The Significant Contribution of Small-Sized and Spherical Aerosol Particles to the Decreasing Trend in Total Aerosol Optical Depth over Land from 2003 to 2018

The optical and microphysical properties of aerosols remain one of the greatest uncertainties associated with evaluating the climate forcing attributed to aerosols.Although the trends in aerosol optical depth(AOD)at global and regional scales have been widely examined,little attention has been paid to the trends in type-dependent AODs related to aerosol particle properties.Here,using the aerosol optical component dataset from the Multi-angle Imaging SpectroRadiometer(MISR)instrument,we investigate decadal-scale trends in total aerosol loading as well as AODs for five aerosol components by particle size and morphology during 2003–2018 over land.Relationships between the total AOD(TAOD)trends and type-dependent AOD changes were examined,and the relative contribution of each type-dependent AOD to the overall TAOD trends was quantified.By dividing the TAOD values into four different aerosol pollution levels(APLs)with splits at 0.15,0.40,and 0.80,we further explored the relationships between TAOD changes and interannual variations in the frequency-of-occurrences(FoOs)of these APLs.Long-term trends in FoOs in the different APLs show that there was a significant improvement in air quality between 2003 and 2018 in most land areas,except South Asia,corresponding to a shift from lightly polluted to clean conditions.However,the effects of different APLs on TAOD changes are regionally dependent and their extent of correlation varied spatially.Moreover,we observed that the annual mean TAOD has decreased by 0.47%.a^(-1)over land since 2003(P<0.05).This significant reduction was mainly attributed to the continued reduction in small-sized(<0.7 mm diameter)AOD(SAOD)(-0.74%.a^(-1))and spherical AOD(SPAOD)(-0.46%.a^(-1)).Statistical analysis shows that SAOD and SPAOD respectively accounted for 57.5%and 89.6%of the TAOD,but contributed 82.6%and 90.4%of the trend in TAOD.Our study suggests that small-sized and spherical aerosols composed of sulfate,organic matter,and black carbon play a dominant role in determining interannual variability in land TAOD.

Atmospheric Particle Hygroscopicity and the Influence by Oxidation State of Organic Aerosols in Urban Beijing

A hygroscopic tandem differentialmobility analyser(H-TDMA)was used to observe the sizeresolved hygroscopic characteristics of submicron particles in January and April 2018 in urban Beijing.The probability distribution of the hygroscopic growth factor(HGF-PDF)in winter and spring usually showed a bimodal pattern,with more hygroscopic mode(MH)being more dominant.The seasonal variation in particle hygroscopicity was related to the origin of air mass,which received polluted southerly air masses in spring and clean northwesterly air masses in winter.Particles showed stronger hygroscopic behaviour during heavy pollution episodes(HPEs)with elevated concentrations of secondary aerosols,especially higher mass fraction of nitrate,which were indicated using the PM2.5(particulate matter with diameter below 2.5μm)mass concentration normalised by CO mass concentration.The hygroscopic parameter(κ)values were calculated using H-TDMA(κhtdma)and chemical composition(κchem).The closure study showed thatκchem was overestimated in winter afternoon when compared withκhtdma,because the organic particle hygroscopic parameter(κorg)was overestimated in the calculations.It was influenced by the presence of a high concentration of hydrocarbon-like organic aerosol(HOA)with a weak water uptake ability.A positive relationship was observed betweenκorg and the ratio of oxygenated organic aerosol(OOA)and HOA,thereby indicating that the strong oxidation state enhanced the hygroscopicity of the particles.This study revealed the effect of local emission sources and secondary aerosol formation processes on particle hygroscopicity,which is of great significance for understanding the pollution formation mechanism in the North China Plain.

