Long-term variations in surface ozone at the Longfengshan Regional Atmosphere Background Station in Northeast China and related influencing factors.

Surface ozone (O3) is a crucial air pollutant that affects air quality, human health, agricultural production, and climate change. Studies on long-term O3 variations and their influencing factors are essential for understanding O3 pollution and its impact. Here, we conducted an analysis of long-term variations in O3 during 2006-2022 at the Longfengshan Regional Atmosphere Background Station (LFS; 44.44°N, 127.36°E, 330.5 m a.s.l.) situated on the northeastern edge of the Northeast China Plains. The maximum daily 8-h average (MDA8) O3 fluctuated substantially, with the annual MDA8 decreasing significantly during 2006-2015 (-0.62 ppb yr-1, p < 0.05), jumping during 2015-2016 and increasing clearly during 2020-2022. Step multiple linear regression models for MDA8 were obtained using meteorological variables, to decompose anthropogenic and meteorological contributions to O3 variations. Anthropogenic activities acted as the primary drivers of the long-term trends of MDA8 O3, contributing 73% of annual MDA8 O3 variability, whereas meteorology played less important roles (27%). Elevated O3 at LFS were primarily associated with airflows originating from the North China Plain, Northeast China Plain, and coastal areas of North China, primarily occurring during the warm months (May-October). Based on satellite products of NO2 and HCHO columns, the O3 photochemical regimes over LFS revealed NOx-limited throughout the period. NO2 increased first, reaching peak in 2011, followed by substantial decrease; while HCHO exhibited significant increase, contributing to decreasing trend in MDA8 O3 during 2006-2015. The plateauing NO2 and decreasing HCHO may contribute to the increase in MDA8 O3 in 2016. Subsequently, both NO2 and HCHO exhibited notable fluctuations, leading to significant changes in O3. The study results fill the gap in the understanding of long-term O3 trends in high-latitude areas in the Northeast China Plain and offer valuable insights for assessing the impact of O3 on crop yields, forest productivity, and climate change.

Proposed Missions to Collect Samples for Analyzing Evidence of Life in the Venusian Atmosphere.

The recent and still controversial claim of phosphine detection in the venusian atmosphere has reignited consideration of whether microbial life might reside in its cloud layers. If microbial life were to exist within Venus' cloud deck, these microorganisms would have to be multi-extremophiles enclosed within the cloud aerosol particles. The most straightforward approach for resolving the question of their existence is to obtain samples of the cloud particles and analyze their interior. While developing technology has made sophisticated in situ analysis possible, more detailed information could be obtained by examining samples with instrumentation in dedicated ground-based facilities. Ultimately, therefore, Venus Cloud-level Sample Return Missions will likely be required to resolve the question of whether living organisms exist in the clouds of Venus. Two multiphase mission concepts are currently under development for combining in situ analyses with a sample return component. The Venus Life Finder architecture proposes collection of cloud particles in a compartment suspended from a balloon that floats for weeks at the desired altitude, while the Novel solUtion for Venus explOration and Lunar Exploitation (NUVOLE) concept involves a glider that cruises within the cloud deck for 1200 km collecting cloud aerosol particles through the key regions of interest. Both architectures propose a rocket-driven ascent with the acquired samples transported to a high venusian orbit as a prelude to returning to Earth or the Moon. Both future conceptual missions with their combined phases will contribute valuable information relative to the habitability of the clouds at Venus, but their fulfillment is decades away. We suggest that, in the meantime, a simplification of a glider cloud-level sample collection scenario could be accomplished in a shorter development time at a lower cost. Even if the cloud particles are not organic and show no evidence of living organisms, they would reveal critical insights about the natural history and evolution of Venus.

Evaluation of MERRA-2 and CAMS reanalysis for black carbon aerosol in China.

