Aerosol Species Research Articles

Distribution and source identification of nitrogen and phosphorus in aerosols in the Qinhuangdao coast, north China

Abstract Nitrogen and phosphorus in aerosols is an important source of nutrients in the coastal waters. To study all forms of composition and potential source of nitrogen and phosphorus in atmospheric particulates in the coastal waters of Qinhuangdao, 135 atmospheric aerosol samples were collected from August 2015 to August 2016. The result showed that the nitrogen in aerosols in the Qinhuangdao coastal area was more soluble (accounting for 91.7%), while phosphorus was more insoluble (62.3%). The same seasonal variation of nitrogen and phosphorus components was discovered, with the highest concentration in winter and the lowest in summer. Frequent dust and haze weather processes have a significant impact on the nitrogen and phosphorus species in aerosols. The concentrations of soluble nitrogen and phosphorus increased more significantly in haze days, while insoluble nitrogen and phosphorus increased more significantly in dust days. Both weather processes may aggravate the phosphorus limitation in the coastal waters of Qinhuangdao. Quantitative analysis of potential sources area indicated that Beijing–Tianjin–Hebei, Mongolia, Inner Mongolia contributed the most to the atmospheric nitrogen and phosphorus in Qinhuangdao coastal area. The total contribution of these three regions to atmospheric nitrogen and phosphorus pollution of Qinhuangdao were about 70%, which indicated that most of the atmospheric nitrogen and phosphorus in Qinhuangdao offshore come from the atmospheric pollutant transport channel in the northwest.

Photo-oxidation of particle phase iron species dominates the generation of reactive oxygen species in secondary aerosol

This study presents an experimental investigation on the photochemical transformation of iron species in aerosol including dissolution of insoluble iron species into soluble fraction, and soluble ferric oxidation to ferrous form. This process has significantly contributed to the aerosol oxidative potential in generation of reactive oxygen species (ROS). We conducted both laboratory experiment of UV irradiation and real world solar irradiation on large variation of aerosol samples for the characterization of iron speciation in insoluble and soluble fractions to investigate their transformation under photooxidation process. The results showed that the real world solar irradiation significantly increased the soluble Fe(II) fraction, and this is corroborated by laboratory simulation of UV irradiation showing increasing soluble Fe(II) fraction with elongating aging time. The results further exhibited that the dissolution of iron component into soluble fraction was a dominant process, followed by the conversion of soluble ferric to ferrous ions. Further, the study confirmed that the oxidative potential of particulate matter (PM) is attributed dominantly to the abundance of transition metals, i.e. Fe, and the incremental ROS generation after photochemical process is attributed largely to the transformation of solid phase iron species to soluble Fe(II). The results suggest that transition metals, for example by iron in this study, play an important role in secondary aerosol process.

The spatially heterogeneous response of aerosol properties to anthropogenic activities and meteorology changes in China during 1980–2018 based on the singular value decomposition method

The unsustainable and rapid economy development brings air pollution prominently in China. In the last decade, the haze weather and its influencing mechanism across China have received increasingly attention. Although previous research has extensively focused on the characteristics of aerosols, better understanding of long-term variation in aerosols and their determinants since the Reform and Opening-up still lack in China. Furthermore, the previous studies exploring the influencing mechanism behind haze episodes by using statistical method only reflect correlation between pollutant concentration and indicators at single station, which cannot consider the remote influences resulting from atmosphere transport. In this research, we investigated the spatiotemporal pattern of aerosol optical depth (AOD) and aerosol species in China during 1980–2018 and explored the spatially heterogeneous response of AOD and aerosol component to meteorological conditions and urbanization based on singular value decomposition (SVD) method. The results indicated that AOD exhibited an upward trend in nearly 40 years, especially in eastern China with the fastest growth of sulfate aerosol. The heterogeneity of determinants revealed a great gap in anthropogenic activities and meteorological influences on aerosol varing regions. In eastern China, anthropogenic activities should be closely monitored. Besides, scientific desert governance and urban construction exert positive impact on air pollution in Xinjiang province.

