Effect of instrumental particle sizing resolution on the modelling of aerosol radiative parameters

A more realistic estimation of the scattering and hemispheric backscattering coefficients, σ_sp and σ_bsp, and their respective optical cross section, C_sca and C_bk, of aerosol particles is presented on the basis of the exact resolution of the width of the size bins of the particle counter instruments when size distribution measurements are used, and, with the exact optical detector instruments ability. The scattering and hemispheric backscattering cross sections, C_sca and C_bk, of the particles are averaged over the full size bins of the particle counter instrument, while these quantities are usually estimated only on the value of the mean geometric diameter of each size bin. Six instruments, the APS, ASASP-X, DMPS, FSSP-100, ELPI, and SMPS frequently used in particle size distribution measurements are reviewed, for spherical sea-salt particles at a wavelength λ=0.55 μm. The comparison using the conventional geometric mean diameter versus the use of the full size bin leads to large amount of errors for the optical cross section with non-negligible effects on their respective optical coefficients. The maximal accuracy expected for these optical quantities depend on the particle diameter as well as on the channel width of the instruments, and are also function of the angular detector probe used to measure them.     

Nucleation of atmospheric aerosol particles

A significant fraction of the total number of particles present in the atmosphere is formed originally by nucleation from the gas phase. Binary nucleation of sulphuric acid and water, ternary nucleation of sulphuric acid, water and ammonia and ion-induced nucleation are thought to be the most important aerosol nucleation processes in the atmosphere. Within the last two decades, instrumentation to observe and characterize nucleation has improved greatly and numerous observations of nucleation have been made including quantification of the nucleation rate, characterization of the growth process and first chemical characterizations of the freshly formed particles. Nucleation has been observed at many different places in the atmosphere: in the boundary layer, in the free troposphere, in remote locations, in coastal areas, in boreal forests as well as urban areas and pollution plumes. In most cases gaseous sulphuric acid is assumed to be the key precursor gas. After nucleation, other supersaturated substances, especially low vapour pressure organics often take part in the subsequent aerosol growth. Iodine oxides seem to be responsible for nucleation observed in some coastal areas.Recent advances in modelling allow for a kinetic treatment of the nucleation process based on measured thermochemical data for the cluster formation. Considerable improvement over the classical nucleation treatment is expected from this approach.A detailed understanding of atmospheric aerosol nucleation processes is needed as the freshly formed particles directly influence the number concentration and size distribution of the atmospheric aerosol. The formation of clouds and precipitation is affected and influences on climate are anticipated. Anthropogenic emissions influence atmospheric aerosol nucleation processes considerably.Despite the comprehensive research efforts, substantial inconsistencies remain and conflicting results of laboratory studies, model studies as well as atmospheric observations persist. Several key questions about the predictability of atmospheric nucleation in general, about the substances, that take part in nucleation and subsequent growth and about the size and composition of the critical cluster, have not been resolved so far. To cite this article: J. Curtius, C. R. Physique 7 (2006).     

双扫描激光雷达精细探测低层大气气溶胶方法

为实现水平非均匀分布的低层大气气溶胶光学特性的遥感探测,提出一种基于双扫描激光雷达的气溶胶精细探测方法.该方法以扫描激光雷达为遥感探测工具,通过双激光雷达相向交叉扫描工作模式,实现对同一空域近地表气溶胶全视野剖面的交叉探测,从而提供双激光雷达方程组以精确求解气溶胶消光和后向散射系数.在数据反演过程中,通过对交叉扫描区域进行坐标化和网格化处理、网格像素单元的初值预设,以及双扫描激光雷达方程组的数值逼近反演得到气溶胶消光.利用长距离扫描激光雷达的数据对该方法进行验证,结果表明,该方法与多角度方法反演所得到的结果随高度变化的趋势具有高度的一致性;同时双扫描激光雷达可提供交叉扫描区域剖面的气溶胶浓度分布,相比于单条廓线具有较大的优势.     

