Modeling the spectral optical properties of ammonium sulfate and biomass burning aerosols: parameterization of relative humidity effects and model results

1999 ◽  
Vol 33 (17) ◽  
pp. 2603-2620 ◽  
Author(s):  
Keith Eric Grant ◽  
Catherine C. Chuang ◽  
Allen S. Grossman ◽  
Joyce E. Penner
2017 ◽  
Author(s):  
Ting Lei ◽  
Andreas Zuend ◽  
Yafang Cheng ◽  
Hang Su ◽  
Weigang Wang ◽  
...  

Abstract. Hygroscopic growth factors of organic surrogate compounds representing biomass burning and mixed organic-inorganic aerosol particles exhibit variability during dehydration experiments depending on their chemical composition, which we observed using a hygroscopicity tandem differential mobility analyzer (HTDMA). We observed that levoglucosan and humic acid aerosol particles release water slightly in the range of 90–5 % relative humidity (RH). 4-Hydroxybenzoic acid aerosol particles, however, remain in the solid state without diameter growth and even slightly shrinking at higher RH compared to the dry size. The measurements were accompanied by RH-dependent thermodynamic equilibrium calculations using the AIOMFAC and the E-AIM models, the ZSR relation, and a fitted hygroscopicity expression. We observed several effects of organic components on the hygroscopicity behavior of mixtures containing ammonium sulfate (AS) in relation to the different mass fractions of organic compounds: (1) a shift of efflorescence relative humidity (ERH) of ammonium sulfate to higher RH due to the presence of 25 wt % levoglucosan in the mixture. (2) There is a distinct efflorescence transition at 25 % RH for mixtures consisting of 25 wt % of 4-hydroxybenzoic acid compared to the ERH at 35 % for organic-free AS particles. (3) There is indication for a liquid-to-solid phase transition of 4-hydroxybenzoic acid in the mixed particles during dehydration. (4) A humic acid component shows no significant effect on the efflorescence of AS in mixed aerosol particles. In addition, relatively good measurement-model agreement in the case of the AIOMFAC and E-AIM models is mainly due to composition-dependent consideration of crystallization of AS in the model prediction. The use of the ZSR relation leads to good agreement with measured diameter growth factors of aerosol particles containing humic acid and ammonium sulfate. A similarity of the hygroscopicity parameter ĸ for organic surrogate compounds mixed with ammonium sulfate for different mass fractions during the different seasonal periods in the Amazon is observed. The RH-dependent hygroscopicity parameter ĸ measured at sub-saturated is consistent with kappa values for observations in the central Amazon Basin at the same environment, which suggests the similar O : C ratios and ammonium sulfate mass fraction in the laboratory and field observation conditions.


1997 ◽  
Vol 63 (2) ◽  
pp. 194-198
Author(s):  
Maher Samet ◽  
Kaworu Nakamura

2015 ◽  
Vol 15 (10) ◽  
pp. 5429-5442 ◽  
Author(s):  
E. Giannakaki ◽  
A. Pfüller ◽  
K. Korhonen ◽  
T. Mielonen ◽  
L. Laakso ◽  
...  

Abstract. Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.


Author(s):  
Lifu Yang ◽  
Madura Pathirage ◽  
Huaizhi Su ◽  
Mohammed Alnaggar ◽  
Giovanni Di Luzio ◽  
...  

2021 ◽  
Author(s):  
Maria Ángeles Burgos Simón ◽  
Elisabeth Andrews ◽  
Gloria Titos ◽  
Angela Benedetti ◽  
Huisheng Bian ◽  
...  