Black carbon (BC) constitutes a pivotal component of atmospheric aerosols, significantly impacting regional and global radiation balance, climate, and human health. In this study, we evaluated BC data in two prominent atmospheric composition reanalysis datasets: the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) and the Copernicus Atmosphere Monitoring Service (CAMS), and analyzed the causes of their deviations. This assessment is based on observational data collected from 34 monitoring stations across China from 2006 to 2022. Our research reveals a significant and consistent decline in BC concentrations within China, amounting to a reduction exceeding 67.33%. However, both MERRA-2 and CAMS reanalysis data fail to capture this declining trend. The average annual decrease of BC in MERRA-2 from 2006 to 2022 is only 0.06 µg/m3 per year, while the BC concentration in CAMS even increased with an average annual value of 0.014 µg/m3 per year. In 2022, MERRA-2 had overestimated BC concentration by 20% compared to observational data, while CAMS had overestimated it by approximately 66%. In the regional BC concentration analysis, the data quality of the reanalysis data is better in the South China (RM = 0.59, RC = 0.53), followed by the North China (RM = 0.50, RC = 0.42). Reanalysis BC data in Northwest China and the Tibetan Plateau are difficult to use for practical analysis due to their big difference with observation. In a comparison of the anthropogenic BC emissions inventory used in the two atmospheric composition reanalysis datasets with the Multi-resolution Emission Inventory model for Climate and air pollution research (MEIC) emissions inventory, we found that: Despite the significant decline in China's BC emissions, MERRA-2 still relies on the 2006 emissions inventory, while CAMS utilizes emission inventories that even show an increasing trend. These factors will undoubtedly lead to greater deviations between reanalysis and observational data.

Aerosolized Cyanobacterial Harmful Algal Bloom Toxins: Microcystin Congeners Quantified in the Atmosphere.

Cyanobacterial harmful algal blooms (cHABs) have the potential to adversely affect public health through the production of toxins such as microcystins, which consist of numerous molecularly distinct congeners. Microcystins have been observed in the atmosphere after emission from freshwater lakes, but little is known about the health effects of inhaling microcystins and the factors contributing to microcystin aerosolization. This study quantified total microcystin concentrations in water and aerosol samples collected around Grand Lake St. Marys (GLSM), Ohio. Microcystin concentrations in water samples collected on the same day ranged from 13 to 23 µg/L, dominated by the d-Asp3-MC-RR congener. In particulate matter <2.5 µm (PM2.5), microcystin concentrations up to 156 pg/m3 were detected; the microcystins were composed primarily of d-Asp3-MC-RR, with additional congeners (d-Asp3-MC-HtyR and d-Asp3-MC-LR) observed in a sample collected prior to a storm event. The PM size fraction containing the highest aerosolized MC concentration ranged from 0.44 to 2.5 µm. Analysis of total bacteria by qPCR targeting 16S rDNA revealed concentrations up to 9.4 × 104 gc/m3 in aerosol samples (≤3 µm), while a marker specific to cyanobacteria was not detected in any aerosol samples. Concentrations of aerosolized microcystins varied even when concentrations in water were relatively constant, demonstrating the importance of meteorological conditions (wind speed and direction) and aerosol generation mechanism(s) (wave breaking, spillway, and aeration systems) when evaluating inhalation exposure to microcystins and subsequent impacts on human health.

Atmospheric parameters play an important role in driving hydrogen sulphide concentrations in ambient air near waste management centres.

