Hygroscopicity of Different Types of Aerosol Particles: Case Studies Using Multi-Instrument Data in Megacity Beijing, China

Water uptake by aerosol particles alters its light-scattering characteristics significantly. However, the hygroscopicities of different aerosol particles are not the same due to their different chemical and physical properties. Such differences are explored by making use of extensive measurements concerning aerosol optical and microphysical properties made during a field experiment from December 2018 to March 2019 in Beijing. The aerosol hygroscopic growth was captured by the aerosol optical characteristics obtained from micropulse lidar, aerosol chemical composition, and aerosol particle size distribution information from ground monitoring, together with conventional meteorological measurements. Aerosol hygroscopicity behaves rather distinctly for mineral dust coarse-mode aerosol (Case I) and non-dust fine-mode aerosol (Case II) in terms of the hygroscopic enhancement factor, fβ(RH,λ532), calculated for the same humidity range. The two types of aerosols were identified by applying the polarization lidar photometer networking method (POLIPHON). The hygroscopicity for non-dust aerosol was much higher than that for dust conditions with the fβ(RH,λ532) being around 1.4 and 3.1, respectively, at the relative humidity of 86% for the two cases identified in this study. To study the effect of dust particles on the hygroscopicity of the overall atmospheric aerosol, the two types of aerosols were identified and separated by applying the polarization lidar photometer networking method in Case I. The hygroscopic enhancement factor of separated non-dust fine-mode particles in Case I had been significantly strengthened, getting closer to that of the total aerosol in Case II. These results were verified by the hygroscopicity parameter, κ (Case I non-dust particles: 0.357 ± 0.024; Case II total: 0.344 ± 0.026), based on the chemical components obtained by an aerosol chemical speciation instrument, both of which showed strong hygroscopicity. It was found that non-dust fine-mode aerosol contributes more during hygroscopic growth and that non-hygroscopic mineral dust aerosol may reduce the total hygroscopicity per unit volume in Beijing.

[1]  Alexei Kolgotin,et al.  Characterization of smoke and dust episode over West Africa: comparison of MERRA-2 modeling with multiwavelength Mie–Raman lidar observations , 2017, Atmospheric measurement techniques.

[2]  Holger Vömel,et al.  Intercomparison of humidity and temperature sensors: GTS1, Vaisala RS80, and CFH , 2011 .

[3]  S. Solomon The Physical Science Basis : Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change , 2007 .

[4]  Sang Woo Kim,et al.  Aerosol hygroscopic properties during Asian dust, pollution, and biomass burning episodes at Gosan, Korea in April 2001 , 2006 .

[5]  Chunsheng Zhao,et al.  Deliquescent phenomena of ambient aerosols on the North China Plain , 2016 .

[6]  Albert Ansmann,et al.  Hygroscopic properties and extinction of aerosol particles at ambient relative humidity in South-Eastern China , 2008 .

[7]  Zhanqing Li,et al.  Analysis of cloud layer structure in Shouxian, China using RS92 radiosonde aided by 95 GHz cloud radar , 2010 .

[8]  Zhanqing Li,et al.  Effect of aerosol humidification on the column aerosol optical thickness over the Atmospheric Radiation Measurement Southern Great Plains site , 2007 .

[9]  Dong Liu,et al.  Hygroscopic growth of atmospheric aerosol particles based on lidar, radiosonde, and in situ measurements: Case studies from the Xinzhou field campaign , 2017 .

[10]  Tomoaki Nishizawa,et al.  Synergistic effect of water-soluble species and relative humidity on morphological changes in aerosol particles in the Beijing megacity during severe pollution episodes , 2019, Atmospheric Chemistry and Physics.

[11]  F. G. Fernald Analysis of atmospheric lidar observations: some comments. , 1984, Applied optics.

[12]  David N. Whiteman,et al.  Absolute accuracy of water vapor measurements from six operational radiosonde types launched during AWEX-G and implications for AIRS validation , 2006 .

[13]  F. Frappart,et al.  Compared performances of SMOS-IC soil moisture and vegetation optical depth retrievals based on Tau-Omega and Two-Stream microwave emission models , 2020 .