<p>The particle hygroscopic growth impacts the optical properties of aerosols and, in turn, affects the aerosol-radiation interaction and calculation of the Earth’s radiative balance. The dependence of particle light scattering on relative humidity (RH) can be described by the scattering enhancement factor f(RH), defined as the ratio between the particle light scattering coefficient at a given RH divided by its dry value.</p><p>The first effort of the AeroCom Phase III – INSITU experiment was to develop an observational dataset of scattering enhancement values at 26 sites to study the uptake of water by atmospheric aerosols, and evaluate f(RH) globally (Burgos et al., 2019). Model outputs from 10 Earth System Models (CAM, CAM-ATRAS, CAM-Oslo, GEOS-Chem, GEOS-GOCART, MERRAero, TM5, OsloCTM3, IFS-AER, and ECMWF) were then evaluated against this in-situ dataset. Building on these results, we investigate f(RH) in the context of other aerosol optical and chemical properties, making use of the same 10 Earth System Models (ESMs) and in-situ measurements as in Burgos et al. (2020) and Titos et al. (2021).</p><p>Given the difficulties of deploying and maintaining instrumentation for long-term, accurate and comprehensive f(RH) observations, it is desirable to find an observational proxy for f(RH). This observation-based proxy would also need to be reproduced in modelling space. Our aim here is to evaluate how ESMs currently represent the relationship between f(RH), scattering Ångström exponent (SAE), and single scattering albedo (SSA). This work helps to identify current challenges in modelling water-uptake by aerosols and their impact on aerosol optical properties within Earth system models.</p><p>We start by analyzing the behavior of SSA with RH, finding the expected increase with RH for all site types and models. Then, we analyze the three variables together (f(RH)-SSA-SAE relationship). Results show that hygroscopic particles tend to be bigger and scatter more than non-hygroscopic small particles, though variability within models is noticeable. This relationship can be further studied by relating SAE to model chemistry, by selecting those grid points dominated by a single chemical component (mass mixing ratios > 90%). Finally, we analyze model performance at three specific sites representing different aerosol types: Arctic, marine and rural. At these sites, the model data can be exactly temporally and spatially collocated with the observations, which should help to identify the models which exhibit better agreement with measurements and for which aerosol type.</p><p> </p><p>Burgos, M.A. et al.: A global view on the effect of water uptake on aerosol particle light scattering. Sci Data 6, 157. https://doi.org/10.1038/s41597-019-0158-7, 2019.</p><p>Burgos, M.A. et al.: A global model–measurement evaluation of particle light scattering coefficients at elevated relative humidity, Atmos. Chem. Phys., 20, 10231–10258, https://doi.org/10.5194/acp-20-10231-2020, 2020.</p><p>Titos, G. et al.: A global study of hygroscopicity-driven light scattering enhancement in the context of other in-situ aerosol optical properties, Atmos. Chem. Phys. Discuss. [preprint], https://doi.org/10.5194/acp-2020-1250, in review, 2020.</p>


2012 ◽  
Vol 12 (7) ◽  
pp. 3437-3454 ◽  
Author(s):  
C. S. Zender ◽  
A. G. Krolewski ◽  
M. G. Tosca ◽  
J. T. Randerson

Abstract. Land clearing for crops, plantations and grazing results in anthropogenic burning of tropical forests and peatlands in Indonesia, where images of fire-generated aerosol plumes have been captured by the Multi-angle Imaging SpectroRadiometer (MISR) since 2001. Here we analyze the size, shape, optical properties, and age of distinct fire-generated plumes in Borneo from 2001–2009. The local MISR overpass at 10:30 a.m. misses the afternoon peak of Borneo fire emissions, and may preferentially sample longer plumes from persistent fires burning overnight. Typically the smoke flows with the prevailing southeasterly surface winds at 3–4 m s−1, and forms ovoid plumes whose mean length, height, and cross-plume width are 41 km, 708 m, and 27% of the plume length, respectively. 50% of these plumes have length between 24 and 50 km, height between 523 and 993 m and width between 18% and 30% of plume length. Length and cross-plume width are lognormally distributed, while height follows a normal distribution. Borneo smoke plume heights are similar to previously reported plume heights, yet Borneo plumes are on average nearly three times longer than previously studied plumes. This could be due to sampling or to more persistent fires and greater fuel loads in peatlands than in other tropical forests. Plume area (median 169 km2, with 25th and 75th percentiles at 99 km2 and 304 km2, respectively) varies exponentially with length, though for most plumes a linear relation provides a good approximation. The MISR-estimated plume optical properties involve greater uncertainties than the geometric properties, and show patterns consistent with smoke aging. Optical depth increases by 15–25% in the down-plume direction, consistent with hygroscopic growth and nucleation overwhelming the effects of particle dispersion. Both particle single-scattering albedo and top-of-atmosphere reflectance peak about halfway down-plume, at values about 3% and 10% greater than at the origin, respectively. The initially oblong plumes become brighter and more circular with time, increasingly resembling smoke clouds. Wind speed does not explain a significant fraction of the variation in plume geometry. We provide a parameterization of plume shape that can help atmospheric models estimate the effects of plumes on weather, climate, and air quality. Plume age, the age of smoke furthest down-plume, is lognormally distributed with a median of 2.8 h (25th and 75th percentiles at 1.3 h and 4.0 h), different from the median ages reported in other studies. Intercomparison of our results with previous studies shows that the shape, height, optical depth, and lifetime characteristics reported for tropical biomass burning plumes on three continents are dissimilar and distinct from the same characteristics of non-tropical wildfire plumes.


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