Emissions of odorous compounds are major contributors to public opposition when siting waste management facilities. Thus, it is essential to understand how to minimise the concentration of odour-causing chemicals in ambient air surrounding such facilities. Although the concentration of pollutants in the atmosphere is a function of meteorology, there is limited data on the atmospheric parameters that drive ambient air concentrations of odour-causing substances in settlements near waste management facilities. Here, we analysed how temperature, wind direction, wind speed, atmospheric pressure and humidity impact the concentrations of hydrogen sulphide (H2S) in the ambient air, a potentially toxic chemical and a chief contributor to noxious odours. The relative contribution of each variable was assessed using multivariate statistical analysis applied to an extensive data set of over 7,000 data points collected during 2021. Our results show that all tested atmospheric parameters significantly affected H2S concentrations in ambient air. Wind direction had the greatest impact on H2S concentrations, followed by temperature, humidity, atmospheric pressure and wind speed. Specifically, the concentration of H2S was positively correlated with humidity and atmospheric pressure and had a U-shaped correlation with temperature. Atmospheric variables were able to explain 15% of variation in H2S concentrations (R2 = 15%), indicating the presence of other factors affecting H2S ambient air concentrations. Our study shows that proper consideration of atmospheric parameters, especially wind direction and temperatures, is of uttermost importance when siting waste management facilities. The conclusions are broadly applicable to odorous compounds near waste management facilities, so adverse effects to human health and the environment can be minimised.

Assessing the Intensity of Marine Biogenic Influence on the Lower Atmosphere: An Insight into the Distribution of Marine Biogenic Aerosols over the Eastern China Seas.

Marine biological activities make a non-negligible contribution to atmospheric aerosols, leading to potential impacts on the regional atmospheric environment and climate. The eastern China seas are highly productive with significant emissions of biogenic substances, but the spatiotemporal variations of marine biogenic aerosols are not well known. Air mass exposure to chlorophyll a (AEC) can be used to indicate the influence of biogenic sources on the atmosphere to a certain degree. In this study, the 12 year (2009-2020) daily AEC were calculated over the eastern China seas, showing the spatial and seasonal patterns of marine biogenic influence intensity which were co-controlled by surface phytoplankton biomass and boundary layer height. By combining the AEC values, relevant meteorological parameters, and extensive observations of a typical biogenic secondary aerosol component, methanesulfonate (MSA), a parameterization scheme for MSA simulation was successfully constructed. This AEC-based approach with observation constraints provides a new insight into the distribution of marine biogenic aerosols. Meanwhile, the wintertime air mass retention over land exhibited a significant decrease, showing a decadal weakening trend of terrestrial transport, which is probably related to the weakening of the East Asian winter monsoon. Thus, marine biogenic aerosols may play an increasingly important role in the studied region.

An analysis of atmospheric stability indices and parameters under air pollution conditions.

The stability of the atmosphere plays an important role in changes in air pollutant concentrations. Stable atmospheric conditions cause pollutant concentrations to reach high values, which degrades the air quality in a particular region. This study aims to reveal the relationship between atmospheric stability indices/parameters (thermodynamic indices) and changes in air pollutant concentrations. Pollutant concentrations of PM10, PM2.5, SO2, NO2, CO, and O3 were statistically analyzed for a 10-year (2013-2022) period for nine air quality stations located in the megacity Istanbul. Based on national and international air quality standards, 145 episode days were determined for the days when these parameters exceeded the threshold values. Five stability indices (Showalter Index - SI, Lifted Index - LI, Severe Weather Index - SWEAT, K Index - KI, Totals Totals Index - TTI), and three stability parameters (Convective Available Potential Energy - CAPE, Convective Inhibition - CIN, Bulk Richardson Number - BRN) were used to determine the stability of the atmosphere for episode days. It has been found that in cases where air pollutant concentrations are high, the stability parameters reveal the stability of the atmosphere better than the stability indices. It was also found that there was at least one vertical inversion layer on 122 of the 145 episode days, these layers mostly (84%) occurred between the surface and 850 hPa levels, and the layer thicknesses were mostly between 0-250 m (84%).

Natural short-lived halogens exert an indirect cooling effect on climate.

