Optical Properties of Aerosol Particles Based on Size-Resolved Chemical Composition: Data Analysis Algorithm Development Mariya Petrenko, Derek Montague, Peter Liu, and Terry Deshler Department of Atmospheric Science, University of Wyoming, Laramie, Wyoming 82071, USA Introduction Atmospheric aerosol particles play a significant role in determining Earth's climate, through their interactions with solar radiation (the direct effect), and through their action as cloud condensation nuclei (the indirect effect). Our current ability to predict the aerosol direct effect on the atmospheric radiation balance on both global and local scales is restricted by a number of factors, among which are the high variability of aerosol properties in space and time, and instrumentation limitations for the production of quantitative size-dependent particle chemical composition and optical properties data with high time resolution. Comprehensive studies of the relationship of aerosol optical properties to particle composition as a function of size are therefore needed to improve our ability to compute radiative scattering by the aerosol on all size scales. Laramie, WY One goal of this study is the development of a data analysis algorithm to calculate aerosol scattering extinction, and hence overall optical properties, using the sizedependent chemical composition of the particles. The algorithm is being tested with data from comprehensive measurements obtained at the UW Keck Aerosol Laboratory in Laramie, WY during the Elk Mountain/Laramie Aerosol Characterization Experiment (EMLACE) in the summer of 2005. A partial data set from August 3, 2005 is shown below. Experimental Setup and Instrumentation Aerodyne Aerosol Mass Spectrometer (AMS) Roof Inlet Size-resolved chemical composition data (SO4, NO3, NH4, Organics) from AMS 0.5 lpm Measures total mass loading (μg/m3) of volatile aerosol species and their size-resolved mass loading (20-1000 nm vacuum aerodynamic diameter range) Heat Coil Data Analysis Scanning Mobility Particle Sizer (SMPS) Measures particle size distribution in 15-770 nm mobility diameter range. (resolution 64 chan/decade, averaging time interval: 303 sec) Total mass loadings from filterpacks (sulphates, nitrates, organics, black carbon, refractory material) To pump 1.Simple/complicated chemical Size-resolved composition chemical model composition (dM/dlogD or dM/dD) RH Sensor TSI 3-wavelength Integrating Nephelometer Measures total- and back-scattering coefficients at 3 wavelengths: 700 nm (red), 550 nm (green), and 450 nm (blue) Aethalometer Measures mass loading of black carbon (μg/m3) 4 lpm Ultrafine Condensation Particle Counter (UCPC) Counts number concentration (up to 105 cm-3) of particles of the size 3 nm and higher 5. Mie Total scattering coefficient calculated calculations from the sampled aerosol 1 lpm Aerodynamic Particle Sizer (APS) (5.0 lpm) Measures particle size distribution in 0.5-20 μm aerodynamic diameter range (resolution 32 chan/decade, averaging time – 1 min) Passive Cavity Aerosol Spectrometer Probe (PCASP) (0.5 lpm) Measures particle size distribution in 0.13 μm optical diameter range (resolution 30 chan total, averaging time – 1sec) Surface Aerosol Properties, Laramie, WY Comparison/ optical closure Size-resolved Refractive index (n) 2. Partial Molar of comprehensive Refraction (PMR) size distribution method for n calc. (Stelson, 1982) Total scattering coefficient measurements from Nephelometer Data Processing Algorithm Development Alignment of size distributions for generated aerosols 2. Partial Molar Refraction (PMR) method for n calc. (Stelson, 1982) 3.Volumeweighted density in each particle size range Mass Closure Size-resolved Refractive index (n) and density (ρ) Comprehensive size distribution over 15 nm – 20 μm size range 4. Diameter conversion and distributions alignment method Size-distribution measurements from SMPS, PCASP, and APS Preliminary Results and Conclusions •The general data analysis algorithm has been tested using lab-generated aerosols (sodium nitrate, ammonium nitrate, and ammonium sulphate). •Size distributions of labgenerated poly- and monodisperse aerosols measured by the APS and SMPS are in excellent agreement. Comparison of PCASP distributions with those from the APS and SMPS show some variability, but are nevertheless reasonable. Optical closure (total scattering coefficient) References • Bohren, C. F. and Huffman, D. R.: Absorption and scattering by small particles, John Wiley and Sons, Inc., 1983 • DeCarlo, P., Slowik, J. G., Worsnop, D. R., Davidovits, P., and Jimenez, J. L.: Particle morphology and density characterization by combined mobility and aerodynamic diameter measurements. Part I: Theory. Aerosol Science and Technology, 38: 1185–1205, 2004. DOI: 10.1080/027868290903907 • • Calc-Blue TotS Cf-B % diff 1.5E-05 1.6E-05 8.25 2.1E-05 2.3E-05 6.82 2E-05 2.2E-05 11.75 1.6E-05 1.8E-05 11.01 1.5E-05 1.6E-05 9.06 1.4E-05 1.5E-05 6.99 Calc -Green TotS Cf-G % diff Calc-Red TotS Cf-R % diff 8.264E-06 8.49E-06 2.70 3.73E-06 3.9E-06 4.47 1.2776E-05 1.33E-05 3.94 6.48E-06 6.5E-06 0.19 0.00001156 1.25E-05 7.31 5.74E-06 6.1E-06 5.80 9.7097E-06 1.13E-05 13.84 5.26E-06 6E-06 11.84 1.0886E-05 1.15E-05 4.99 5.86E-06 6E-06 1.62 1.0511E-05 1.09E-05 3.73 5.54E-06 5.7E-06 2.82 Total extinction coefficient for ammonium sulphate ((NH4)2SO4) polydisperse aerosol calculated using Mie theory for TSI Hand, J. L. and Kreidenweis, S. M.: Size corrections based on refractive index for Particle Measuring Nephelometer wavelengths: red (700 nm), green (550 nm) and blue Systems Active Scattering Aerosol Spectrometer Probe, CIRA report 0373-5352-31, Colorado State (450 nm) over 7-170 degrees (determined by instrument optics), University, Fort Collins, CO, 1996 compared with the total scattering coefficient measured by the TSI Nephelometer. Stelson, A. W.: Urban aerosol refractive index prediction by partial molar refraction approach, Environ. Sci. Technol., 24, 1676–1679, 1990 •Comparison of measured scattering extinctions at three wavelengths for dried polydisperse (NH4)2SO4 aerosol with values calculated by Mie theory using measured size distributions are in very good agreement (≤ 14%). •The analytical tools developed in this study are now being applied to the ambient aerosol data acquired during EMLACE. These analyses account for variability in the size-dependent chemical composition of the particles.