[14]  S H Melfi,et al.  Remote measurements of the atmosphere using Raman scattering. , 1972, Applied optics.

[15]  Ting Yang,et al.  Formation and evolution mechanism of regional haze : a case study in the megacity Beijing , China , 2012 .

[16]  Albert Ansmann,et al.  Vertically resolved separation of dust and smoke over Cape Verde using multiwavelength Raman and polarization lidars during Saharan Mineral Dust Experiment 2008 , 2009 .

[17]  Lucas Alados-Arboledas,et al.  Hygroscopic growth of atmospheric aerosol particles based on active remote sensing and radiosounding measurements: selected cases in southeastern Spain , 2014 .

[18]  V. Grassian,et al.  Interactions of Water with Mineral Dust Aerosol: Water Adsorption, Hygroscopicity, Cloud Condensation, and Ice Nucleation. , 2016, Chemical reviews.

[19]  Steffen Beirle,et al.  Comparison of ambient aerosol extinction coefficients obtained from in-situ, MAX-DOAS and LIDAR measurements at Cabauw , 2010 .

[20]  V. Freudenthaler,et al.  Optical and microphysical properties of smoke over Cape Verde inferred from multiwavelength lidar measurements , 2011 .

[21]  Lidia Morawska,et al.  Concentrations of submicrometre particles from vehicle emissions near a major road , 2000 .

[22]  David N. Whiteman,et al.  Demonstration of Aerosol Property Profiling by Multiwavelength Lidar Under Varying Relative Humidity Conditions , 2009 .

[23]  Yuk L. Yung,et al.  Radiative absorption enhancement of dust mixed with anthropogenic pollution over East Asia , 2018, Atmospheric Chemistry and Physics.

[24]  A. Ansmann,et al.  Fine and coarse dust separation with polarization lidar , 2014 .

[25]  P. Reilly,et al.  Prediction of the properties of mixed electrolytes from measurements on common ion mixtures , 1969 .

[26]  W. R. Leaitch,et al.  The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation , 2010 .

[27]  Tim Elliott,et al.  Four Years of Continuous Surface Aerosol Measurements from the Department of Energy's Atmospheric Radiation Measurement Program Southern Great Plains Cloud and Radiation Testbed Site , 2022 .

[28]  Yele Sun,et al.  Analysis of Chemical Composition, Source and Processing Characteristics of Submicron Aerosol during the Summer in Beijing, China , 2019, Aerosol and Air Quality Research.

[29]  M. Petters,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity , 2006 .

[30]  Chunsheng Zhao,et al.  A novel method for deriving the aerosol hygroscopicity parameter based only on measurements from a humidified nephelometer system , 2017 .

[31]  Erik Swietlicki,et al.  Hygroscopic growth and critical supersaturations for mixed aerosol particles of inorganic and organic compounds of atmospheric relevance , 2005 .

[32]  Sonia M. Kreidenweis,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 3: Including surfactant partitioning , 2012 .

[33]  P. D. Girolamo,et al.  Raman lidar observations of a Saharan dust outbreak event: Characterization of the dust optical properties and determination of particle size and microphysical parameters , 2012 .

[34]  A. Dell'Acqua,et al.  Aerosol hygroscopicity at a regional background site (Ispra) in Northern Italy , 2012 .

[35]  Qiang Fu,et al.  Dust aerosol vertical structure measurements using three MPL lidars during 2008 China-U.S. joint dust field experiment , 2010, Journal of Geophysical Research.

[36]  Zhe Wang,et al.  Real-time observational evidence of changing Asian dust morphology with the mixing of heavy anthropogenic pollution , 2017, Scientific Reports.

[37]  Igor Veselovskii Interactive comment on “ Characterization of smoke / dust episode over West Africa : comparison of MERRA-2 modeling with multiwavelength Mie-Raman lidar observations , 2017 .

[38]  Bruce Morley,et al.  Aerosol hygroscopic properties as measured by lidar and comparison with in situ measurements , 2003 .

[39]  L. Alados-Arboledas,et al.  Monitoring of the Eyjafjallajökull volcanic aerosol plume over the Iberian Peninsula by means of four EARLINET lidar stations , 2011 .