Observational evidence shows the ubiquitous presence of ocean-emitted short-lived halogens in the global atmosphere1-3. Natural emissions of these chemical compounds have been anthropogenically amplified since pre-industrial times4-6, while, in addition, anthropogenic short-lived halocarbons are currently being emitted to the atmosphere7,8. Despite their widespread distribution in the atmosphere, the combined impact of these species on Earth's radiative balance remains unknown. Here we show that short-lived halogens exert a substantial indirect cooling effect at present (-0.13 ± 0.03 watts per square metre) that arises from halogen-mediated radiative perturbations of ozone (-0.24 ± 0.02 watts per square metre), compensated by those from methane (+0.09 ± 0.01 watts per square metre), aerosols (+0.03 ± 0.01 watts per square metre) and stratospheric water vapour (+0.011 ± 0.001 watts per square metre). Importantly, this substantial cooling effect has increased since 1750 by -0.05 ± 0.03 watts per square metre (61 per cent), driven by the anthropogenic amplification of natural halogen emissions, and is projected to change further (18-31 per cent by 2100) depending on climate warming projections and socioeconomic development. We conclude that the indirect radiative effect due to short-lived halogens should now be incorporated into climate models to provide a more realistic natural baseline of Earth's climate system.

Global PM2.5 Prediction and Associated Mortality to 2100 under Different Climate Change Scenarios.

Ambient fine particulate matter (PM2.5) has severe adverse health impacts, making it crucial to reduce PM2.5 exposure for public health. Meteorological and emissions factors, which considerably affect the PM2.5 concentrations in the atmosphere, vary substantially under different climate change scenarios. In this work, global PM2.5 concentrations from 2021 to 2100 were generated by combining the deep learning technique, reanalysis data, emission data, and bias-corrected CMIP6 future climate scenario data. Based on the estimated PM2.5 concentrations, the future premature mortality burden was assessed using the Global Exposure Mortality Model. Our results reveal that SSP3-7.0 scenario is associated with the highest PM2.5 exposure, with a global concentration of 34.5 µg/m3 in 2100, while SSP1-2.6 scenario has the lowest exposure, with an estimated of 15.7 µg/m3 in 2100. PM2.5-related deaths for individuals under 75 years will decrease by 16.3 and 10.5% under SSP1-2.6 and SSP5-8.5, respectively, from 2030s to 2090s. However, premature mortality for elderly individuals (>75 years) will increase, causing the contrary trends of improved air quality and increased total PM2.5-related deaths in the four SSPs. Our results emphasize the need for stronger air pollution mitigation measures to offset the future burden posed by population age.

Aerosols' variability and their relationship with climatic parameters over West Africa.

Aerosols' influences on Earth's climate have been documented by several authors. This ranges from scattering and reflecting of shortwave radiation (direct effect) which is also regarded as the "Whitehouse Effect," to the ability to act as condensation nuclei (indirect effect) which results in cloud droplet formation. This broad summary of aerosol's effect on earth's climate has in turn affected some other weather variables either positively or negatively depending on people's perspectives. This work was done in a view to ascertaining some of these claims by determining the statistical significance of some certain aerosol's relationships with some selected weather variables. This was done over six (6) stations across the West African region to represent the climatic zones from the rainforest around the coasts to the desert of the Sahel. Data used consist of aerosol types (biomass burning, carbonaceous, dust, and PM2.5) and climatic types (convective precipitation, wind speed, and water vapor) over a period of 30 years, with the python and ferret programs explicitly used for the graphical analyses. Climatologically, locations close to the point source seem to record more of the presence of the pollutants than the farthest ones. Results indicated that aerosols were more pronounced in the dry months of NDJF over the rainforest region depending on the latitudinal position of the location. The relationship result showed a negative correlation between convective precipitation and aerosols, except carbonaceous. But the strongest relationship can be found between water vapor and the selected aerosol types.

Sources, size-resolved deposition in the human respiratory tract and health risks of submicron black carbon in urban atmosphere in Pearl River Delta, China.