Aerosol source (biomass,traffic and coal emission) apportionment in Lithuania using stable carbon and radiocarbon analysis*

In the present study, a combination of the stable carbon isotope ratio (¹³C/¹²C) with radiocarbon data (¹⁴C) allowed us to perform the aerosol source apportionment. Filter samples of PM₁ were collected during the warm and cold periods in rural and urban sites in Lithuania. The ¹⁴C/¹²C ratio of total carbon (TC) was measured using the single stage accelerator mass spectrometer quantifying of fossil and non-fossil derived aerosol emissions. The δ¹³C value was measured using an elemental analyser interfaced with an isotope ratio mass spectrometer. We have found that the highest fraction of contemporary carbon (f_c?=?0.82) was measured during a warm period in a rural location. A higher fraction of fossil fuel-derived carbon was observed for air masses transported from highly industrialized Western European regions during both seasons. Isotope mass balance calculations revealed that the traffic emissions composed 15 and 25?% in rural and urban sites, respectively, and did not change during either season. Input from coal-derived aerosol particles was estimated to be 15?% at an urban site during the cold period. The combination of the stable carbon isotope ratio with the radiocarbon data allowed us to distinguish coal, liquid fossil fuel combustion, and non-fossil derived aerosol particle emissions.     

Micro-droplet Trapping and Manipulation: Understanding Aerosol Better for a Healthier Environment

Understanding the physicochemical properties and heterogeneous processes of aerosols is key not only to elucidate the impacts of aerosols on the atmosphere and humans but also to exploit their further applications, especially for a healthier environment. Experiments that allow for spatially control of single aerosol particles and investigations on the fundamental properties and heterogeneous chemistry at the single-particle level have flourished during the last few decades, and significant breakthroughs in recent years promise better control and novel applications aimed at resolving key issues in aerosol science. Here we propose graphene oxide (GO) aerosols as prototype aerosols containing polycyclic aromatic hydrocarbons, and GO can behave as two-dimensional surfactants which could modify the interfacial properties of aerosols. We describe the techniques of trapping single particles and furthermore the current status of the optical spectroscopy and chemistry of GO. The current applications of these single-particle trapping techniques are summarized and interesting future applications of GO aerosols are discussed.     

Analysis of additive metals in fuel and emission aerosols of diesel vehicles with and without particle traps

Fuel additives used in particle traps have to comply with environmental directives and should not support the formation of additional toxic substances. The emission of metal additives from diesel engines with downstream particle traps has been studied. Aspects of the optimisation of sampling procedure, sample preparation and analysis are described. Exemplary results in form of a mass balance calculation are presented. The results demonstrate the high retention rate of the studied filter system but also possible deposition of additive metals in the engine.     

The agglomeration state of nanosecond laser-generated aerosol particles entering the ICP

Fundamental understanding of aerosol formation and particle transport are important aspects of understanding and improving laser-ablation ICP–MS. To obtain more information about particles entering the ICP, laser aerosols generated under different ablation conditions were collected on membrane filters. The particles and agglomerates were then visualised using scanning electron microscope (SEM) imaging. To determine variations between different sample matrices, opaque (USGS BCR-2G) and transparent (NIST SRM 610) glass, CaF₂, and brass (MBH B26) samples were ablated using two different laser wavelengths, 193 and 266 nm. This study showed that the condensed nano-particles (∼10 nm in diameter) formed by laser ablation reach the ICP as micron-sized agglomerates; this is apparent from filters which contain only a few well-separated particles and particle agglomerates. Ablation experiments on different metals and non-metals show that the structure of the agglomerates is matrix-dependent. Laser aerosols generated from silicates and metals form linear agglomerates whereas particle-agglomerates of ablated CaF₂ have cotton-like structures. Amongst other conditions, this study shows that the absorption characteristics of the sample and the laser wavelength determine the production of micron-sized spherical particles formed by liquid droplet ejection.     

