Aerosol climatology for the planetary boundary layer derived from regular lidar measurements

Regular aerosol extinction and backscatter measurements using a UV Raman Lidar have been performed for almost 3 years in Hamburg in the frame of the German Lidar Network. A set of 92 aerosol extinction and 164 aerosol backscatter profiles has been used for statistical investigations. Mean values and variances of the aerosol extinction and backscatter in the boundary layer have been calculated. Large fluctuations during the whole year have been found. The measured aerosol extinction over Hamburg shows a seasonal cycle with highest values in early fall and a second less prominent peak in spring.An analysis of the data using back trajectories showed a dependence of the aerosol extinction on the origin of the air mass. The residence time of the air mass over industrialized areas was found to be an important parameter for the measured aerosol extinction at Hamburg. However, only a small part of the total variability could be explained by the air mass origin.For 75 cases of aerosol extinction measurements under cloud-free conditions, the aerosol backscatter profile and therefore, the lidar ratio as a function of altitude could be determined. Winter measurements of the lidar ratio are often close to model results for maritime aerosol, the summer measurements are close to the model results for urban or continental aerosols.The high quality of the data has been proven by intercomparisons with other lidar systems and with star photometer measurements of the aerosol optical depth during the Lindenberg Aerosol Characterization Experiment (LACE'98) field campaign.     

Intercomparison of NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>, SO<Subscript>2</Subscript>, O<Subscript>3</Subscript>, and aromatic hydrocarbons measured by a commercial DOAS system and traditional point monitoring techniques

A field-based intercomparison study of a(DOAS) instrument (OPSIS AB, Sweden) andcommercial Differential Optical Absorption Spectroscopydifferent point-sample monitoring techniques (PM, basedon an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted inBeijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2,03, benzene, and toluene were monitored continuously during the four months. A good agreement betweenthe DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene,and NO obtained by DOAS were significantly lower than those measured by the point monitors. Theozone levels monitored by the DOAS were generally higher than those measured by point monitors. Theseresults may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics atthe measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer ofthe DOAS system, the error in the DOAS analysis can also not be excluded.     

Intercomparison of NO_x, SO_2, O_3, and Aromatic Hydrocarbons Measured by a Commercial DOAS System and Traditional Point Monitoring Techniques

A field-based Intercomparison study of a commercial Differential Optical Absorption Spectroscopy (DOAS) instrument (OPSIS AB, Sweden) and different point-sample monitoring techniques (PM, based on an air monitoring station, an air monitoring vehicle, and various chemical methods) was conducted in Beijing from October 1999 to January 2000. The mixing ratios of six trace gases including NO, NO2, SO2, O3, benzene, and toluene were monitored continuously during the four months. A good agreement between the DOAS and PM data was found for NO2 and SO2. However, the concentrations of benzene, toluene, and NO obtained by DOAS were significantly lower than those measured by the point monitors. The ozone levels monitored by the DOAS were generally higher than those measured by point monitors. These results may be attributed to a strong vertical gradient of the NO-O3-NO2 system and of the aromatics at the measurement site. Since the exact data evaluation algorithm is not revealed by the manufacturer of the DOAS sys     

南京北郊 O3、NO2和 SO2变化特征分析

利用 2008年1-12月南京北郊O₃、NO₂及SO₂质量浓度连续观测资料,分析了南京北郊气体污染物(O₃、NO₂、SO₂) 的质量浓度变化规律。结果表明：南京北郊O₃浓度夏季较高,日变化曲线呈单峰型,NO₂和SO₂浓度夏季较低,日变化曲线呈双峰型,NO₂与O₃的日变化呈现负相关关系,该地区SO₂浓度整体较高,夏季周末效应NO₂和SO₂较O₃更明显。     

Intercomparison of Tropospheric OH Measurements by Different Laser Techniques during the POPCORN Campaign 1994

In-situ OH measurements by laser-induced fluorescence (LIF) spectroscopy and folded long-path differential optical absorption spectroscopy (DOAS) were carried out in a rural environment in North-East Germany as part of the field experiment POPCORN in August 1994. The large set of OH data obtained allowed an intercomparison of both techniques based on relative diurnal profiles and simultaneously measured absolute concentrations. Most of the time the two OH instruments encountered the same air and agreed well in the measured relative diurnal variations. Only on a few occasions the measurements significantly disagreed due to a perturbation of the DOAS measurements by a local OH source in the north-western wind sector. Excluding data from this wind direction, the statistical analysis of 137 data pairs yields a correlation coefficient of r = 0.90 and a weighted linear fit with a slope of 1.09 ± 0.12. The correlations are carefully analyzed. The comparison of both instruments is discussed in the light of newly published effective absorption cross-sections for H2O and O2 that affect the calibration of LIF.     