Black carbon (BC) has a significantly negative impact on air quality, climate and human health. Here we investigated the sources and health effects of BC in urban area of the Pearl River Delta (PRD) based on online data measured by Aerodyne soot particle high-resolution time of flight aerosol mass spectrometer (SP-AMS). In urban PRD, BC particles mainly came from vehicle emissions especially heavy-duty vehicle exhausts (contributing 42.9 % of total BC mass concentration), long-range transport (27.6 %), and aged biomass combustion emissions (22.3 %). Indicated by source analysis using simultaneous aethalometer data, BC associated with local secondary oxidation and transport may also be originated from fossil fuel combustion, especially traffic sources in urban and surrounding areas. Size-resolved BC mass concentrations provided by SP-AMS, for the first time to our best knowledge, were used to calculate BC deposition in the human respiratory tract (HRT) of different populations (children, adults, and the elderly) by the Multiple-Path Particle Dosimetry (MPPD) model. We found that submicron BC was deposited more in the pulmonary (P) region (49.0-53.2 % of the total BC deposition dose), while less in the tracheobronchial (TB, 35.6-37.2 %) and head (HA, 11.2-13.8 %) regions. Adults suffered the highest BC deposition (1.19 µg day-1) than the elderly (1.09 µg day-1) and children (0.25 µg day-1). BC deposition rate was greater at night (especially 18:00-24:00) than during the daytime. The maximum deposition in the HRT was found for BC particles around 100 nm, mainly in deeper respiratory regions (TB and P), which may cause more serious health effects. Adults and the elderly group are confronted with the notable carcinogenic risk of BC in the urban PRD, up to 29 times higher than the threshold. Our study emphasizes the need to control BC pollution in the urban area, especially nighttime vehicle emissions.

Unexpectedly Efficient Aging of Organic Aerosols Mediated by Autoxidation.

Multiphase oxidative aging is a ubiquitous process for atmospheric organic aerosols (OA). But its kinetics was often found to be slow in previous laboratory studies where high hydroxyl radical concentrations ([•OH]) were used. In this study, we performed heterogeneous oxidation experiments of several model OA systems under varied aging timescales and gas-phase [•OH]. Our results suggest that OA heterogeneous oxidation may be 2-3 orders of magnitude faster when [•OH] is decreased from typical laboratory flow tube conditions to atmospheric levels. Direct laboratory mass spectrometry measurements coupled with kinetic simulations suggest that an intermolecular autoxidation mechanism mediated by particle-phase peroxy radicals greatly accelerates OA oxidation, with enhanced formation of organic hydroperoxides, alcohols, and fragmentation products. With autoxidation, we estimate that the OA oxidation timescale in the atmosphere may be from less than a day to several days. Thus, OA oxidative aging can have greater atmospheric impacts than previously expected. Furthermore, our findings reveal the nature of heterogeneous aerosol oxidation chemistry in the atmosphere and help improve the understanding and prediction of atmospheric OA aging and composition evolution.

Human-induced weakening of the Northern Hemisphere tropical circulation.

By accounting for most of the poleward atmospheric heat and moisture transport in the tropics, the Hadley circulation largely affects the latitudinal patterns of precipitation and temperature at low latitudes. To increase our preparednesses for human-induced climate change, it is thus critical to accurately assess the response of the Hadley circulation to anthropogenic emissions1-3. However, at present, there is a large uncertainty in recent Northern Hemisphere Hadley circulation strength changes4. Not only do climate models simulate a weakening of the circulation5, whereas atmospheric reanalyses mostly show an intensification of the circulation4-8, but atmospheric reanalyses were found to have artificial biases in the strength of the circulation5, resulting in unknown impacts of human emissions on recent Hadley circulation changes. Here we constrain the recent changes in the Hadley circulation using sea-level pressure measurements and show that, in agreement with the latest suite of climate models, the circulation has considerably weakened over recent decades. We further show that the weakening of the circulation is attributable to anthropogenic emissions, which increases our confidence in human-induced tropical climate change projections. Given the large climate impacts of the circulation at low latitudes, the recent human-induced weakening of the flow suggests wider consequences for the regional tropical-subtropical climate.

Aircraft surveys for air eDNA: probing biodiversity in the sky.