Compositional Characteristics of Atmospheric Aerosols during a Consecutive High Concentration Episode in Seoul, Korea

This study focuses on the temporal variation in the compositional characteristics of atmospheric aerosols in Seoul, South Korea, during the consecutive high aerosol concentration episode from 30 December 2013 to 2 January 2014. The temporal variations in the observed physical, optical, and chemical properties show that there were three distinct episodes during the period: haze, mixed haze/Asian dust, and Asian dust episodes. For the haze period, the concentration of secondary inorganic aerosols increased and both secondary inorganic aerosols and calcium species exhibited simultaneously high concentrations during the mixed haze/Asian dust period. The neutralization factors by ammonia in the haze periods were higher as 1.03 than the other periods, meanwhile the neutralization contribution by calcium carbonate was relatively higher as 1.39 during the Asian dust episode. The backward trajectory analysis showed that concentrations of SO42−, NO3−, and NH4+ were relatively high when air masses moved over East China. Principal component analysis showed that water-soluble components originated from soil dust/incineration, secondary aerosols/biomass burning, and road dust from the haze aerosol. For the mixed haze/Asian dust episode, the major source of aerosols was estimated to have originated from soil dust, pollutants from fossil fuel combustion, biomass burning, and sea-salt emissions. Furthermore, the main sources of ionic species in the Asian dust aerosols were estimated to be sea-salt/soil dust, secondary aerosols/coal combustion, and road dust.

Long-term sub-micrometer aerosol chemical composition in the boreal forest: inter- and intra-annual variability

Abstract. The Station for Measuring Ecosystem–Atmosphere Relations (SMEAR) II is well known among atmospheric scientists due to the immense amount of observational data it provides of the Earth–atmosphere interface. Moreover, SMEAR II plays an important role for the large European research infrastructure, enabling the large scientific community to tackle climate- and air-pollution-related questions, utilizing the high-quality long-term data sets recorded at the site. So far, this well-documented site was missing the description of the seasonal variation in aerosol chemical composition, which helps understanding the complex biogeochemical and physical processes governing the forest ecosystem. Here, we report the sub-micrometer aerosol chemical composition and its variability, employing data measured between 2012 and 2018 using an Aerosol Chemical Speciation Monitor (ACSM). We observed a bimodal seasonal trend in the sub-micrometer aerosol concentration culminating in February (2.7, 1.6, and 5.1 µg m−3 for the median, 25th, and 75th percentiles, respectively) and July (4.2, 2.2, and 5.7 µg m−3 for the median, 25th, and 75th percentiles, respectively). The wintertime maximum was linked to an enhanced presence of inorganic aerosol species (ca. 50 %), whereas the summertime maximum (ca. 80 % organics) was linked to biogenic secondary organic aerosol (SOA) formation. During the exceptionally hot months of July of 2014 and 2018, the organic aerosol concentrations were up to 70 % higher than the 7-year July mean. The projected increase in heat wave frequency over Finland will most likely influence the loading and chemical composition of aerosol particles in the future. Our findings suggest strong influence of meteorological conditions such as radiation, ambient temperature, and wind speed and direction on aerosol chemical composition. To our understanding, this is the longest time series reported describing the aerosol chemical composition measured online in the boreal region, but the continuous monitoring will also be maintained in the future.

Organosulfates in Ambient Aerosol: State of Knowledge and Future Research Directions on Formation, Abundance, Fate, and Importance.

