Aerosols, Light, and Water: Measurements of Aerosol Optical Properties at Different Relative Humidities
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Date
2016-01-01
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Physics
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Physics, Atmospheric
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This item may be protected under Title 17 of the U.S. Copyright Law. It is made available by UMBC for non-commercial research and education. For permission to publish or reproduce, please see http://aok.lib.umbc.edu/specoll/repro.php or contact Special Collections at speccoll(at)umbc.edu
Distribution Rights granted to UMBC by the author.
Distribution Rights granted to UMBC by the author.
Abstract
The Earth'satmosphere is composed of a large number of different gases as well as tiny suspended particles, both in solid and liquid state. These tiny particles,called atmospheric aerosols, have an immense impact on our health and on our global climate. Atmospheric aerosols influence the Earth'sradiation budget both directly and indirectly. In the direct effect, aerosols scatter and absorb sunlight changing the radiative balance of the Earth-atmosphere system. Aerosols indirectly influence theEarth'sradiation budget by modifying the microphysical and radiative properties of clouds as well as their water content and lifetime.In ambient conditions, aerosol particles experience hygroscopic growth due to the influence of relative humidity (RH), scattering more light than when the particles are dry. The quantitative knowledge of the RH effect and its influence on the light scattering coefficient and, in particular, on the phase function and polarization of aerosol particles is of substantial importance when comparing ground based observations with other optical aerosol measurements techniques such satellite and sunphotometric retrievals of aerosol optical depth and their inversions.This dissertations presents the aerosol hygroscopicity experiment investigated using a novel dryer-humidifier system, coupled to a TSI-3563 nephelometer, to obtain the light scattering coefficient (sp) as a function of relative humidity (RH) in hydration and dehydration modes. The measurements were performed in Porterville, CA (Jan 10-Feb 6, 2013), Baltimore, MD (Jul 3-30, 2013), and Golden, CO(Jul 12 - Aug 10, 2014). Observations in Porterville and Golden were part of theNASA-sponsored DISCOVER-AQ project. The measured sp under varying RH in the three sites was combined with ground aerosol extinction, PM2:5mass concentrations, particle composition measurements, and compared with airborne observations performed during campaigns. The enhancement factor, f(RH), defined as the ratio of sp(RH) at a certain RH divided by sp at a dry value, was used to evaluate the aerosol hygroscopicity. Different empirical fits were evaluated using the f(RH) data. The widely used gamma model was found inappropriate, as it overestimates f(RH) for RH<75%. Abetter empirical fit with two power-law curve-fitting parameters c and k was found to replicate f(RH) accurately from the three sites. The relationship between the organic carbon mass (OMC) and the species that are affected by RH and f(RH) was also studied and categorized between the sites. A second experiment is reported where the first two elements of the scatter-ing matrix of laboratory generated particles were studied under different humidity conditions. The non-spherical particles generated were ammonium sulfate, sodium chloride, and ammonium nitrate. The optical measurements were performed with a polarized imaging nephelometer (PI-Neph) installed in series with the humidifier dryer apparatus. The inorganic salts experienced low (<30%) and high (>80%) RH levels so that the observations could contrast the differences when the salts were crystallized (low RH) and when the particles turned to aqueous solutions after deliquesence (high RH). The measurements with the PI-Neph produce the aerosol phase function and the polarized phase function in a range of angles that go from3to177. The results showed significant changes in the phase function and polarized phase function due to the hygroscopic growth. Although the inorganic salts used inthe experiments were non-spherical, the dry measurements were successfully reproduced with the Mie theory using literature values for the dry index of refraction. Moreover, the changes in the particle size distribution and index of refraction were evaluated through classic thermodynamic equilibrium theory producing comparable results with the simulations performed with Mie formalism.The final experiment consisted in the measurements of phase function and degree of linear polarization of ambient aerosols sampled in Baltimore, MD with the PI-Neph. This study was centered on specific case studies where different aerosol conditions were experienced such as clean, haze episode, and transported smoke event. The approach employed consisted of dry and humid observations of ambient aerosols to compare them with total column products by AERONET. A relatively low difference between the phase function and the degree of linear polarization was measured at high and low RH. The small difference found in the scattering elements and their retrievals is attributed to the general aerosol composition in the region. It was observed that a RH increase causes the particles to scatter more light uniformly over all the scattering angles, and also, that the water uptake did not change markedly the particle'spolarization properties. The comparison between in-situ and total column derived observations were highly correlated for most of the cases. The size distribution retrievals from the in-situ measurements were very comparable to the size distributions reported by AERONET, but only for the fine modes.