current viewpoint, features of their microphysical evolution and structure. Alas, such simplifying position following a ridiculed principle "it cannot be because it can be never" has received wide resonance among cloud physicists. Objections of the opponents refer to such properties of the liquid fraction in ICC as condensation equilibrium with ice (Fig.
1) and high refractivity. However, the counterarguments put forward by those opponents contain obviously unreal and inaccurate prerequisites which make them null and void. Their alternative ideas
and counterarguments put forward are critically considered below.
3. LWC measurements: liquid water or ice effect?
Numerous measurements in cold stratiform clouds using the IVO (Cloud Water
Content Meter) device, best known as Nevzorov TWC/LWC probe (Korolev et al., 1998), invariably
indicate the presence of a liquid fraction in practically any ICC. Paradoxically, this result obtained
over the world contradicts WBF principles those exclude any possibility of ubiquity and permanence
of liquid water droplets in clouds at Т <0оС, because of regular processes of their freezing and recondensation on ice particles with the formation of purely ice clouds. This paradox still needs realistic explanation.
Earlier we postulated (e.g. Nevzorov, 2000) that the condensation equilibrium in phase mixed
clouds is a cause and effect of that that so named “quasi-liquid” surface layer of ice particles (Jellinek, 1967) consists of the same A-water as the liquid droplets.
On the other hand, in the paper of Korolev et al. (2003a) and in consequent papers of same and
other authors sharing the traditional notion of uniqueness of well-known physicochemical form of
liquid water, that “anomaly” is considered as a residual effect of ice particles on the LWC’s hot collector. No objective substantiation of this idea but initial notion of zero LWC is adduced. The evaluations of “ice share” in LWC readings WL were made from measurements in clouds taken a priory as
purely ice ones. Within this assumption, the seeming “ice share” has been evaluated as the relation R
= WL / WT, where WT is the TWC output. In instant readings the R value showed a spread from 0 up
to 1 often within the same cloud, while the cloud-averaged values varied between 0.1 and 0.5.
Such a widely variable relation between WL and WT implies the absence of their significant
spatial correlation as naturally expected for the version of ice effect. The declared result itself cannot
be physically feasible, because in contrast to the surface-film mechanism of fast evaporation of liquid droplets colliding with any collector, the ice particles or their fragments do tower above the surface like a sail. As a result, the air flow instantly blows them out from the streamline LWC sensor
with negligible losses of their mass and therefore of sensor heat. This effect can be promoted by a
slippery action of liquid and/or repulsion action of vapor both appearing as very thin layer between
the contact spot of ice particle and the collector surface. As a confirmation of this action, it has been
revealed (Emery et al., 2004; Korolev et al., 2007) that ice crystals, impacting with the plane speed
on a hot (70o – 100oC) solid surface, instantly rebound from it like elastic balls and are carried away
by the air flow. Why must the streamlined IVO LWC sensor be exclusion?
As early as in 1980s, we followed another approach to estimate possible residual effect of ice
on the LWC collector. On hundreds meters of visual records made in dozens of various cloud samples at a rate of 2.5 mm/sec., the situations with WL = 0 at WT > 0 were selected. For each ones the
relation R0 = ΔWL / WT was determined, where ΔWL is the possible absolute error in case of latent
(subzero) drift of LWC output, and R0 = 0 when the instrumental drift doesn’t hide zero output. The
intuitive conclusion follows that the real ice effect is at least half less than the measurement error
caused by the output drift. This method seems both simplest and most adequate.
Fortunately, in typical ICCs the main contribution to the liquid А-water content (AWC) is generally made by droplets of a large enough size and density (Nevzorov, 2009) to result in collection
efficiencies close to unity for both sensor-collectors. This circumstance extremely simplifies the calculation of the cloud disperse phases content from the IVO outputs:
LWС  WL ,
IWC 
EW
(WT  WL ) ,
EI
LAWC 
EW
WL .
E AW
(1)
(2)
(3)
Here EW, EAW, EI are the magnitudes of the specific energy of evaporation of water-1, A-water and
ice, respectively. Basing on own experience, we confidently assert that these working formulas are
not only simplest and quite obvious, but, in essence, as accurate as possible.
The experimental corroboration of the viewpoint shared by the authors of Korolev et al. (2003)
paper by means of comparing synchronous outputs of the IVO and the Rosemount icing detector,
RICE, in essence cannot be correct because of significant difference in their threshold sensitivity to
liquid phase. As theoretically evaluated by Mazin et al. (2001), the RICE sensitivity threshold must
be of order of 10 mg-3. However this theory concerns only water-1 and does not consider alternative
properties of A-water and specific features of freezing process of metastable water (Nevzorov,
2006b), as well as crumbling loss of ice in the course of its deposition. The latter phenomenon is typically peculiar to mixed clouds (the author personally observed it during numerous cloud penetrations) and most probably somewhat intensifies in case of the vibrating pin sensor of RICE. As a result, the RICE actually is much less sensitive than declared, as can be seen from the sample of incloud synchronous records copied from (Korolev et al., 2003) paper and shown in Fig.2.