大气CO_(2)观测支持核校我国2018~2021年人为碳排放与陆地碳交换

准确估算人为碳排放和自然碳交换对我国实现碳中和目标至关重要.当前自下而上的排放清单在区域尺度上存在不确定性,且缺乏大气观测的独立验证.本文利用我国39个高精度CO_(2)地基观测站,自上而下反演获得45 km×45 km分辨率的人为碳排放与自然碳交换,实现了对排放清单的核校支持.结果表明,2018~2021年反演获得的我国年均人为碳排放总量约为125亿吨CO_(2),高于自下而上的五套排放清单约15%.扣除人和动物呼吸排放后,2018~2021年我国年均人为碳排放约为115亿吨CO_(2).从逐年变化看,2021年我国人为二氧化碳排放总量较前一年增加4%,高于2020年同比增速(1.1%),略高于2019年同比年增速(3.7%),与我国观测到的大气中的CO_(2)年增量趋势一致.扣除农田碳汇、非CO_(2)碳排放、水蚀及火点排放后,2018-2021年我国年均陆地生态系统碳汇约为21亿吨CO_(2),高于大多数全球反演模式,占同期人为碳排放约17%.陆地生态系统自然碳交换受气候变化年际波动影响较大,其中2019年受弱厄尔尼诺事件影响,碳汇同比降幅最大,2020年碳汇有所增加,2021年同比2020年增加13.7%.自上而下反演给出了大气观测视角下CO_(2)源汇时空变化,并重点突出了不同省份在实现碳中和目标时面临的挑战.

Modeling study on the roles of the deposition and transport of PM_(2.5) in air quality changes over central-eastern China

The role of PM_(2.5)(particles with aerodynamic diameters≤_(2.5)μm)deposition in air quality changes over China remains unclear.By using the three-year(2013,2015,and 2017)simulation results of the WRF/CUACE v1.0 model from a previous work(Zhang et al.,2021),a non-linear relationship between the deposition of PM_(2.5)and anthropogenic emissions over central-eastern China in cold seasons as well as in different life stages of haze events was unraveled.PM_(2.5)deposition is spatially distributed differently from PM_(2.5)concentrations and anthropogenic emissions over China.The North China Plain(NCP)is typically characterized by higher anthropogenic emissions compared to southern China,such as the middlelow reaches of Yangtze River(MLYR),which includes parts of the Yangtze River Delta and the Midwest.However,PM_(2.5)deposition in the NCP is significantly lower than that in the MLYR region,suggesting that in addition to meteorology and emissions,lower deposition is another important factor in the increase in haze levels.Regional transport of pollution in central-eastern China acts as a moderator of pollution levels in different regions,for example by bringing pollution from the NCP to the MLYR region in cold seasons.It was found that in typical haze events the deposition flux of PM_(2.5)during the removal stages is substantially higher than that in accumulation stages,with most of the PM_(2.5)being transported southward and deposited to the MLYR and Sichuan Basin region,corresponding to a latitude range of about 24°N-31°N.

Construction and Application of a Regional Kilometer-Scale Carbon Source and Sink Assimilation Inversion System(CCMVS-R)

CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.

Relative Contributions of Boundary-Layer Meteorological Factors to the Explosive Growth of PM2.5 during the Red-Alert Heavy Pollution Episodes in Beijing in December 2016

Based on observations of urban mass concentration of fine particulate matter smaller than 2.5 μm in diameter(PM_(2.5)), ground meteorological data, vertical measurements of winds, temperature, and relative humidity(RH), and ECMWF reanalysis data, the major changes in the vertical structures of meteorological factors in the boundary layer(BL) during the heavy aerosol pollution episodes(HPEs) that occurred in winter 2016 in the urban Beijing area were analyzed. The HPEs are divided into two stages: the transport of pollutants under prevailing southerly winds, known as the transport stage(TS), and the PM_(2.5) explosive growth and pollution accumulation period characterized by a temperature inversion with low winds and high RH in the lower BL, known as the cumulative stage(CS). During the TS, a surface high lies south of Beijing, and pollutants are transported northwards. During the CS, a stable BL forms and is characterized by weak winds, temperature inversion, and moisture accumulation. Stable atmospheric stratification featured with light/calm winds and accumulated moisture(RH > 80%) below 250 m at the beginning of the CS is closely associated with the inversion, which is strengthened by the considerable decrease in near-surface air temperature due to the interaction between aerosols and radiation after the aerosol pollution occurs. A significant increase in the PLAM(Parameter Linking Aerosol Pollution and Meteorological Elements) index is found, which is linearly related to PM mass change. During the first 10 h of the CS, the more stable BL contributes approximately 84% of the explosive growth of PM_(2.5) mass. Additional accumulated near-surface moisture caused by the ground temperature decrease, weak turbulent diffusion, low BL height, and inhibited vertical mixing of water vapor is conducive to the secondary aerosol formation through chemical reactions, including liquid phase and heterogeneous reactions, which further increases the PM_(2.5) concentration levels. The contribution of these reaction mechanisms to the explosive growth of PM_(2.5) mass during the early CS and subsequent pollution accumulation requires further investigation.