OH-initiated degradation of several hydrocarbons in the atmosphere simulation chamber SAPHIR

Degradation of isoprene, m-xylene, n-octane, propene, and methacrolein by hydroxyl radicals has been studied in the simulation chamber SAPHIR under burden of trace gases as they are typical for the moderately polluted planetary boundary layer. Measured time series of the hydrocarbon mixing ratios and the OH concentrations were used to determine the rate constants. The hydrocarbons were measured with gas chromatography and proton transfer reaction mass spectrometry. OH was measured with the Jülich DOAS (differential optical absorption spectroscopy) instrument. In all cases except methacrolein good agreement was found with the reference rate constants taken from the Master Chemical Mechanism (MCM3.1). The data for methacrolein are consistent with the results of Karl et al. (J. Atmos. Chem 55, 2006, doi:) who reported a 12% smaller value. The degradation of hydrocarbons provides an independent method to analyse precision and accuracy of the OH measurements. A precision of better than 4% over a period of nearly 4 months was found. The accuracy is within the limitations given by the light absorption cross section of OH. Both results are consistent with earlier results by Hausmann et al. (J. Geophys. Res. 102:16011–16022, 1997).     

Nephelometer derived and directly measured aerosol optical depth of the atmospheric boundary layer

The aerosol optical depth of the atmospheric boundary layer was determined both from direct solar irradiance measurements and from vertical extrapolation of ground-based nephelometry, during a period with cloudless skies and high aerosol mass loadings in the Netherlands. The vertical profile of the aerosol was obtained from lidar measurements. From humidity controlled nephelometry at the ground and humidity profiles from soundings, the scattering aerosol extinction as a function of height was assessed. Integration of the extinction over the aerosol layer gave the aerosol optical depth of the atmospheric boundary layer. This optical depth at the narrow band of the nephelometer was translated to a spectrally integrated value, assuming an Angstrom wavelength exponent of 1.5, a typical value for The Netherlands.It was found that scattering by the boundary layer aerosol contributed on average 80% to the total atmospheric aerosol optical depth. The uncertainty in this value is estimated to be of the order of 13%. Ammonium nitrate dominated the light scattering. This is an anthropogenic aerosol component.The radiative forcing caused by the light scattering of the anthropogenic aerosol was calculated assuming an upward scattered fraction of 0.3. An average value of − 12 W m ⁻² was found (with an estimated uncertainty of 20%). This corresponds to an absolute increase in the planetary albedo of 0.03, which is equivalent to a 15% increase in the local planetary albedo of 0.2.     

成都夏季气溶胶消光特性研究

本文利用成都2017年6~8月的米散射微脉冲激光雷达观测数据,对成都夏季气溶胶消光系数、边界层高度以及气溶胶光学厚度进行了反演,并结合太阳光度计观测资料、地面颗粒物浓度以及大气能见度数据研究了气溶胶消光系数日变化与月变化规律,气溶胶消光系数的垂直分布特征及影响因素。结果表明:气溶胶消光系数的日变化受人类活动以及边界层日变化影响显著,表现出凌晨与傍晚最大,早晨次之,午后最小的特征。消光高值出现在200m以下和300~700m的高度区间,夜间观察到的消光高值可能与颗粒物在夜间近地面浓度较高以及本地夜间降水频发有关。激光雷达反演的消光系数与光度计反演的气溶胶光学厚度在夏季各月的表现一致,夏季各月消光极值均出现在100~150m的近地面层。近地面消光系数与地面颗粒物浓度之间具有较好的正相关,并且粒子粒径更小时相关性更好。气溶胶光学厚度主要来自低层大气的贡献,0.1~0.2μm的细粒子气溶胶占比对于大气消光有主要影响,但气溶胶对大气的消光影响除了与粒子浓度有关,还与粒子的理化性质有关。      

Intercomparison of Two Hydroxyl Radical Measurement Techniques at the Atmosphere Simulation Chamber SAPHIR

At the atmosphere simulation chamber SAPHIR in Jülich both Laser-Induced Fluorescence Spectroscopy (LIF) and Long-Path Differential Optical Laser Absorption Spectroscopy (DOAS) are operational for the detection of OH radicals at tropospheric levels. The two different spectroscopic techniques were compared within the controlled environment of SAPHIR based on all simultaneous measurements acquired in 2003 (13 days). Hydroxyl radicals were scavenged by added CO during four of these days in order to experimentally check the calculated precisions at the detection limit. LIF measurements have a higher precision (σ= 0.88×10⁶ cm^–3) and better time resolution (Δt = 60 s), but the DOAS method (σ= 1.24×10⁶ cm^–3, Δt = 135 s) is regarded as primary standard for comparisons because of its good accuracy. A high correlation coefficient of r = 0.95 was found for the whole data set highlighting the advantage of using a simulation chamber. The data set consists of two groups. The first one includes 3 days, where the LIF measurements yield (1 – 2) ×10⁶ cm^–3 higher OH concentrations than observed by the DOAS instrument. The experimental conditions during these days are characterized by increased NO_x concentration and a small dynamic range in OH. Excellent agreement is found within the other group of 6 days. The regression to the combined data of this large group yields unity slope without a significant offset.     