Organosulfates (OSs), also referred to as organic sulfate esters, are well-known and ubiquitous constituents of atmospheric aerosol particles. Commonly, they are assumed to form upon mixing of air masses of biogenic and anthropogenic origin, that is, through multiphase reactions between organic compounds and acidic sulfate particles. However, in contrast to this simplified picture, recent studies suggest that OSs may also originate from purely anthropogenic precursors or even directly from biomass and fossil fuel burning. Moreover, besides classical OS formation pathways, several alternative routes have been discovered, suggesting that OS formation possibly occurs through a wider variety of formation mechanisms in the atmosphere than initially expected. During the past decade, OSs have reached a constantly growing attention within the atmospheric science community with evermore studies reporting on large numbers of OS species in ambient aerosol. Nonetheless, estimates on OS concentrations and implications on atmospheric physicochemical processes are still connected to large uncertainties, calling for combined field, laboratory, and modeling studies. In this Critical Review, we summarize the current state of knowledge in atmospheric OS research, discuss unresolved questions, and outline future research needs, also in view of reductions of anthropogenic sulfur dioxide (SO2) emissions. Particularly, we focus on (1) field measurements of OSs and measurement techniques, (2) formation pathways of OSs and their atmospheric relevance, (3) transformation, reactivity, and fate of OSs in atmospheric particles, and (4) modeling efforts of OS formation and their global abundance.

Chemical Differences Between PM1 and PM2.5 in Highly Polluted Environment and Implications in Air Pollution Studies

AbstractSubmicron aerosol (PM1) species measured by aerosol mass spectrometers have been widely used to validate chemical transport models; however, the uncertainties due to chemical differences between PM1 and PM2.5 are poorly constrained. Here we characterized such differences in a highly polluted environment in north China in winter. Our results showed that the changes in PM1/PM2.5 ratios as a function of relative humidity (RH) were largely different for primary and secondary species. Secondary organic and inorganic aerosol (SOA and SIA) presented clear decreases in PM1/PM2.5 ratios at RH > 60% during periods with high SIA contributions (>50%), likely driven by the changes in aerosol hygroscopicity and phase states, while the traffic and coal combustion OA had limited dependence on RH. Thermodynamic modeling showed negligible impacts of PM differences on predictions of particle acidity, yet these impacts can cause a difference in aerosol water content by up to 50–70%.

An aerosol climatology for global models based on the tropospheric aerosol scheme in the Integrated Forecasting System of ECMWF

Abstract. An aerosol climatology to represent aerosols in the radiation schemes of global atmospheric models was recently developed. We derived the climatology from a reanalysis of atmospheric composition produced by the Copernicus Atmosphere Monitoring Service (CAMS). As an example of an application in a global atmospheric model, we discuss the technical aspects of the implementation in the European Centre for Medium Range Weather Forecasts Integrated Forecasting System (ECMWF-IFS) and the impact of the new climatology on the medium-range weather forecasts and 1-year simulations. The new aerosol climatology was derived by combining a set of model simulations with constrained meteorological conditions and an atmospheric composition reanalysis for the period 2003–2013 produced by the IFS. The aerosol fields of the reanalysis are constrained by assimilating the aerosol optical thickness (AOT) retrievals product by the Moderate Resolution Imaging Spectroradiometer (MODIS) instruments. In a further step, we used modelled aerosol fields to correct the aerosol speciation and the vertical profiles of the aerosol reanalysis fields. The new climatology provides the monthly-mean mass mixing ratio of five aerosol species constrained by assimilated MODIS AOT. Using the new climatology in the ECMWF-IFS leads to changes in the direct aerosol radiative effect compared to the climatology previously implemented, which have a small but non-impact on the forecast skill of large-scale weather patterns in the medium-range. However, details of the regional distribution of aerosol radiative forcing can have a large local impact. This is the case for the area of the Arabian Peninsula and the northern Indian Ocean. Here changes in the radiative forcing of the mineral dust significantly improve the summer monsoon circulation.

Evaluation of sea salt aerosols in climate systems: global climate modeling and observation-based analyses**The data that support the findings of this study are available from the corresponding author upon reasonable request.