In Fig.2 the characteristic intervals of the records of both devices are positioned between the
vertical lines. The intervals Nos 1, 3 and 5 correspond to the events where RICE indications (corresponding to increasing icing of its sound pin) denote the presence of liquid water. It can be seen that
they occur only when WL surpass 0.07 ÷ 0.08 g.m-3 (horizontal line). This value does be a rough estimate of true sensitivity threshold of RICE on the water-1 scale. This implies that the RICE provides
no information of the liquid phase when according to Eq. (3) LAWC values are less than ~0.4 g·m-3,
i.e. in most of cold stratiform clouds by Nevzorov (2009).
Fig.2. An example of simultaneous records of RICE (a) and IVO (b) probes. The
lowest (thicker) curve is for water-1. Copied from Korolev et al. (2003) paper and
lined with colors as described in the text.
Note that relatively fast decreasing of RICE record immediately after WL falling below its sensitivity threshold (Fig.1, interval #2) results from ice crumbling rather than from its evaporation. It is
also characteristic that the highest peaks within interval #2 in the IVO TWC record do not accordingly affect the LWC record, which directly contradicts the declared “ice effect” on the LWC sensor.
It is worth to emphasize that the concept of A-water does not deny the existence and role of
WBF process in phase evolution of cold clouds. Virtually, this implies that the vapor produced by
evaporating water-1 droplets deposits both onto the intermediate surface layer of A-water covering
icy particles (Jellinek, 1967) and simultaneously onto the free A-water droplets.
Really, only the WBF conceptions make it possible to explain the phenomenon of significant
uncoordination between RICE and IVO readings in the interval #4 in Fig.2. Here the behavior of
IVO outputs is readily interpreted as the image of the frontal process of transforming water-1 cloud
(interval #5 and on) into phase-stable mixed cloud. The front of this cloud glaciation moves left to
right, the cloud itself staying unmoving. The deep decline of LWC curve within the frontal forward
zone results from evaporating water-1, while the ascent of TWC in the back zone is the result of the
growth of particles of A-water and ice newly arising on droplet “dry’ residuals (Nevzorov, 2006b,
2009). Both these processes are running at almost water-1 saturation which corresponds to very high
ice su persaturation of vapor pressure. Under this condition, the vapor excess over ice saturation can
deposit on the ice covering the RICE pin sensor, thereby creating the illusion of real condensed water
even outside a true cloud as seen in Fig.2. On this and abovesaid reasons, the RICE device may
claim to be objective enough icing indicator rather than an autonomous LWC probe, the more as a
reference instrument.
Thus only a single example of typically similar others seems to be enough to show the groundlessness of the speculative idea of distorting LWC measurement by the ‘ice effect’. The most convincing acknowledgement of the permanent presence of liquid droplets in ice-containing clouds lies
in the glory phenomenon typically arising around the airplane shadow in direct sunlight on tops of
high- and middle-level clouds. Really, there is the undeniable axiom that the glory is produced by
spherical particles, i.e. liquid or just frozen droplets.
4. Glory formation: virtual models and nature
Our recent papers (Nevzorov, 2006, 2009) were followed by the papers whose authors contest
our assertion of glory formation by the А-water droplets (Mayer and Emde, 2007; Romanov and
Doubnichenko, 2011). Their principal argument is the statement that the glory formation by the droplets of ordinary water-1 (with refractivity n =1.33) has been already proved by them and another authors beginning from van de Hulst (1957) .
In fact, all those authors follow analogous methodologies and present similar results, which
makes it possible to consider them together within a united virtual model of glory on water-1 spheres
with refractivity n = 1.33. Let us designate it W1-model, as opposed to AW-model with n ~ 1.81.
The W1-model is based on the belief that the glory naturally consists of several concentric
rings as this seemingly follows from Mie (Mayer et al., 2004, 2007; Romanov and Doubnichenko,
2011) and Debye (Laven, 2005) theories. The theoretical descriptions of this phenomenon are largely
focused on the relative position of the rings. Meanwhile, being failed to find any realistic explanations of physical nature of the secondary rings, van de Hulst (1957) has put forward an idea of “superficial waves” which supposedly deflect the light beams tangentially incident onto a spherical surface by a small discrete angle. Despite the absence of a sound proof, and for lack of any alternative
approach, this idea is still supported by some authors. The other, diffraction hypothesis though rejected by van de Hulst (1957) remains popular for speculative explanation of the phenomenon.