A New Method for Aerosol Retrieval Based on Lidar Observations in Beijing

Lidar has been used extensively in the area of atmospheric aerosol measurement. Two unknowns at the reference altitude, the lidar ratio and the backscatter coefficient, need to be resolved from the lidar equation. In the actual application, these two values are difficult to obtain, particularly the backscatter coefficient. To better characterize the optical properties of aerosols, optical thickness, and attenuated backscatter obtained by other instruments are usually used as the input for joint inversion. However, this method is limited by location and time. In this study, the authors propose a new method for aerosol retrieval by using Mie scatter- ing lidar data to solve this problem. The authors take the horizontal aerosol extinction coefficient as the con- straint to begin the iteration until a self-consistent aerosol vertical profile was obtained. By comparing their results with Aerosol Robotic Network （AERONET） data, the authours determine that the aerosol extinction coefficient obtained by combining horizontal and vertical lidar observations is more pre- cise than that obtained by using the traditional Fernald method. This new method has been adopted for re- trieving the extinction coefficient of aerosols during the observation days.     

SBDART辐射传输模式及其在飞机潜在积冰区反演中的应用

SBDART(平面平行辐射传输模式)是近年来国际上比较流行的一种计算辐射传输的模式，该模式旨在解决在卫星遥感和大气辐射能量平衡研究中遇到的各种辐射传输问题。它是基于大量经过仔细筛选的物理模式而建立起来的辐射传输模式，并且在实践中发展完善。文章详细介绍了SBDART模式的功能和结构，并利用SBDART模式结合卫星资料反演出云的光学厚度、有效粒子半径及消光系数，实现了对飞机积冰区域的有效识别。     

Effect of particle shape on dust shortwave direct radiative forcing calculations based on MODIS observations for a case study

Assuming spheroidal and spherical particle shapes for mineral dust aerosols, the effect of particle shape on dust aerosol optical depth retrievals, and subsequently on instantaneous shortwave direct radiative forcing (SWDRF) at the top of the atmosphere (TOA), is assessed based on Moderate Resolution Imaging Spectroradiometer (MODIS) data for a case study. Specifically, a simplified aerosol retrieval algorithm based on the principle of the Deep Blue aerosol retrieval method is employed to retrieve dust aerosol optical depths, and the Fu-Liou radiative transfer model is used to derive the instantaneous SWDRF of dust at the TOA for cloud-free conditions. Without considering the effect of particle shape on dust aerosol optical depth retrievals, the effect of particle shape on the scattering properties of dust aerosols (e.g., extinction efficiency, single scattering albedo and asymmetry factor) is negligible, which can lead to a relative difference of at most 5% for the SWDRF at the TOA. However, the effect of particle shape on the SWDRF cannot be neglected provided that the effect of particle shape on dust aerosol optical depth retrievals is also taken into account for SWDRF calculations. The corresponding results in an instantaneous case study show that the relative differences of the SWDRF at the TOA between spheroids and spheres depend critically on the scattering angles at which dust aerosol optical depths are retrieved, and can be up to 40% for low dust-loading conditions.     

Ground‐based lidar measurements of aerosols during ACE‐2: instrument description, results, and comparisons with other ground‐based and airborne measurements

A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr⁻¹. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.     

Vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai

A comparative study on the vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai was conducted based on the data obtained from a micro pulse lidar.There was a distinct difference in layer thickness and extinction coefficient under the two types of weather conditions.Aerosols were concentrated below 1 km and the aerosol extinction coefficients ranged from 0.25 to 1.50km^-1 on haze days.In contrast,aerosols with smaller extinction coefficients(0.20 0.35 km^-1) accumulated mainly from the surface to 2 km on floating dust days.The seasonal variations of extinction and aerosol optical depth（AOD） for both haze and floating dust cases were similar greatest in winter,smaller in spring,and smallest in autumn.More than 85%of the aerosols appeared in the atmosphere below 1 km during severe haze and floating dust weather.The diurnal variation of the extinction coefficient of haze exhibited a bimodal shape with two peaks in the morning or at noon,and at nightfall,respectively.The aerosol extinction coefficient gradually increased throughout the day during floating dust weather.Case studies showed that haze aerosols were generated from the surface and then lifted up,but floating dust aerosols were transported vertically from higher altitude to the surface.The AOD during floating dust weather was higher than that during haze.The boundary layer was more stable during haze than during floating dust weather.     

