Simultaneous estimation of aerosol optical constants and size distribution from angular light-scattering measurement signals

The angular light-scattering measurement（ALSM） method combined with an improved artificial bee colony algorithm is introduced to determine aerosol optical constants and aerosol size distribution（ASD） simultaneously. Meanwhile, an optimized selection principle of the ALSM signals based on the sensitivity analysis and principle component analysis（PCA）is proposed to improve the accuracy of the retrieval results. The sensitivity analysis of the ALSM signals to the optical constants or characteristic parameters in the ASD is studied first to find the optimized selection region of measurement angles. Then, the PCA is adopted to select the optimized measurement angles within the optimized selection region obtained by sensitivity analysis. The investigation reveals that, compared with random selection measurement angles, the optimized selection measurement angles can provide more useful measurement information to ensure the retrieval accuracy. Finally,the aerosol optical constants and the ASDs are reconstructed simultaneously. The results show that the retrieval accuracy of refractive indices is better than that of absorption indices, while the characteristic parameters in ASDs have similar retrieval accuracy. Moreover, the retrieval accuracy in studying L-N distribution is a little better than that in studying Gamma distribution for the difference of corresponding correlation coefficient matrixes of the ALSM signals. All the results confirm that the proposed technique is an effective and reliable technique in estimating the aerosol optical constants and ASD simultaneously.

Aerosol size distributions during haze episodes in winter in Jinan, China

Number concentrations and distributions of 10-10,000 nm particles in a large city （Jinan） in the North China Plain were measured in winter 2009. The mean number concentrations of nucleation mode （10-20 nm）, Aitken mode （20-100 nm）, and accumulation mode （100-1000 nm） particles, as well as total particles were 925, 6898, 2476, and 10,299cm-3, respectively. Two severe haze episodes, with elevated concentrations caused by pollutants accumulating, were observed. Accumulation mode particle concen- trations were significantly higher during the episodes than on clear days, and nucleation mode particle concentrations were pronouncedly higher on clear days than during the episodes. The peaks of domi- nant number, surface area, and mass size distributions were around 30-50, 200-300, and 200-400 rim, respectively, both during the haze episodes and on clear days, but elevated mass and surface area con- centrations around 500-600 nm were also observed during the haze episodes, suggesting these particles had significant contributions to haze formation. These particles were probably formed through larger droplets in cloud and fog evaporating. Two new particle formation events, probably triggered by strong photochemical processes on clear days and significant traffic emissions during haze episode 2, were found. Significant insights were made into haze formation in a oolluted Chinese urban area.

Preliminary study on concentrations and size distribution of marine aerosols over the East China Sea

In summer and winter, 1987,and in spring and autumn, 1988, the concentrations and size distribution of marine aerosols were measured over the East China Sea and the South Japan Sea. This paper deals with the study on the seasonal variation of the marine aerosols with the meteorological parameters, the differences and the relations between the marine and continental aerosols. The results show that the marine aerosol concentrations and size distribution over the East China Sea have distinct seasonal change characteristics, which may be attributed to the East Asian atmospheric circulation. The size distribution is discussed by using a three-parameter size distribution model.

Airborne Observations of Cloud Condensation Nuclei Spectra and Aerosols over East Inner Mongolia

A set of vertical profiles of aerosol number concentrations, size distributions and cloud condensation nuclei（CCN）spectra was observed using a passive cloud and aerosol spectrometer（PCASP） and cloud condensation nuclei counter, over the Tongliao area, East Inner Mongolia, China. The results showed that the average aerosol number concentration in this region was much lower than that in heavily polluted areas. Monthly average aerosol number concentrations within the boundary layer reached a maximum in May and a minimum in September, and the variations in CCN number concentrations at different supersaturations showed the same trend. The parameters c and k of the empirical function N = c S^kwere 539 and1.477 under clean conditions, and their counterparts under polluted conditions were 1615 and 1.42. Measurements from the airborne probe mounted on a Yun-12（Y12） aircraft, together with Hybrid Single-Particle Lagrangian Integrated Trajectory model backward trajectories indicated that the air mass from the south of Tongliao contained a high concentration of aerosol particles（1000–2500 cm^（-3）） in the middle and lower parts of the troposphere. Moreover, detailed intercomparison of data obtained on two days in 2010 indicated that the activation efficiency in terms of the ratio of NCCNto N_a（aerosols measured from PCASP） was 0.74（0.4 supersaturations） when the air mass mainly came from south of Tongliao, and this value increased to 0.83 on the relatively cleaner day. Thus, long-range transport of anthropogenic pollutants from heavily polluted mega cities,such as Beijing and Tianjin, may result in slightly decreasing activation efficiencies.