In the works of Mayer et al. (2004), Laven (2005) and other theorists in the W1-model, harmonic oscillations on the light scattering indicatrix are revealed in the form of attached "ripple", as
shown in Fig.3 copied from the cited paper; the peaks of the oscillations are interpreted by the authors as belonging to the glory rings.
Fig.3. Full indicatrix of light scattering by 12 µm sphere as calculated by Mayer et al.
(2004). The "ripples" on the graph result from the truncation of the Mie series, i.e. are in fact
the calculation error.
In fact, all observations of natural glory from aircraft1 including the author’s ones, show that
far not always the external rings do accompany the basic ring of the glory proper as classically defined (Minnaert, 1969). If occurring, their number rarely reaches a mere two; they are much weaker
and successively decreasing in brightness as compared with the basic ring.
1
See e.g. http://www.atoptics.co.uk/droplets/gloim.htm.
In our calculations of the scattering indicatrix with similar conditions such oscillations were
not at all detected, as shown in Figs. 4 to 6 below. The stated discrepancy between the both calculated results and their distinction from the natural phenomenon is a matter of principle and requires an
explanation which can be as follows.
Fig.4. Scattering indicatrixes by spheres with n=1.33 and n=1.81 of diameters
(µm) given in the legend. The legend format is “ droplet diameter (µm) /n”.
The solution of rigorous Mie theory for each combination of the scattering angle θ, the diffraction parameter x, and the refractivity n of glory-forming particles is the sum of infinite and weakly
convergent sign-variable series. In common real computations the number, N, of the summands in a
series is taken limited and equal for all θ. The N value being thus fixed, the series residual Δ (the difference between the sums of truncated and infinite series) is naturally harmonically dependent on all
the parameters, specifically on the scattering angle θ. Therefore, the dependence of both amplitude
and period of the fluctuations Δ on the angle θ as well as on droplet size range (insertion in Fig.3) is
nothing but a purely mathematical effect. Thus the theoretical W1-model under consideration is build
upon not only Mie theory, but also upon the sign-alternative error of computation. As a matter of
fact, Fig.3 reveals the dependence of optimal summand number N, as providing comprehensible accuracy of Mie computation, on the scattering angle θ.
Our calculations by Mie theory were made with the computer program developed by Petrushin
(1989), in which the number N of summands in every point of θ is not fixed but automatically increases until the residual Δ becomes less than a given negligible value. This algorithm permits calculated results to be as close to the rigorous Mie theory as desirable. By default, the results hereafter
presented were computed for yellow light with  = 0.58 µm.
Fig. 4 demonstrates a significant difference between the indicatrixes for the both models in that
that only at n = 1.33 the rainbow peak at θ ~ 140o is present being comparable in height with that at θ
~ 180о when droplet diameters exceed at least 5 ÷ 10 µm. This implies that the glory if occurring on
a cloud containing water-1 droplets must be accompanied by a concentric ring with angular radius of
about 40о. Really such a ring utterly rarely accompanies natural glory, and when occurs, perhaps
informs of simultaneous presence of both liquid disperse phases in a cloud or in a cloud system
which includes upper transparent layer(s) producing the colored glory.
It is of great importance that, as a fact, a distinct optical image of the backscattering phenomenon is formed not in the whole depth of cloud body where the diffuse (multiple) scattering suppresses the directed light beams, but in its frontier layer whose optical thickness is no more than a unity.
This strongly restricts the upper limit of image brightness. The backscattering indicatrix of monophase cloud of both liquid states keeps the same proportion as in Fig.4 because of being normalized to the same sum of droplet cross-sections per a unit area of the image-forming layer, according
to analytical definition of the optical thickness. As a result, it follows from Fig.4 that the glory on Awater droplets must be almost two orders brighter than the image formed in water-1 clouds under the
same sunlight.
Fig.5. Expanded backscattering parts of indicatrixes for sphere diameters (µm) as in legend, and n =
1.33.
Fig.6. As in Fig.5 for n = 1.81.
The details of the indicatrixes of yellow light scattering by the droplets of different nature and
size within the angle range adjacent to 180o and including the glory-forming peaks are plotted in
Figs.5 and 6 on the same linear scale for both models. In the both Figures the experimental domain
of 1.6 to 3.8 µm of radial angles of natural glory (Nevzorov, 2006a) is marked. As before, no peak
corresponding to the additional ring around a natural glory is present on the indicatrixes for both
models. In view of their natural incidental occurrence, brightness variability and certain geometric
features, we suggested that they are created by the peaks of secondary forward scattering of gloryforming beams by cloud ice crystals of specific shapes (Nevzorov, 2006a).