Sea salt aerosols (SSA), one of the most abundant aerosol species over the global oceans, play important roles for Earth’s climate. State-of-the-art SSA parameterizations in global climate models (GCMs) are typically modeled using near-surface wind speed, sea surface temperature (SST), and precipitation. However, these have non-trivial biases in CMIP3 and CMIP5 GCMs over the tropical Pacific Ocean that can contribute to biases in the simulated SSA. This study investigates the impacts of falling ice radiative effects on the biases of the aforementioned modeled parameters and the resulting modeled SSA biases. We compare the CMIP5 modeled SSA against satellite observations from MISR and MODIS using a pair of sensitivity experiments with falling ice radiative effects on and off in the CESM1-CAM5 model. The results show that when falling ice radiative effects are not taken into account, models have weaker surface wind speeds, warmer SSTs, excessive precipitation, and diluted sea surface salinity (SSS) over the Pacific trade-wind regions, leading to underestimated SSA. In the tropical Pacific Ocean, the inclusion of falling ice radiative effects leads to improvements in the modeled near-surface wind speeds, SSTs, and precipitation through cloud-precipitation-radiation-circulation coupling, which results in more representative patterns of SSA and reduces the SSA biases by ∼10% to 15% relative to the satellite observations. Models including falling ice radiative effects in CMIP5 produce smaller biases in SSA than those without falling ice radiative effects. We suggest that one of the causes of these biases is likely the failure to account for falling ice radiative effects, and these biases in turn affect the direct and indirect effects of SSA in the GCMs.

Chemical composition and sources of submicron aerosols in winter at a regional site in Beijing-Tianjin-Hebei region: Implications for the Joint Action Plan

The Ministry of Environmental Protection released a Joint Action Plan for Control of Air Pollution (Hereafter, Joint Action Plan, JAP), to reduce PM2.5 concentrations in the Beijing-Tianjin-Hebei region (BTH) during the winter of 2017. To investigate the effectiveness of the controls, we deployed an aerosol chemical speciation monitor and collected filter samples at Xianghe, a representative site for the BTH, to characterize the aerosol composition during the implementation of the JAP. Those results were compared with earlier data obtained from a literature survey and reanalysis of studies in the BTH. During several pollution episodes in the control period, the major aerosol types changed relative to the earlier studies from sulfate, oxygenated organic aerosol, and coal combustion organic aerosol to nitrate and biomass burning organic aerosol. The dominant secondary inorganic aerosol species during the JAP changed from sulfate to nitrate, and the main source for primary organic aerosol switched from coal combustion to biomass burning. These changes can be explained by the fact that the JAP controls targeted coal combustion and SO2 but not biomass burning or NOx emissions. Our evaluation of the control measures provides a scientific basis for developing new policies in the future.

Near-ultraviolet Transmission Spectroscopy of HD 209458b: Evidence of Ionized Iron Beyond the Planetary Roche Lobe

Abstract The inflated transiting hot Jupiter HD 209458b is one of the best studied objects since the beginning of exoplanet characterization. Transmission observations of this system between the mid-infrared and the far-ultraviolet have revealed the signature of atomic, molecular, and possibly aerosol species in the lower atmosphere of the planet, as well as escaping hydrogen and metals in the upper atmosphere. From a re-analysis of near-ultraviolet transmission observations of HD 209458b we detect ionized iron (Fe+) absorption in a 100 Å-wide range around 2370 Å, lying beyond the planetary Roche lobe. However, we do not detect absorption of equally strong Fe+ lines expected to be around 2600 Å. Further, we find no evidence for absorption by neutral magnesium (Mg), ionized magnesium (Mg+), nor neutral iron (Fe). These results avoid the conflict with theoretical models previously found by Vidal-Madjar et al., which detected Mg but did not detect Mg+ from this same data set. Our results indicate that hydrodynamic escape is strong enough to carry atoms as heavy as iron beyond the planetary Roche lobe, even for planets less irradiated than the extreme ultra-hot Jupiters such as WASP-12 b and KELT-9 b. The detection of iron and nondetection of magnesium in the upper atmosphere of HD 209458b can be explained by a model in which the lower atmosphere forms (hence, sequesters) primarily magnesium-bearing condensates, rather than iron condensates. This is suggested by current microphysical models. The inextricable synergy between upper- and lower-atmosphere properties highlights the value of combining observations that probe both regions.

