[1] The refractive index is the fundamental property controlling aerosol optical properties. Secondary organic aerosol (SOA) real refractive indices (m r ) were derived from polar nephelometer measurements using parallel and perpendicular polarized 670 nm light, using a genetic algorithm method with Mie-Lorenz scattering theory and measured particle size distributions. The absolute error associated with the m r retrieval is ±0.03, and the instrument has sufficient sensitivity to achieve reliable retrievals for particles larger than about 200 nm. SOA generated by oxidizing a-pinene, b-pinene, and toluene with ozone and NO x /sunlight are explored. Retrieved refractive indices for the SOA vary between 1.38 and 1.61, depending on several factors. For a-and b-pinene ozonolysis, SOA m r ranges from 1.4 to 1.5 and, within the resolution of our method and bounds of our experiments, is not affected by the addition of an OH scavenger, and is only slightly dependent on the aerosol mass concentration. For photochemically generated SOA, m r generally increases as experiments progress, ranging from about 1.4 to 1.53 for a-pinene, 1.38 to 1.53 for b-pinene, and 1.4 to 1.6 for toluene. The pinene SOA m r appear to decrease somewhat toward the end of the experiments. Aspects of the data suggest aerosol mass concentration, oxidation chemistry, temperature, and aerosol aging may all influence the refractive index. There is more work to be done before recommendations can be made for atmospheric applications, but our calculations of the resulting asymmetry parameter indicate that a single value for SOA refractive index will not be sufficient to accurately model radiative transfer.Citation: Kim, H., B. Barkey, and S. E. Paulson (2010), Real refractive indices of a-and b-pinene and toluene secondary organic aerosols generated from ozonolysis and photo-oxidation,
The refractive index is an important property affecting aerosol optical properties, which in turn help determine the aerosol direct effect and satellite retrieval results. Here, we investigate the real refractive indices (m(r)) of secondary organic aerosols (SOA) generated from the photooxidation of limonene and α-pinene with different HC/NO(x) ratios. Refractive indices were obtained from polar nephelometer data using parallel and perpendicular polarized 532 nm light combined with measured size distributions, and retrievals were performed using a genetic algorithm and Mie-Lorenz scattering theory. The absolute error associated with the m(r) retrieval is ±0.03, and reliable retrievals are possible for mass concentrations above 5-20 μg/m(3) depending on particle size. The limonene SOA data suggest the most important factor controlling the refractive index is the HC/NO(x) ratio; the refractive index is much less sensitive to the aerosol age or mass concentration. The refractive index ranges from about 1.34 to 1.56 for limonene and from 1.36 to 1.52 for α-pinene, and generally decreases as the HC/NO(x) ratio increases. Especially for limonene, the particle diameter is also inversely related to the HC/NO(x) ratio; the final size mode increases from 220 to 330 nm as the HC/NO(x) ratio decreases from 33 to 6. In an effort to explore the ability of models from the literature to explain the observed refractive indices, a recent limonene oxidation mechanism was combined with SOA partitioning and a structure-property relationship for estimating refractive indices of condensing species. The resulting refractive indices fell in a much narrower range (1.475 ± 0.02) of m(r) than observed experimentally. We hypothesize the experimentally observed high m(r) values are due to oligomerization and the low values to water uptake, small soluble molecules such as glyoxal and other factors, each of which is not included in the oxidation mechanism. Aerosol formation yields were measured over the mass concentration range from 6 to ∼150 μg/m(3), over which they increased steadily, and were higher for high HC/NO(x) ratio experiments.
A polar nephelometer that measures the light scattered into a two dimensional plane by a stream of aerosols that intersect a 350 milliwatt diode laser beam with a wavelength of 670 nm is described. A half wave plate is used to orient the laser light both parallel and perpendicular to the measurement plane. This scattering information combined with simultaneously measured size distribution information is used to determine the real (m r ) refractive index of the aerosols using a Genetic Algorithm search method. Errors in the retrieved m r based on noise in the scattering measurement as well as uncertainties in the size distribution measurement are examined. The m r of polystyrene latex spheres and ammonium sulfate droplets are determined and match expectations within experimental uncertainties using Mie-Lorenz theory. The angular scattering properties of spherical secondary organic aerosols generated by oxidizing α-pinene do not follow this theory and calls into question the inferred m r .
We report on a small, lightweight polar nephelometer for the measurement of the light-scattering properties of cloud particles, specifically designed for use on a balloonborne platform in cirrus cloud conditions. The instrument consists of 33 fiber-optic light guides positioned in a two-dimensional plane from 5 degrees to 175 degrees that direct the scattered light to photodiode detectors-amplifier units. The system uses an onboard computer and data acquisition card to collect and store the measured signals. The instrument's calibration is tested by measurement of light scattered into a two-dimensional plane from small water droplets generated by an ultrasonic humidifier. Excellent comparisons between the measured water-droplet scattering properties and expectations generated by Mie calculation are shown. The measured scattering properties of ice crystals generated in a cold chamber also compare reasonably well with the theoretical results based on calculations from a unified theory of light scattering by ice crystals that use the particle size distribution measured in the chamber.
Angular scattering properties of ice crystal particles generated in a laboratory cloud chamber are measured with a lightweight polar nephelometer with a diode laser beam. This cloud chamber produces distinct plate and hollow column ice crystal types for light-scattering experiments and provides a controlled test bed for comparison with results computed from theory. Ice clouds composed predominantly of plates and hollow columns generated noticeable 22 degrees and 46 degrees halo patterns, which are predicted from geometric ray-tracing calculations. With the measured ice crystal shape and size distribution, the angular scattering patterns computed from geometrical optics with a significant contribution by rough surfaces closely match those observed from the nephelometer.
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