The impact of meteorological changes from 2013 to 2017 on PM2.5 mass reduction in key regions in China

In 2013,China issued the"Action Plan for the Prevention and Control of Air Pollution"("Ten Statements of Atmosphere")and implemented a series of pollution reduction measures from 2013 to 2017.In key regions of China,the mass concentrations of particulate matter with aerodynamic equivalent diameters less than 2.5μm(PM2.5)have dropped significantly.However,the contributions of meteorological changes to PM2.5 reduction are largely uncertain,which has attracted particular concern from the government and the public.Here,we investigated the impact of large-scale and boundary layer(BL)meteorological conditions on aerosol pollution and estimated the contributions of meteorological changes to PM2.5 reduction based on in-depth analysis and diagnosis of various observed meteorological elements and an integrated pollution-linked meteorological index(PLAM,which is approximately and linearly related to PM mass concentration).In this study,we found that the meteorological conditions worsened in 2014 and 2015 and improved in 2016 and 2017 relative to those in 2013 in key regions in China.In 2017 relative to 2013,only^5%(approximately 13%of the total PM2.5 decline)of the 39.6%reduction in PM2.5 mass concentrations can be attributed to meteorological changes in the Beijing-Tianjin-Hebei(BTH)region,and only^7%(approximately 20%of the total PM2.5 decline)of the 34.3%reduction can be attributable to meteorological changes in the Yangtze River Delta(YRD)region.Overall,the PM2.5 reduction due to meteorological improvement is much lower than the observed PM2.5 reduction in these areas,which indicates that emission reduction during the five-year implementation of the"Ten Statements of Atmosphere"is the dominant factor in the improvement in air quality.The changes in meteorology and climate are conducive to PM2.5 reduction but do not dominate the substantial improvement in air quality.Similar to the above regions,in the Pearl River Delta(PRD)region,the impact of meteorological changes on the annual averaged PM2.5 concentration from 2013 to2017 was relatively weak,and the PM2.5 reduction was mainly due to emission reductions.During winter 2017(January,February,and December of this year),the meteorological conditions improved-20%in the BTH region(observed total PM2.5reduction:40.2%)and-30%in the YRD region(observed total PM2.5 reduction:38.2%)relative to those in 2013,showing the meteorological factors played more important role in the decrease of PM2.5 in winter of these years in the two regions,respectively.The meteorological conditions in winter 2016 were 14%better than those in winter 2017,but the PM2.5 reduction in winter 2016 was still less than that in winter 2017,reinforcing the significant contributions of the increasing efforts to reduce PM2.5 emissions in 2017.The substantial progress of strict emission measures was also confirmed by a comparison of several persistent heavy aerosol pollution episodes(HPEs)with similar meteorological conditions.It is found that the decrease of PM2.5mass caused by emission reduction increases year by year,especially the decrease of PM2.5 concentration in 2016 and 2017.In China,HPEs mainly occur in winter,when meteorological conditions are approximately 40-100%worse than in other seasons.This worsening is partly due to the harbor effect of high topography,including downdrafts and the weak wind zone,and partly due to the increasingly stable regional BL structure caused by climate warming.For the formation of HPEs,it occurred under regional stagnant and stable conditions associated with upper-level circulation patterns,including the zonal westerly winds type and high-pressure ridges.After pollution formation,PM2.5 with mass accumulated to a certain degree can further worsen the BL meteorological conditions.The feedback effect associated with worsening conditions dominates PM2.5 mass explosive growth.In the context of high air pollutant emissions in China,unfavorable meteorological conditions are the necessary external conditions for the formation and accumulation of HPEs.Therefore,reducing aerosol pollution significantly during the earlier transport stage is critical in reducing persistent HPEs.Currently,even under favorable meteorological conditions,allowing emissions without restriction is also not advisable because aerosol pollution allowed to accumulate to a certain extent will significantly worsen the BL meteorological conditions and close the"meteorological channels"available for pollution dispersion.