Sensitivity of Radiative Fluxes to Aerosols in the ALADIN-HIRLAM Numerical Weather Prediction System

The direct radiative effect of aerosols is taken into account in many limited-area numerical weather prediction models using wavelength-dependent aerosol optical depths of a range of aerosol species. We studied the impact of aerosol distribution and optical properties on radiative transfer, based on climatological and more realistic near real-time aerosol data. Sensitivity tests were carried out using the single-column version of the ALADIN-HIRLAM numerical weather prediction system, set up to use the HLRADIA simple broadband radiation scheme. The tests were restricted to clear-sky cases to avoid the complication of cloud–radiation–aerosol interactions. The largest differences in radiative fluxes and heating rates were found to be due to different aerosol loads. When the loads are large, the radiative fluxes and heating rates are sensitive to the aerosol inherent optical properties and the vertical distribution of the aerosol species. In such cases, regional weather models should use external real-time aerosol data for radiation parametrizations. Impacts of aerosols on shortwave radiation dominate longwave impacts. Sensitivity experiments indicated the important effects of highly absorbing black carbon aerosols and strongly scattering desert dust.

Spaceborne lidar retrieved composite and speciated aerosol extinction profiles and optical depths over India: A decade of observations

Despite several independent observational studies, a comprehensive picture on the aerosol vertical distribution and its spatial gradients has not yet evolved over the Indian subcontinent. The present study analyses around 10 years (June 2006 to December 2016) of version 3 level 3 CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) spaceborne lidar (light detection and ranging) retrieved night time, cloud free vertical extinction profiles (at 532 nm) of composite aerosol, and its major species (dust, polluted dust and smoke) to understand the three-dimensional distribution of aerosols over India. The shape and vertical extent of the extinction profiles varied in space and time. The vertical extent of the aerosol distribution is shallower in the colder seasons compared to that of warmer seasons, which could potentially be due to suppressed convection during colder months. Meridional gradients are observed in the near-surface extinction coefficients (increasing towards north of India). Polluted dust (defined as a mixture of dust and smoke) emerged as the dominant aerosol species over most parts of the study region. Over the north western and central India, dust aerosols contributed the most to the aerosol optical depths and extinction profiles during the summer and monsoon months. Smoke aerosols prevailed over the southern and north eastern parts of India, which are attributed to biomass, agricultural burning, and long-range transport. Boundary layer aerosol optical depths (AOD) contributed to columnar AOD significantly during post-monsoon and winter, while the elevated-AOD had almost an equal share in columnar AOD during the summer and monsoon seasons.

Arsenic species in electronic cigarettes: Determination and potential health risk

Human exposure to contaminants from electronic cigarettes (e-cigarettes) and the associated health effects are poorly understood. There has been no report on the speciation of arsenic in e-liquid (solution used for e-cigarettes) and aerosols. We report here determination of arsenic species in e-liquids and aerosols generated from vaping the e-liquid. Seventeen e-liquid samples of major brands, purchased from local and online stores in Canada and China, were analyzed for arsenic species using high-performance liquid chromatography and inductively coupled plasma mass spectrometry. Aerosols condensed from vaping the e-liquids were also analyzed and compared for arsenic species. Six arsenic species were detected, including inorganic arsenate (iAsV), arsenite (iAsIII), monomethylarsonic acid (MMA), and three new arsenic species not reported previously. In e-liquids, iAsIII was detected in 59%, iAsV in 94%, and MMA in 47% of the samples. In the condensate of aerosols from vaping the e-liquids, iAsIII was detected in 100%, iAsV in 88%, and MMA in 13% of the samples. Inorganic arsenic species were predominant in e-liquids and aerosols of e-cigarettes. The concentration of iAsIII in the condensate of aerosols (median 3.27 μg/kg) was significantly higher than that in the e-liquid (median 1.08 μg/kg) samples. The concentration of inorganic arsenic in the vaping air was approximately 3.4 μg/m3, which approaches to the permissible exposure limit (10 μg/m3) set by the United States Occupational Safety and Health Administration (OSHA). According to the Environmental Protection Agency's unit risk factor (4.3 × 10−3 per μg/m3) for inhalation exposure to inorganic arsenic in the air, the estimated excess lung cancer risk from lifetime exposure to inorganic arsenic in the e-cigarette vaping air (3.4 μg/m3), assuming e-cigarette vaping at 1% of the time, is as high as 1.5 × 10−4. These results raise health concerns over the exposure to arsenic from electronic cigarettes.