A Comparison of Two Bulk Microphysics Parameterizations for the Study of Aerosol Impacts on an Idealized Supercell

Idealized supercell storms are simulated with two aerosol-aware bulk microphysics schemes(BMSs),the Thompson and the Chen-Liu-Reisner(CLR),using the Weather Research and Forecast(WRF)model.The objective of this study is to investigate the parameterizations of aerosol effects on cloud and precipitation characteristics and assess the necessity of introducing aerosols into a weather prediction model at fine grid resolution.The results show that aerosols play a decisive role in the composition of clouds in terms of the mixing ratios and number concentrations of liquid and ice hydrometeors in an intense supercell storm.The storm consists of a large amount of cloud water and snow in the polluted environment,but a large amount of rainwater and graupel instead in the clean environment.The total precipitation and rain intensity are suppressed in the CLR scheme more than in the Thompson scheme in the first three hours of storm simulations.The critical processes explaining the differences are the auto-conversion rate in the warm-rain process at the beginning of storm intensification and the low-level cooling induced by large ice hydrometeors.The cloud condensation nuclei(CCN)activation and auto-conversion processes of the two schemes exhibit considerable differences,indicating the inherent uncertainty of the parameterized aerosol effects among different BMSs.Beyond the aerosol effects,the fall speed characteristics of graupel in the two schemes play an important role in the storm dynamics and precipitation via low-level cooling.The rapid intensification of storms simulated with the Thompson scheme is attributed to the production of hail-like graupel.

Observed Changes in Aerosol Physical and Optical Properties before and after Precipitation Events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter ＆lt;0.8 μm [measured using an aerodynamic particle sizer（APS）], and fine particles with diameter ＆lt;0.1 μm [measured using a scanning mobility particle sizer（SMPS）]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution（measured using the SMPS） before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.

Field study of a soft X-ray aerosol neutralizer combined with electrostatic classifiers for nanoparticle size distribution measurements

Most conventional aerosol neutralizers are based on radioactive sources, which are controlled by strict regulations restricting their handling, transport, and storage. The TSI 3087 soft X-ray （SXR） neutralizer circumvents these legal restrictions. The aim of the present work is to compare the performance of a standalone SXR aerosol neutralizer with that of conventional radioactive aerosol neutralizers based on 85Kr （TSI 3077） and 241Am （Grimm 5522） by performing field tests in a real environmental scenario. The results obtained when the SXR neutralizer was connected to a mobility particle sizer spectrometer （MPS）, different from the device suggested by the manufacturer, were comparable with those obtained with the use of radioactive aerosol neutralizers. In changing the neutralizer, the particle number concentrations, measured with the MPS connected to the SXR neutralizer, almost remained within the 10% uncertainty bounds for the particle size interval 10-300 nm, when diffusion losses inside the SXR tube were considered. Based on our comparisons, the SXR neutralizer can be regarded as a standalone instrument that could solve the problems associated with legal restrictions on radioactive neutralizers and fulfil the need for a portable instrument for different field test purposes.

GROUND-BASED REMOTE SENSING OF THE SIZE DISTRIBUTION OF PINATOBU'S VOLCANIC CLOUD

In this paper,data of solar direct spectral radiance observation in summer and autumn of 1990 and 1991 were used to derive the average atmospheric extinction spectra for very clear days each year.The difference of these two extinction spectra is obvious and considered as the contribution of volcanic cloud resulting from Pinatobu's volcanic eruption in middle June of 1991.This average size distribution of volcanic cloud was retrieved from the difference spectra and given in this paper which will be useful for estimation and modeling of the effects of volcanic eruption.