Air is a medium for dispersal of environmental DNA (eDNA) carried in bioaerosols, yet the atmosphere is mostly unexplored as a source of genetic material encompassing all domains of life. In this study, we designed and deployed a robust, sterilizable hardware system for airborne nucleic acid capture featuring active filtration of a quantifiable, controllable volume of air and a high-integrity chamber to protect the sample from loss or contamination. We used our hardware system on an aircraft across multiple height transects over major aerosolization sources to collect air eDNA, coupled with high-throughput amplicon sequencing using multiple DNA metabarcoding markers targeting bacteria, plants, and vertebrates to test the hypothesis of large-scale genetic presence of these bioaerosols throughout the planetary boundary layer in the lower troposphere. Here, we demonstrate that the multi-taxa DNA assemblages inventoried up to 2,500 m using our airplane-mounted hardware system are reflective of major aerosolization sources in the survey area and show previously unreported airborne species detections (i.e., Allium sativum L). We also pioneer an aerial survey flight grid standardized for atmospheric sampling of genetic material and aeroallergens using a light aircraft and limited resources. Our results show that air eDNA from terrestrial bacteria, plants, and vertebrates is detectable up to high altitude using our airborne air sampler and demonstrate the usefulness of light aircraft in monitoring campaigns. However, our work also underscores the need for improved marker choices and reference databases for species in the air column, particularly eukaryotes. Taken together, our findings reveal strong connectivity or mixing of terrestrial-associated eDNA from ground level aerosolization sources and the atmosphere, and we recommend that parameters and indices considering lifting action, atmospheric instability, and potential for convection be incorporated in future surveys for air eDNA. Overall, this work establishes a foundation for light aircraft campaigns to comprehensively and economically inventory bioaerosol emissions and impacts at scale, enabling transformative future opportunities in airborne DNA technology.

Spatial and temporal heterogeneity of air pollution in East Africa.

East Africa's air pollution levels are deteriorating due to anthropogenic and biomass burning emissions and unfavorable weather conditions. This study investigates the changes and influencing factors of air pollution in East Africa from 2001 to 2021. The study found that air pollution in the region is heterogeneous, with increasing trends observed in pollution hot spots (PHS) while it decreased in pollution cold spots (PCS). The analysis identified four major pollution periods: High Pollution period 1, Low Pollution period 1, High Pollution period 2, and Low Pollution period 2, which occur during Feb-Mar, Apr-May, Jun-Aug and Oct-Nov, respectively. The study also revealed that long range transport of pollutants to the study area is primarily influenced by distant sources from the eastern, western, southern, and northern part of the continent. The seasonal meteorological conditions, such as high sea level pressure in the upper latitudes, cold air masses from the northern hemisphere, dry vegetation, and a dry and less humid atmosphere from boreal winter, further impact the transport of pollutants. The concentrations of pollutants were found to be influenced by climate factors, such as temperature, precipitation, and wind patterns. The study identified different pollution patterns in different seasons, with some areas having minimal anthropogenic pollution due to high vegetation vigor and moderate precipitation. Using Ordinary Least Square (OLS) regression and Detrended Fluctuation Analysis (DFA), the study quantified the magnitude of spatial variation in air pollution. The OLS trends indicated that 66 % of pixels exhibited decreasing trends while 34 % showed increasing trends, and DFA results indicating that 36 %, 15 %, and 49 % of pixels exhibited anti-persistence, random, and persistence in air pollution, respectively. Areas in the region experiencing increasing or decreasing trends in air pollution, which can be used to prioritize interventions and resources for improving air quality, were also highlighted. It also identifies the driving forces behind air pollution trends, such as anthropogenic or biomass burning, which can inform policy decisions aimed at reducing air pollution emissions from these sources. The findings on the persistence, reversibility, and variability of air pollution can inform the development of long-term policies for improving air quality and protecting public health.

Regional transportation and influence of atmospheric aerosols triggered by Tonga volcanic eruption.

