Refractory black carbon aerosols in rainwater in the summer of 2019 in Beijing:Mass concentration,size distribution and wet scavenging ratio

Black carbon(BC)aerosols in the atmosphere play a significant role in climate systems due to their strong ability to absorb solar radiation.The lifetime of BC depends on atmospheric transport,aging and consequently on wet scavenging processes(in-cloud and below-cloud scavenging).In this study,sequential rainwater samples in eight rainfall events collected in 2 mm interval were measured by a tandem system including a single particle soot photometer(SP2)and a nebulizer.The results showed that the volume-weighted average(VWA)mass concentrations of refractory black carbon(rBC)in each rainfall event varied,ranging from 10.8 to 78.9μg/L.The highest rBC concentrations in the rainwater samples typically occurred in the first fraction from individual rainfall events.The geometric mean median mass-equivalent diameter(MMD)decreased under precipitation,indicating that rBC with larger sizes was relatively aged and preferentially removed by wet scavenging.A positive correlation(R2=0.73)between the VWA mass concentrations of rBC in rainwater and that in ambient air suggested the important contribution of scavenging process.Additionally,the contributions of in-cloud and below-cloud scavenging were distinguished and accounted for 74%and 26%to wet scavenging,respectively.The scavenging ratio of rBC particles was estimated to be 0.06 on average.This study provides helpful information for better understanding the mechanism of rBC wet scavenging and reducing the uncertainty of numerical simulations of the climate effects of rBC.

影响我国霾天气的多尺度过程

频发的霾天气是我国现阶段面临的最主要大气环境问题之一.霾期间高浓度大气细颗粒物(PM2.5)是多种物理化学过程综合影响的结果,包括排放、气-粒转化、大气边界层、局地环流、天气与气候等过程.上述过程的时空尺度跨越了几个数量级,在空间尺度上涵盖了纳米尺度至上千千米尺度.多尺度过程本身的复杂性以及不同过程之间的相互影响是目前大气环境领域面临的最严峻挑战,直接影响到对于霾天气形成机制的科学认识、预报技术与数值模式研发,以及相应的大气污染治理.文章综述了在影响我国霾天气的多尺度过程及其与气溶胶的相互作用领域取得的研究进展.研究表明:二次气溶胶已经成为我国大气气溶胶的主要部分,在霾过程后期,液相非均相过程对气-粒转化有重要贡献;PM2.5呈现多时间尺度周期性振荡,包括1,4~7以及40~60 d等,边界层、天气和气候等多尺度过程是造成上述周期性变化的主因;已有证据表明,我国高气溶胶已经影响到该区域大气光化学、大气边界层,甚至天气和气候过程.气溶胶与上述过程的相互作用进一步影响了气溶胶浓度及其空间分布,但是此问题极为复杂,尚存在很大不确定性.为此,今后需重点加强以下研究:加强包含气溶胶理化性质、大气光化学、气象要素在内的多要素协同观测,重点开展对流层内多要素协同垂直探测;增强跨学科领域研究,尤其是大气物理-大气化学-天气/气候等多学科间的交叉性研究;加强气溶胶与大气化学、边界层、天气气候等过程相互作用的数值模拟研究.

Evolution of planetary boundary layer under different weather conditions,and its impact on aerosol concentrations

A field experiment was conducted in Tianjin, China from September 9-30, 2010, focused on the evolution of Planetary Boundary Layer （PBL） and its impact on surface air pollutants. The experiment used three remote sensing instruments, wind profile radar （WPR）, microwave radiometer （MWR） and micro-pulse lidar （MPL）, to detect the vertical profiles of winds, temperature, and aerosol backscattering coefficient and to measure the vertical profiles of surface pollutants （aerosol, CO, SO2, NOx）, and also collected sonic anemometers data from a 255-m meteorological tower. Based on these measurements, the evolution of the PBL was estimated. The averaged PBL height was about 1000-1300 m during noon/afternoon-time, and 200-300 m during night-time. The PBL height and the aerosol concentrations were anti-correlated during clear and haze conditions. The averaged maximum PBL heights were 1.08 and 1.70 km while the averaged aerosol concentrations were 52 and 17 μg/m＆3 under haze and clear sky conditions, respectively, The influence of aerosols and clouds on solar radiation was observed based on sonic anemometers data collected from the 255-m meteorological tower. The heat flux was found significantly decreased by haze （heavy pollution） or cloud, which tended to depress the development of PBL, while the repressed structure of PBL further weakened the diffusion of pollutants, leading to heavy pollution. This possible positive feedback cycle （more aerosols→lower PBL height → more aerosols） would induce an acceleration process for heavy ground pollution in megacities.