Mapping the drivers of uncertainty in atmospheric selenium deposition with global sensitivity analysis

Abstract. An estimated 0.5–1 billion people globally have inadequate intakes of selenium (Se), due to a lack of bioavailable Se in agricultural soils. Deposition from the atmosphere, especially through precipitation, is an important source of Se to soils. However, very little is known about the atmospheric cycling of Se. It has therefore been difficult to predict how far Se travels in the atmosphere and where it deposits. To answer these questions, we have built the first global atmospheric Se model by implementing Se chemistry in an aerosol–chemistry–climate model, SOCOL-AER (modeling tools for studies of SOlar Climate Ozone Links – aerosol). In the model, we include information from the literature about the emissions, speciation, and chemical transformation of atmospheric Se. Natural processes and anthropogenic activities emit volatile Se compounds, which oxidize quickly and partition to the particulate phase. Our model tracks the transport and deposition of Se in seven gas-phase species and 41 aerosol tracers. However, there are large uncertainties associated with many of the model's input parameters. In order to identify which model uncertainties are the most important for understanding the atmospheric Se cycle, we conducted a global sensitivity analysis with 34 input parameters related to Se chemistry, Se emissions, and the interaction of Se with aerosols. In the first bottom-up estimate of its kind, we have calculated a median global atmospheric lifetime of 4.4 d (days), ranging from 2.9 to 6.4 d (2nd–98th percentile range) given the uncertainties of the input parameters. The uncertainty in the Se lifetime is mainly driven by the uncertainty in the carbonyl selenide (OCSe) oxidation rate and the lack of tropospheric aerosol species other than sulfate aerosols in SOCOL-AER. In contrast to uncertainties in Se lifetime, the uncertainty in deposition flux maps are governed by Se emission factors, with all four Se sources (volcanic, marine biosphere, terrestrial biosphere, and anthropogenic emissions) contributing equally to the uncertainty in deposition over agricultural areas. We evaluated the simulated Se wet deposition fluxes from SOCOL-AER with a compiled database of rainwater Se measurements, since wet deposition contributes around 80 % of total Se deposition. Despite difficulties in comparing a global, coarse-resolution model with local measurements from a range of time periods, past Se wet deposition measurements are within the range of the model's 2nd–98th percentiles at 79 % of background sites. This agreement validates the application of the SOCOL-AER model to identifying regions which are at risk of low atmospheric Se inputs. In order to constrain the uncertainty in Se deposition fluxes over agricultural soils, we should prioritize field campaigns measuring Se emissions, rather than laboratory measurements of Se rate constants.