Chemical characteristics of size-resolved aerosols in winter in Beijing

Size-resolved aerosols were continuously collected by a Nano Sampler for 13 days at an urban site in Beijing during winter 2012 to measure the chemical composition of ambient aerosol particles. Data collected by the Nano Sampler and an ACSM（Aerodyne Aerosol Chemical Speciation Monitor） were compared. Between the data sets,similar trends and strong correlations were observed,demonstrating the validity of the Nano Sampler. PM10 and PM2.5concentrations during the measurement were 150.5 ± 96.0 μg/m3（mean ± standard variation）and 106.9 ± 71.6 μg/m3,respectively. The PM2.5/PM10 ratio was 0.70 ± 0.10,indicating that PM2.5dominated PM10. The aerosol size distributions showed that three size bins of 0.5–1,1–2.5 and 2.5–10 μm contributed 21.8%,23.3% and 26.0% to the total mass concentration（TMC）,respectively. OM（organic matter） and SIA（secondary ionic aerosol,mainly SO42-,NO3-and NH4＋） were major components of PM2.5. Secondary compounds（SIA and secondary organic carbon） accounted for half of TMC（about 49.8%） in PM2.5,and suggested that secondary aerosols significantly contributed to the serious particulate matter pollution observed in winter. Coal burning,biomass combustion,vehicle emissions and SIA were found to be the main sources of PM2.5. Mass concentrations of water-soluble ions and undetected materials,as well as their fractions in TMC,strikingly increased with deteriorating particle pollution conditions,while OM and EC（elemental carbon） exhibited different variations,with mass concentrations slightly increasing but fractions in TMC decreasing.

Physicochemical and toxicological characteristics of nanoparticles in aerosols in southern Thailand during recent haze episodes in lower southeast Asia

Transboundary haze from biomass burning is one of the most important air pollutions in Southeast Asia.The most recent serious haze episode occurred in 2015.Southern Thailand was affected by the haze during September to October when the particulate matter concentration hit a record high.We investigated physical and chemical characteristics of aerosols,including concentration and aerosol size distribution down to sub-micron sizes during haze episodes in 2013 and 2015 and,for reference,an insignificant haze period in 2017.The highest total suspended particulates and PM 10 levels in Hat Yai city were 340.1 and 322.5μg/m^3.The mass fractions were nanoparticles(<100 nm)3.1%-14.8%and fine particles(<1μm)54.6%-59.1%.Polycyclic aromatic hydrocarbon size distributions in haze periods peaked at 0.75μm and the concentrations are 2-30 times higher than the normal period.High molecular weight(4-6 ring)PAHs during the haze episode contribute to about 56.7%-88.0%for nanoparticles.The average values of benzo(a)pyrene toxic equivalency quotient were 3.34±2.54ng/m^3 in the 2015 haze period but only 0.89±0.17 ng/m^3 in 2017.It is clear that particles smaller than 1μm,were highly toxic.Nanoparticles contributed 19.4%-26.0%of total BaP-TEQ,whereas the mass fraction is 13.1%-14.8%.Thus the nanoparticles were more carcinogenic and can cause greater health effect than larger particles.The fraction of BaP-TEQ for nanoparticles during 2017 non-haze period was nearly the same,while the mass fraction was lower.This indicates that nanoparticles are the significant source of carcinogenic aerosols both during haze and non-haze periods.

Characteristics of the water-soluble components of aerosol particles in Hefei,China

Size-classified daily aerosol mass concentrations and concentrations of water-soluble inorganic ions were measured in Hefei,China,in four representative months between September 2012 and August 2013.An annual average mass concentration of 169.09μg/m^3 for total suspended particulate（TSP）was measured using an Andersen Mark-II cascade impactor.The seasonal average mass concentration was highest in winter（234.73μg/m^3）and lowest in summer（91.71μg/m^3）.Water-soluble ions accounted for 59.49%,32.90%,48.62%and 37.08%of the aerosol mass concentration in winter,spring,summer,and fall,respectively,which indicated that ionic species were the primary constituents of the atmospheric aerosols.The four most abundant ions were NO3^-,SO4^2-,Ca^2＋ and NH4^＋.With the exception of Ca^2＋,the mass concentrations of water-soluble ions were in an intermediate range compared with the levels for other Chinese cities.Sulfate,nitrate,and ammonium were the dominant fine-particle species,which were bimodally distributed in spring,summer and fall;however,the size distribution became unimodal in winter,with a peak at 1.1–2.1μm.The Ca^2＋ peak occurred at approximately 4.7–5.8μm in all seasons.The cation to anion ratio was close to 1.4,which suggested that the aerosol particles were alkalescent in Hefei.The average NO3^-/SO4^2-mass ratio was 1.10 in Hefei,which indicated that mobile source emissions were predominant.Significant positive correlation coefficients between the concentrations of NH4^＋ and SO4^2-,NH4^＋ and NO3^-,SO4^2-and NO3^-,and Mg^2＋ and Ca^2＋ were also indicated,suggesting that aerosol particles may be present as（NH4）2SO4,NH4HSO4,and NH4NO3.