[40]  G. A. Moreira,et al.  Hygroscopic growth study in the framework of EARLINET during the SLOPE I campaign: synergy of remote sensing and in situ instrumentation , 2017 .

[41]  Qi Zhang,et al.  Source apportionment of organic aerosol from 2-year highly time-resolved measurements by an aerosol chemical speciation monitor in Beijing, China , 2018, Atmospheric Chemistry and Physics.

[42]  Chuanfeng Zhao,et al.  East Asian Study of Tropospheric Aerosols and their Impact on Regional Clouds, Precipitation, and Climate (EAST‐AIRCPC) , 2019, Journal of Geophysical Research: Atmospheres.

[43]  Jonathan Crosier,et al.  © Author(s) 2007. This work is licensed under a Creative Commons License. Atmospheric Chemistry and Physics A revised linear ozone photochemistry parameterization for use in transport and general circulation models: multi-annual simulations , 2006 .

[44]  Zhanqing Li,et al.  Aerosol and boundary-layer interactions and impact on air quality , 2017 .

[45]  O. Boucher,et al.  A satellite view of aerosols in the climate system , 2002, Nature.

[46]  Yan Yin,et al.  Aerosol and monsoon climate interactions over Asia , 2016 .

[47]  Shihua Chen,et al.  De-noising and retrieving algorithm of Mie lidar data based on the particle filter and the Fernald method. , 2015, Optics express.

[48]  Ernest Weingartner,et al.  Effects of relative humidity on aerosol light scattering: results from different European sites , 2012 .

[49]  Fang Zhang,et al.  Aerosol chemistry and particle growth events at an urban downwind site in North China Plain , 2018, Atmospheric Chemistry and Physics.

[50]  Jing Li,et al.  Impact of aerosol hygroscopic growth on retrieving aerosol extinction coefficient profiles from elastic-backscatter lidar signals , 2017 .

[51]  B. Wehner,et al.  Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods , 2009 .

[52]  K. Moffett,et al.  Remote Sens , 2015 .

[53]  Pasi Aalto,et al.  Aerosol number size distributions from 3 to 500 nm diameter in the arctic marine boundary layer during summer and autumn , 1996 .

[54]  Ping Wang,et al.  Aerosol Optical Properties over China from RAMS-CMAQ Model Compared with CALIOP Observations , 2017 .

[55]  Vicki H. Grassian,et al.  The transformation of solid atmospheric particles into liquid droplets through heterogeneous chemistry: Laboratory insights into the processing of calcium containing mineral dust aerosol in the troposphere , 2003 .

[56]  Maureen Cribb,et al.  Significant contribution of organics to aerosol liquid water content in winter in Beijing, China , 2019, Atmospheric Chemistry and Physics.

[57]  S. H. Melfi,et al.  Raman lidar system for the measurement of water vapor and aerosols in the Earth's atmosphere. , 1992, Applied optics.

[58]  Qi Zhang,et al.  An Aerosol Chemical Speciation Monitor (ACSM) for Routine Monitoring of the Composition and Mass Concentrations of Ambient Aerosol , 2011 .

[59]  Qi Zhang,et al.  Liquid water: Ubiquitous contributor to aerosol mass , 2016 .

[60]  Wei Wang,et al.  Aerosol hygroscopic growth, contributing factors, and impact on haze events in a severely polluted region in northern China , 2019, Atmospheric Chemistry and Physics.

[61]  Zhanqing Li,et al.  Enhanced hydrophobicity and volatility of submicron aerosols under severe emission control conditions in Beijing , 2017, Atmospheric Chemistry and Physics.

[62]  Arnoud Apituley,et al.  Study of aerosol hygroscopic events over the Cabauw experimental site for atmospheric research (CESAR) using the multi-wavelength Raman lidar Caeli , 2015 .

[63]  Allen L. Robinson,et al.  Cloud condensation nuclei activity of fresh primary and aged biomass burning aerosol , 2012 .

[64]  Jie Guang,et al.  Correlation between PM concentrations and aerosol optical depth in eastern China , 2009 .