Measurements of Nighttime Nitrate Radical Concentrations in the Atmosphere by Long-Path Differential Optical Absorption Spectroscopy

The long-path differential optical absorption spectroscopy(LP-DOAS)technique was developed to mea- sure nighttime atmospheric nitrate radical(NO_3)concentrations.An optimized retrieval method,resulting in a small residual structure and low detection limits,was developed to retrieve NO_3.The time series of the NO_3 concentration were collected from 17 to 24 March,2006,where a nighttime average value of 15.8 ppt was observed.The interfering factors and errors are also discussed.These results indicate that the DOAS technique provides an essential tool for the quantification of NO_3 concentration and in the study of its effects upon nighttime chemistry.     

宽带消光法反演气溶胶光学厚度与AERONET北京站探测结果的对比研究

该文简要介绍了遥感气溶胶光学厚度的宽带消光法, 重点比较与分析了2001～2002年间北京地区宽带消光法和全球气溶胶探测网(AERONET)气溶胶光学厚度的探测结果.对比结果表明, 两类探测结果在无云晴天的条件下具有很好的吻合, 二者的相关系数达到90%以上.另外, 作者还针对宽带消光法反演月平均气溶胶光学厚度问题, 提出了一个减小云对反演结果影响的方法, 即月平均光学厚度约束法, 并与全球气溶胶探测网探测结果做对比分析.二者结果的一致性表明该约束方法的有效性.     

Aerosol properties and air pollutants over an urban area

For a better understanding of urban aerosols, sun/sky photometry has been undertaken at the Kinki University campus in Higashi-Osaka as a NASA/AERONET station since 2002. A new instrument, the SPM-613D (Kimoto Electric), has been taking measurements at the same site since March 15, 2004. The relationship between aerosol properties obtained from radiometry with AERONET and the SPM measurements is examined. It is found that there is a linear correlation between SPM concentrations and aerosol properties, which indicates that aerosol characteristics can be estimated from SPM data, and vice versa.It is also shown that the air quality of the Higashi-Osaka site is poor due to not only the anthropogenic particles by local emissions, such as diesel vehicles and chemical industries, but also due to the dust particles coming from continental desert areas by large scale climatic conditions.     

地基曙暮光光谱观测反演平流层O3和NO2柱含量

用差分光学吸收光谱(DOAS)方法,从曙暮光天顶散射可见光光谱资料反演了北京上空的O3和NO2柱含量,并对反演结果进行了验证和误差分析.斜柱含量的反演采用了线性和非线性最小二乘拟合方法,拟合时考虑了O3、NO2和H2O的吸收、Ring效应和散射的影响;斜柱含量除以空气质量因子转换成垂直柱含量.空气质量因子的计算使用伪球面DISORT辐射传输模式.O3和NO2总量的检验分别用北京的Dobson O3资料和卫星SAGE Ⅱ的NO2廓线资料.反演的O3总量与Dobson O3总量相比偏差小于10%;NO2总量与SAGE Ⅱ的偏差约20%.     

Aerosol properties and air pollutants over an urban area

For a better understanding of urban aerosols, sun/sky photometry has been undertaken at the Kinki University campus in Higashi-Osaka as a NASA/AERONET station since 2002. A new instrument, the SPM-613D (Kimoto Electric), has been taking measurements at the same site since March 15, 2004. The relationship between aerosol properties obtained from radiometry with AERONET and the SPM measurements is examined. It is found that there is a linear correlation between SPM concentrations and aerosol properties, which indicates that aerosol characteristics can be estimated from SPM data, and vice versa.It is also shown that the air quality of the Higashi-Osaka site is poor due to not only the anthropogenic particles by local emissions, such as diesel vehicles and chemical industries, but also due to the dust particles coming from continental desert areas by large scale climatic conditions.     

Optical growth of highly viscous organic/sulfate particles

Light extinction by atmospheric particles is strongly dependent on their chemical composition and water content. Since light extinction directly impacts climate, optical measurements of atmospherically relevant aerosols at varying relative humidities (RH) are needed. Recent studies have highlighted the possibility that some atmospheric aerosols are glassy under ambient conditions. Here, the particle optical growth factor, fRH_ext, was measured for liquid and glassy particles using cavity ring-down aerosol extinction spectroscopy. The particles were composed of ammonium sulfate (AS), 1,2,6-hexanetriol, sucrose, raffinose, and mixed particles containing AS and either sucrose or raffinose. Both sucrose and raffinose can be glassy at room temperature. For the pure organics, the highly viscous sucrose and raffinose particles have similar optical growth curves to the liquid 1,2,6 hexanetriol particles. However, for particles composed of sucrose or raffinose mixed with AS, optical growth depends on the AS weight-percent, which in turn controls the phase state of the AS and ultimately the water uptake.