Comparison of four scanning mobility particle sizers at the Fresno Supersite

Size distributions of ambient aerosols at the Fresno Supersite were measured with four commercially available scanning mobility particle sizers （SMPS）. TSI nano, TSI standard, Grimm, and MSP instruments were collocated at the Fresno Supersite and particle size distributions were measured continuously from August 18 through September 18, 2005. For particles with diameters between 10 and 200 nm, differences among hourly-average ambient particle concentrations ranged from 0% between the TSI nano and Grimm in the 30-50 nm size range to 39% between the Grimm and MSP in the 10-30 nm size range. MSP concentrations were 10-33% lower than those measured with the TSI standard for particles smaller than 200 nm. The TSI nano and TSI standard agreed to within 5% in their overlapping size range （10-84 nm）. The TSI nano and Grimm agreed to within 40% for 5-10 nm particles.

Haze insights and mitigation in China: An overview

The present article provides an overview of the chemical and physical features of haze in China, focusing on the relationship between haze and atmospheric fine particles, and the formation mechanism of haze. It also summarizes several of control technologies and strategies to mitigate the occurrence of haze. The development of instruments and the analysis of measurements of ambient particles and precursor concentrations have provided important information about haze formation. Indeed, the use of new instruments has greatly facilitated current haze research in China. Examples of insightful results include the relationship between fine particles and haze, the chemical compositions and sources of particles, the impacts of the aging process on haze formation, and the application of technologies that control the formation of haze. Based on these results, two relevant issues need to be addressed： understanding the relationship between haze and fine particles and understanding how to control PM2.5.

Macro-and Micro-Structures of Heavy Fogs and Visibility in the Dayaoshan Expressway

Belonging to the southern subtropical moist type of monsoon climate, the Nanling mountainous area experiences heavy fogs whenever quasi-stationary fronts appear there from September to May. There can be as many as 15-18 days of heavy fogs per month. Fogs have more serious consequences in the Lechang-Ruyuan section of the Beijing-Zhuhai Expressway （the longest expressway in China） that passes through the main part of the Nanling Mts., where the road rises from 200 m to more than 800 m above sea level （ASL）. For a major motorway in the mountainous areas of Nanling Mts., two multidisciplinary integrated field observations were carried out, which measured visibility by the naked eyes, visibility by instrument, spectrum of fogdrops, liquid water content （LWC） of fog, tethered sounding, dual-parameter low-level sounding, turbulence diffusion within fog layers, aerosol spectra of size and composition, sampled fog water compositions, and sampled rainwater compositions. Typical cases were probed for their analyses of synoptics, micro- and macro-structures and microphysics. It is understood that heavy fogs take place with high frequency in the area and bring about serious consequences. Being typical advection and upslope fogs, they are in essence low-lying clouds appearing at high altitudes, which are closely related with the activity of South China frontal processes, especially the South China quasi-stationary fronts, and reflect on the role of local terrain as well. The heavy fogs are characteristic of long duration, extremely low visibility, well-organized lumpshaped structure, large-size fog-drops, moderate concentration, high LWC, and stronger turbulent diffusion within the fog layers than in fine sky. They differ much from radiation fogs, which are better documented in previous study in China. It is found that fog LWC is in significant anti-correlation with visibility so that large LWC is associated with small visual range. It is also noted that one of the reasons for the fluctuation of characteristic quantities of micro-structure such as the LWC of fog in the area is, in addition to the inhomogeneous structure of the fog itself, the effect of advection and inhomogeneous underlying surface; during the translation of fog with the ambient wind, irregular upslope and cross-over movement is another reason for the inhomogeneous structure and fluctuation of fog. The spectrum of the aerosol size displays itself as the power function of monotonous descent. The concentration of submicrometer particles is even higher. The high-concentration sulfate particles found in the aerosols of Nanling Mts. are actually good nuclei for condensation, which are favorable for the formation of fog. The presence of fog can help cleanse the trace compositions in the atmosphere so that fog droplets contain high levels of polluting elements. In the meantime, compared to cloud droplets, fog droplets are easier to be captured by the vertical surfaces of objects on the land surface, such as vegetation and buildings to constitute another kind of cleansing process. In vast stretches of forest like the Nanling Mts., this kind of cleansing may be quite important. Studying the characteristic variation of fogs in the area realistically assists in setting up a forecast and warning system for local fogs and provides basic information for fog dispersal experiments.