Research Progress on Estimation of the Atmospheric Boundary Layer Height

Atmospheric boundary layer height(ABLH)is an important parameter used to depict characteristics of the planetary boundary layer(PBL)in the lower troposphere.The ABLH is strongly associated with the vertical distributions of heat,mass,and energy in the PBL,and it is a key quantity in numerical simulation of the PBL and plays an essential role in atmospheric environmental assessment.In this paper,various definitions and methods for deriving and estimating the ABLH are summarized,from the perspectives of turbulent motion,PBL dynamics and thermodynamics,and distributions of various substances in the PBL.Different methods for determining the ABLH by means of direct observation and remote sensing retrieval are reviewed,and comparisons of the advantages and disadvantages of these methods are presented.The paper also summarizes the ABLH parameterization schemes,discusses current problems in the estimation of ABLH,and finally points out the directions for possible future breakthroughs in the ABLHrelated research and application.

Variability of SO_2 in an intensive fog in North China Plain:Evidence of high solubility of SO_2

A field experiment was conducted in an intensive fog event between November 5 and November 8, 2009, in a heavily SO2-polluted area in North China Plain （NCP）, to measure SO2 and other air pollutants, liquid water content （LWC） of fog droplets, and other basic meteorological parameters. During the fog period, the concentrations of SO2 showed large variability, which was closely related to the LWC in the fog droplets. The averaged concentration of SO2 during non-fog periods was about 25 ppbv, while during the fog period, it rapidly reduced to about 4-7 ppbv. Such large reduction of SO2 suggested that a majority of SO2 （about 70%-80%） had reverted from gas to aqueous phase on account of the high solubility of SO2 in water in the fog droplets. However, the calculated gas to aqueous phase conversion was largely underestimated by merely using the Henry＇s Law constant of SO2, thus suggesting that aqueous reaction of SO2 in fog droplets might play some important role in enhancing the solubility of SO2. To simplify the phenomenon, an ＂effective solubility coefficient＂ is proposed in this study. This variability of SO2 measurement during the extensive fog event provides direct evidence of oxidation of SO2 in fog droplets, thus providing important implications for better understanding of the acidity in clouds, precipitation, and fogs in NCP, now a central environmental focus in China due to its rapid economic development.

Ground-high altitude joint detection of ozone and nitrogen oxides in urban areas of Beijing

Based on observational data of ozone （O3） and nitrogen oxide （NOx） mixing ratios on the ground and at high altitude in urban areas of Beijing during a period of six days in November 2011, the temporal and spatial characteristics of mixing ratios were analyzed. The major findings include： urban O3 mixing ratios are low and NOx mixing ratios are always high near the road in November. Vertical variations of the gases are significantly different in and above the planetary boundary layer. The mixing ratio of O3 is negatively correlated with that of NOx and they are positively correlated with air temperature, which is the main factor directly causing vertical variation of O3 and NOx mixing ratios at 600-2100 m altitude. The NOx mixing ratios elevated during the heating period, while the O3 mixing ratios decreased： these phenomena are more significant at high altitudes compared to lower altitudes. During November, air masses in the urban areas of Beijing are brought by northwesterly winds, which transport O3 and NOx at low mixing ratios. Due to Beijing＇s natural geographical location, northwest air currents arc beneficial to the dilution and dispersion of pollutants, which can result in lower O3 and NOx background values in the Beijing urban area.

Assessing the Influence of Aerosol on Radiation and Its Roles in Planetary Boundary Layer Development

A comprehensive measurement of planetary boundary layer(PBL)meteorology was conducted at 140 and 280 m on a meteorological tower in Beijing,China,to quantify the effect of aerosols on radiation and its role in PBL development.The measured variables included four-component radiation,temperature,sensible heat flux(SH),and turbulent kinetic energy(TKE)at 140 and 280 m,as well as PBL height(PBLH).In this work,a method was developed to quantitatively estimate the effect of aerosols on radiation based on the PBLH and radiation at the two heights(140 and 280 m).The results confirmed that the weakened downward shortwave radiation(DSR)on hazy days could be attributed predominantly to increased aerosols,while for longwave radiation,aerosols only accounted for around onethird of the enhanced downward longwave radiation.The DSR decreased by 55.2 W m^(-2) on hazy days during noontime(1100–1400 local time).The weakened solar radiation decreased SH and TKE by enhancing atmospheric stability,and hence suppressed PBL development.Compared with clean days,the decreasing rates of DSR,SH,TKE,and PBLH were 11.4%,33.6%,73.8%,and 53.4%,respectively.These observations collectively suggest that aerosol radiative forcing on the PBL is exaggerated by a complex chain of interactions among thermodynamic,dynamic,and radiative processes.These findings shed new light on our understanding of the complex relationship between aerosol and the PBL.