Investigating size-segregated sources of elemental composition of particulate matter in the South China Sea during the 2011 <i>Vasco</i> cruise

Abstract. The South China Sea (SCS) is a receptor of numerous natural and anthropogenic aerosol species from throughout greater Asia. A combination of several developing countries, archipelagic and peninsular terrain, a strong Asian monsoon climate, and a host of multi-scale meteorological phenomena make the SCS one of the most complex aerosol–meteorological systems in the world. However, aside from the well-known biomass burning emissions from Indonesia and Borneo, the current understanding of aerosol sources is limited, especially in remote marine environments. In September 2011, a 2-week research cruise was conducted near Palawan, Philippines, to sample the remote SCS environment. Size-segregated aerosol data were collected using a Davis Rotating Uniform size-cut Monitor (DRUM) sampler and analyzed for concentrations of 28 elements measured via X-ray fluorescence (XRF). Positive matrix factorization (PMF) was performed separately on the coarse, fine, and ultrafine size ranges to determine possible sources and their contributions to the total elemental particulate matter mass. The PMF analysis resolved six sources across the three size ranges: biomass burning, oil combustion, soil dust, a crustal–marine mixed source, sea spray, and fly ash. Additionally, size distribution plots, time series plots, back trajectories and satellite data were used in interpreting factors. The multi-technique source apportionment revealed the presence of biogenic sources such as soil dust, sea spray, and a crustal–marine mixed source. Anthropogenic sources were also identified: biomass burning, oil combustion, and fly ash. Mass size distributions showed elevated aerosol concentrations towards the end of the sampling period, which coincided with a shift of air mass back trajectories to southern Kalimantan. Covariance between coarse-mode soil dust and fine-mode biomass burning aerosols were observed. Agreement between the PMF and the linear regression analyses indicates that the PMF solution is robust. While biomass burning is indeed a key source of aerosol, this study shows the presence of other important sources in the SCS. Identifying these sources is not only key for characterizing the chemical profile of the SCS but, by improving our picture of aerosol sources in the region, also a step forward in developing our understanding of aerosol–meteorology feedbacks in this complex environment.

Dust Constraints from joint Observational-Modelling-experiMental analysis (DustCOMM): comparison with measurements and model simulations

Abstract. Mineral dust is the most abundant aerosol species by mass in the atmosphere, and it impacts global climate, biogeochemistry, and human health. Understanding these varied impacts on the Earth system requires accurate knowledge of dust abundance, size, and optical properties, and how they vary in space and time. However, current global models show substantial biases against measurements of these dust properties. For instance, recent studies suggest that atmospheric dust is substantially coarser and more aspherical than accounted for in models, leading to persistent biases in modelled impacts of dust on the Earth system. Here, we facilitate more accurate constraints on dust impacts by developing a new dataset: Dust Constraints from joint Observational-Modelling-experiMental analysis (DustCOMM). This dataset combines an ensemble of global model simulations with observational and experimental constraints on dust size distribution and shape to obtain more accurate constraints on three-dimensional (3-D) atmospheric dust properties than is possible from global model simulations alone. Specifically, we present annual and seasonal climatologies of the 3-D dust size distribution, 3-D dust mass extinction efficiency at 550 nm, and two-dimensional (2-D) atmospheric dust loading. Comparisons with independent measurements taken over several locations, heights, and seasons show that DustCOMM estimates consistently outperform conventional global model simulations. In particular, DustCOMM achieves a substantial reduction in the bias relative to measured dust size distributions in the 0.5–20 µm diameter range. Furthermore, DustCOMM reproduces measurements of dust mass extinction efficiency to almost within the experimental uncertainties, whereas global models generally overestimate the mass extinction efficiency. DustCOMM thus provides more accurate constraints on 3-D dust properties, and as such can be used to improve global models or serve as an alternative to global model simulations in constraining dust impacts on the Earth system.

Atmospheric visibility variation over global land surface during 1973–2012: Influence of meteorological factors and effect of aerosol, cloud on ABL evolution