Aerosol Hygroscopicity during the Haze Red-Alert Period in December 2016 at a Rural Site of the North China Plain

A humidification system was deployed to measure aerosol hygroscopicity at a rural site of the North China Plain during the haze red-alert period 17–22 December 2016. The aerosol scattering coefficients under dry [relative humidity(RH) < 30%] and wet(RH in the range of 40%–85%) conditions were simultaneously measured at wavelengths of450, 550, and 700 nm. It is found that the aerosol scattering coefficient and backscattering coefficient increased by only 29% and 10%, respectively when RH went up from 40% to 80%, while the hemispheric backscatter fraction went down by 14%, implying that the aerosol hygroscopicity represented by the aerosol scattering enhancement factor f(RH) is relatively low and RH exerted little effects on the aerosol light scattering in this case. The scattering enhancement factors do not show significant differences at the three wavelengths, only with an approximate 2% variation, suggesting that the aerosol hygroscopicity is independent of the wavelength. Aerosol hygroscopicity is highly dependent on the aerosol chemical composition. When there is a large mass fraction of inorganics and a small mass fraction of organic matter, f(RH) reaches a high value. The fraction of NO_3^- was strongly correlated with the aerosol scattering coefficient at RH = 80%, which suggests that NO_3^- played an important role in aerosol hygroscopic growth during the heavy pollution period.

Intensified wintertime secondary inorganic aerosol formation during heavy haze pollution episodes(HPEs) in Beijing,China

Air pollution in China is complex,and the formation mechanism of chemical components in particulate matter is still unclear.This study selected three consecutive heavy haze pollution episodes(HPEs)during winter in Beijing for continuous field observation,including an episode with heavy air pollution under red alert.Clean days during the observation period were selected for comparison.The HPE characteristics of Beijing in winter were:under the influence of adverse meteorological conditions such as high relative humidity,temperature inversion and low wind speed;and strengthening of secondary transformation reactions,which further intensified the accumulation of secondary aerosols and other pollutants,promoting the explosive growth of PM_(2.5).PM_(2.5)/CO values,as indicators of the contribution of secondary transformation in PM_(2.5),were approximately 2 times higher in the HPEs than the average PM_(2.5)/CO during the clean period.The secondary inorganic aerosols(sulfate nitrate and ammonium salt)were significantly enhanced during the HPEs,and the conversion coefficients were remarkably improved.In addition,it is interesting to observe that the production of sulfate tended to exceed that of nitrate in the late stage of all three HPEs.The existence of aqueous phase reactions led to the explosive growth sulfur oxidation ratio(SOR)and rapid generation of sulfate under high relative humidity(RH>70%).

Comparison of Submicron Particles at a Rural and an Urban Site in the North China Plain during the December 2016 Heavy Pollution Episodes

An extensive field experiment for measurement of physical and chemical properties of aerosols was conducted at an urban site in the Chinese Academy of Meteorological Sciences(CAMS) in Beijing and at a rural site in Gucheng(GC), Hebei Province in December 2016. This paper compares the number size distribution of submicron particle matter(PM1, diameter < 1 μm) between the two sites. The results show that the mean PM1 number concentration at GC was twice that at CAMS, and the mass concentration was three times the amount at CAMS. It is found that the accumulation mode(100–850 nm) particles constituted the largest fraction of PM1 at GC, which was significantly correlated with the local coal combustion, as confirmed by a significant relationship between the accumulation mode and the absorption coefficient of soot particles. The high PM1 concentration at GC prevented the occurrence of new particle formation(NPF) events, while eight such events were observed at CAMS. During the NPF events, the mass fraction of sulfate increased significantly, indicating that sulfate played an important role in NPF. The contribution of regional transport to PM1 mass concentration was approximately 50% at both sites, same as that of the local emission. However, during the red-alert period when emission control took place, the contribution of regional transport was notably higher.

2022汤加火山灰羽流的气溶胶光学、微物理和辐射特性

作为21世纪乃至近30年最强的火山喷发之一,2022年汤加火山喷发事件已经引起了广泛关注.研究表明,汤加火山喷发所产生的大量火山灰气溶胶突破对流层进入平流层,形成了一个顶部高度约为25~30 km的火山灰羽流.在喷发后的4天内,火山灰羽流在平流层环流的驱动下迅速向西移动了近10000 km.侵入平流层的火山灰气溶胶导致整个澳大利亚北部的大气气溶胶负荷显著增加,气溶胶光学厚度(AOD)在澳大利亚东北部海岸达到1.5,约为侵入前一日的15倍.此次汤加火山灰羽流主要以半径集中在~0.26μm处的细模态颗粒物为主,同时其体积峰值达到0.25μm^(3)μm^(-2).汤加火山喷发对平流层AOD和辐射平衡的影响显著,卫星观测到的平流层AOD的扰动高达0.6.这种扰动在很大程度上解释了区域性地表(大气层顶)的瞬时短波辐射强迫可达-105.0 W m^(-2)(-65.0 W m^(-2)).