Portable,Ambient PM2.5 Sensor for Human and/or Animal Exposure Studies

A field-portable device for logging PM_2.5 mass concentration data has been developed. The device combines the Arduino microprocessor with an SD card, a Sharp DN7C3CA006 optical dust monitor, and 10,000-mAh battery. The dust sensor uses a virtual impactor to size select particles <2.5 microns prior to illuminating the selected fraction with an LED. The LED is triggered by a circuit controlled with the Arduino. Nephelometric detection at 120° referenced to incidence is used. The voltage signal reported by the dust sensor is converted to PM_2.5 mass through calibration onboard the Arduino. Data points can be saved to the SD card as rapidly as 0.3?s, although averaging signals over 60?s produced more optimal detection limits. For a 60?s average, the PM_2.5 mass limit of detection was 9?µg?m^?3, indicating that the sensor will be useful for monitoring human exposure to fine particles. Portable exposure monitoring has been demonstrated with the sensing platform as several individuals carried the device with them during daily activities in Lubbock, TX and Atlanta, GA. For this group of test subjects, values of PM_2.5 exposure varied from 0 to 1000?µg?m^?3 during the sampling periods. It was observed that, by far, the highest levels of PM_2.5 occur during periods of cooking, or being near cooking operations. Other periods of high PM_2.5 occurred during ground transportation, use of personal care products, vacuuming, and visiting restrooms. When hourly personal exposure data were correlated with hourly average PM_2.5 for outdoor air for the Atlanta data set, a very weak correlation was found (R²?=?0.026). Only two out of eight sampling periods did the personal monitoring estimate of exposure agree with that predicted by outdoor monitoring to within 15%. Personal exposure was often affected by circumstantial, short-term, high exposure events that are difficult to model or predict effectively. The short-term exposure events generally cause true exposure to be higher than that predicted by using outdoor ambient PM_2.5 to generate estimates. This finding complicates interpretation of epidemiological studies that find links between ambient outdoor PM_2.5 levels and human health, while it buttresses the case for using personal ambient monitors.     

Possible effects of climate change of wind on aerosol variation during winter in Shanghai,China

Several data sets were introduced to investigate the possible effects of climate-change-related variation of wind on aerosol concentration during winter in Shanghai, China. These data sets included the daily wind speed, wind direction, visibility, and precipitation from 1956 to 2010, hourly PM₁₀ concentration from 2008 to 2010, and the NCEP/NCAR reanalysis data of global atmospheric circulation from 1956 to 2010. The trend of aerosol concentration and its correlations with wind speed and wind direction in winter were analyzed. Results indicated that there was an increase in the number of haze days in winter of 2.1 days/decade. Aerosol concentration, represented by PM₁₀ in this study, was highly correlated to both wind speed and direction in winter. The PM₁₀ concentration increased as wind speed decreased, reaching maximum values under static wind conditions. The PM₁₀ concentration was relatively lower under easterly winds and higher under westerly winds. The analysis showed that weaker East Asia winter monsoons have resulted in a reduction of wind speed, increase in static wind frequency, and decline in the frequency of northerly winds since the 1980s. Moreover, the rapid expansion of urban construction in Shanghai has changed the underlying surface considerably, which has led to a reduction in wind speed. Finally, a wind factor was defined to estimate the combined effects of wind speed and wind direction on aerosol concentrations in Shanghai. The analysis of this factor indicated that changes in atmosphere circulation and urbanization have had important effects on the number of winter haze days in Shanghai.     

Aerosol optical properties and its direct radiative forcing over Tibetan Plateau from 2006 to 2017

Studies on optical properties of aerosols can reduce the uncertainty for modelling direct radiative forcing (DRF) and improve the accuracy for discussing aerosols effects on the Tibetan Plateau (TP) climate. This study investigated the spatiotemporal variation of aerosol optical and microphysical properties over TP based on OMI and MERRA2, and assessed the influence of aerosol optical properties on DRF at NamCo station (30°46.44′N, 90°59.31′E, 4730 m) in the central TP from 2006 to 2017 based on a long measurement of AERONET and the modelling of SBDART model. The results show that aerosol optical depth (AOD) exhibits obvious seasonal variation over TP, with higher AOD_500nm (>0.75) during spring and summer, and lower value (<0.25) in autumn and winter. The aerosol concentrations show a fluctuated rising from 1980 to 2000, significant increasing from 2000 to 2010 and slight declining trend after 2013. Based on sensitivity experiments, it is found that AOD and single scattering albedo (SSA) have more important impact on the DRF compared with α values and ASY. When AOD_440nm increases by 60%, DRF at the TOA and ATM is increased by 57.2% and 60.2%, respectively. When SSA_440nm increases by 20%, DRF at the TOA and ATM decreases by 121% and 96.7%, respectively.