Atmospheric visibility (Vis) is used to evaluate air pollution over global land surface during 1973–2012. Over global more populated areas with major anthropogenic emissions and hygroscopic aerosol species, weaker surface wind is generally associated with more severe air pollution and Vis degradation, while an increase of relative humidity (RH) generally favors more efficient secondary formation and hygroscopic growth of aerosol and Vis impairment. The allocation of meteorological factor with the major aerosol component over global different areas can influence the formation and variation of aerosol and cloud, and their effects on the atmospheric boundary layer (ABL) evolution and air pollution. Over East Asia, India and Southeast Asia, the air pollution with a growing concern with Vis decrease can be associated to an increase in anthropogenic emission and a synchronous stabilization of ABL (characterized by a weakened, less variable surface wind and a decreased diurnal temperature range, DTR). Both the increase of aerosol loading and cloud cover could (i) increase daily minimum air temperature versus decrease daily maximum air temperature and result in a decrease of DTR, (ii) reduce solar radiation reaching the surface, stabilize the ABL and aggravate air pollution. While Vis increase over Europe could be related to more effective emission control and an intensification of surface wind. Also significantly, a close relationship is identified between RH and DTR; RH explains about 90% of the variance of DTR over Europe in summer; a drier weather is corresponding to a greater surface incoming short-wave flux and a greater DTR.

A review of aerosol chemistry in Asia: insights from aerosol mass spectrometer measurements.

Anthropogenic emissions in Asia have significantly increased during the last two decades; as a result, the induced air pollution and its influences on radiative forcing and public health are becoming increasingly prominent. The Aerodyne Aerosol Mass Spectrometer (AMS) has been widely deployed in Asia for real-time characterization of aerosol chemistry. In this paper, we review the AMS measurements in Asia, mainly in China, Korea, Japan, and India since 2001 and summarize the key results and findings. The mass concentrations of non-refractory submicron aerosol species (NR-PM1) showed large spatial distributions with high mass loadings occurring in India and north and northwest China (60.2-81.3 μg m-3), whereas much lower values were observed in Korea, Japan, Singapore and regional background sites (7.5-15.1 μg m-3). Aerosol composition varied largely in different regions, but was overall dominated by organic aerosols (OA, 32-75%), especially in south and southeast Asia due to the impact of biomass burning. While sulfate and nitrate showed comparable contributions in urban and suburban regions in north China, sulfate dominated inorganic aerosols in south China, Japan and regional background sites. Positive matrix factorization analysis identified multiple OA factors from different sources and processes in different atmospheric environments, e.g., biomass burning OA in south and southeast Asia and agricultural seasons in China, cooking OA in urban areas, and coal combustion in north China. However, secondary OA (SOA) was a ubiquitous and dominant aerosol component in all regions, accounting for 43-78% of OA. The formation of different SOA subtypes associated with photochemical production or aqueous-phase/fog processing was widely investigated. The roles of primary emissions, secondary production, regional transport, and meteorology on severe haze episodes, and different chemical responses of primary and secondary aerosol species to source emission changes and meteorology were also demonstrated. Finally, future prospects of AMS studies on long-term and aircraft measurements, water-soluble OA, the link of OA volatility, oxidation levels, and phase state were discussed.

Towards an Algorithm for Near Real Time Profiling of Aerosol Species, Trace Gases, and Clouds Based on the Synergy of Remote Sensing Instruments

In this manuscript we present the concept of a novel algorithmic chain that aims to a dataset of unprecedented detail in the vertical distribution of multiple atmospheric components in near real time conditions. The analysis will be based on the following remote sensing instruments: a depolarization Raman lidar, a visible and a thermal all-sky camera, a Brewer spectrophotometer, and up to three mini DOAS/MAX-DOAS systems. Based on both individual and synergistic processing of the data collected, novel products will be made available in near real time conditions to the end users. Columnar aerosol information from the spectrophotometers will be combined with lidar data to retrieve vertical profiles of individual aerosol species. Cloud layers will be detected and classified based mainly on the synergy of the lidar and the sky cameras and a realistic 3D representation of cloud conditions around the measurement site will be produced. Lidar profiles will be implemented as a priori information for radiative transfer purposes, that are necessary in order to obtain high quality trace gases profiles from the DOAS/MAX-DOAS spectrophotometer. Fast synergistic data processing will ensure that the algorithm can be applied for near real time public data dissemination in the future.