To simulate as well as possible the behavior of natural glory, the W1-model with n = 1.33 requires that a cloud consists only of highly monodisperse droplets (Mayer et al, 2004, 2007) of ~8 to
~16 µm modal diameter (Fig. 5). It is however known from thousands aircraft measurements of
cloud microstructure that such situation would meet extremely rare, if any, at least as compared with
the natural glory on high clouds. Real sun-lit atmospheric clouds of water-1 produce such optical image as diffused white-spot aureole. The entirely filled aureole around the plane shade on a cloud did
not attract special attention as inexpressive and rather rare in occurrence being most often shielded
from direct solar radiation by overlying layer(s).
In the AW-model with n = 1.81 (Fig. 6) a single backscattering peak on its scattering indicatrix
appears with droplet diameter exceeding somewhat less than 20 µm. In contrast to W1-model, the
peak from every droplet of widest size range from 20 µm to, at least, 160 µm entirely fit into the angle domain as experimentally determined. By their absolute height over the background, these peaks
surpass ones in the W1-model by as much as almost two orders. The presence in a cloud of droplets
smaller than 20 µm and/or ice crystals makes the glory-forming layer thinner and thereby the image
weakening. By this reason, smallest natural glories look as a rule much less contrast than biggest
ones. All this is why the visible (angular) size, brightness, and color contrast of the natural glory tend
to be positively correlated.
Thus, of both glory models under consideration, only one for n = 1.81 closely corresponds to the
natural glory as respect to its definition and properties (Nevzorov, 2006a). The analysis above convinces that the glory phenomenon is intimately connected with А-water droplets, reliably signifying
its presence in a cloud. It seems obvious that the presence of A-water droplets in ICCs appears as
common as the occurrence of a colored ring around a shadow cast by a sun-lit airplane.
Note that the interpretation of the remote sensing experiment by Mayer et al. (2004), though
usually referred to, cannot oppose the A-water conception by the reason that both the algorithm of
the inverse task and the interpretation of its solution are based on the same W1-model carrying the
spurious rings as above, and in addition no in situ control of cloud microstructure and even temperature was made. On the contrary, the brightness contrast and spatial stability of the described phenomenon despite of visual cloud inhomogeneity is fitting the inherent features of glory on a cold
stratiform cloud.
To summarize, we have made sure that in adequate understanding of physical nature of the optical phenomenon of on-cloud glory it is impossible to do without the A-water conception. Recent
model study of the problem by Prigarin et al. (2012) has supported this statement.
5. Conclusions
Considered here are the most resonant, in our opinion, arguments against our finding the existence of liquid amorphous water in natural cold clouds. These arguments refer to different aspects of
the phenomenon, but follow the same logic, proceeding from such assumptions that wittingly lead to
expected orthodox results, thus supposedly supporting a preconceived position of the opponents. Unfortunately, this artificial approach (apropos, not so infrequent in science) builds upon dogmatic
statements that may actually be or prove objectively wrong.
In both our topics under consideration, the replacement of well-know properties of water-1 by
the specific properties of A-water easily resolves the involved intractable problems without using
questionable, unnatural or inadequate, preconditions. Indeed, ignoring the fact of condensation equilibrium between liquid and ice in stable phase-mixed clouds leads to the absurd statement concerning
interaction between ice particles and a hot surface in airstream. Also this contradicts the fact of permanent occurrence of antisun glory on cold ice-containing clouds that is the reliable sign of the liquid droplets therein. In turn, the mandatory requirement of monodisperse cloud structure for glory
formation completely excludes its feasibility as to normal atmosphere clouds. The absence of regular
40o ring around a glory on stable phase-mixed cloud implies the absence of droplets of ordinary water-1 therein.
It stands specifically to note that such exasperating phenomenon as winter-type freezing precipitation has hitherto no reasonable explanatio but using the A-water conception.
Thus we tried to prove that every failure in negating or ignoring the A-water conception in the
microphysics of mixed clouds can thus be considered as an auxiliary convincing argument in favor
of its validity.
To finalize, the author is hopeful that the critical analysis presented above is sufficiently reasonable, objective and convincing.
Acknowledgements. The author is grateful to the CAO management for support the given research,
and to CAO scientific staff for its understanding and assistance in this work. We would be very much
obliged to those who despite prevailing skepticism has understood an essence and significance of
this most mysterious of problems of cloud physics, Especially we would welcome those honestminded and creative cloud physicists who will perform thorough and objective, free of prevailing
dogmas investigations to confirm or disprove the A-water conception.
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