A cataclysmic submarine volcano at Hunga Tonga-HungaHa'apai (HTHH) near Tonga, erupted violently on 15 January 2022, which injected a plume of ash cloud soaring into the upper atmosphere. In this study, we examined the regional transportation and potential influence of atmospheric aerosols triggered by HTHH volcano, based on active and passive satellite products, ground-based observations, multi-source reanalysis datasets and atmospheric radiative transfer model. The results indicated that about 0.7 Tg (1 Tg = 109 kg) sulfur dioxide (SO2) gas were emitted into stratosphere from the HTHH volcano, and were lifted to an altitude of 30 km. The regional averaged SO2 columnar content over the western Tonga increased by 10-36 Dobson Units (DU), and the mean aerosol optical thickness (AOT) retrieved from satellite products increased to 0.25-0.34. The stratospheric AOT values caused by HTHH emissions increased to 0.03, 0.20, and 0.23 on 16, 17, and 19 January, respectively, accounting for 1.5%, 21.9%, and 31.1% of total AOT. Ground-based observations also showed an AOT increase of 0.25-0.43, with the maximum daily average of 0.46-0.71 appeared on 17 January. The volcanic aerosols were remarkably dominated by fine-mode particles and posed strong light-scattering and hygroscopic abilities. Consequently, the mean downward surface net shortwave radiative flux was reduced by 2.45-11.9 Wm-2 on different regional scales, and the surface temperature decreased by 0.16-0.42 K. The maximum aerosol extinction coefficient was 0.51 km-1 appeared at 27 km, which resulted in an instantaneous shortwave heating rate of 1.80 Khour-1. These volcanic materials stayed stable in the stratosphere and completed one circle around the earth within 15 days. This would exert a profound influence on the energy budget, water vapor and ozone exchange in the stratosphere, which deserves to be further studied.

Field Evidence for Asian Outflow and Fast Depletion of Total Gaseous Mercury in the Polluted Coastal Atmosphere.

Atmospheric mercury (Hg) cycling in polluted coastal atmosphere is complicated and not fully understood. Here, we present measurements of total gaseous mercury (TGM) monitored at a coastal mountaintop in Hong Kong downwind of mainland China. Sharp TGM peaks during cold front passages were frequently observed due to Asian pollution outflow with typical TGM/CO slopes of 6.8 ± 2.2 pg m-3 ppbv-1. Contrary to the daytime maximums of other air pollutants, TGM exhibited a distinct diurnal variation with a midday minimum. Moreover, we observed four cases of extremely fast TGM depletion after sunrise, during which TGM concentrations rapidly dipped to 0.3-0.6 ng m-3 accompanied by other pollutants on the rise. Simulated meteorological fields revealed that morning upslope flow transporting anthropogenically polluted but TGM-depleted air masses from the mixed layer caused morning TGM depletion at the mountaintop location. The TGM-depleted air masses were hypothesized to result mainly from fast photooxidation of Hg after sunrise with minor contributions from dry deposition (5.0%) and nocturnal oxidation (0.6%). A bromine-induced two-step oxidation mechanism involving abundant pollutants (NO2, O3, etc.) was estimated to play a dominant role, contributing 55%-60% of depleted TGM and requiring 0.20-0.26 pptv Br, an amount potentially available through sea salt aerosol debromination. Our findings suggest significant effects of the interaction between anthropogenic pollution and marine halogen chemistry on atmospheric Hg cycling in the coastal areas.

A geospatial risk analysis graphical user interface for identifying hazardous chemical emission sources.

Background: Performing back trajectory and forward trajectory using the Hybrid Single-Particle Lagrangian Integrated Trajectory Model (HYSPLIT) is a reliable approach for assessing particle transport after release among mid-field atmospheric models. HYSPLIT has an externally facing online interface that allows non-expert users to run the model trajectories without requiring extensive training or programming. However, the existing HYSPLIT interface is limited if simulations have a large amount of meteorological data and timesteps that are not coincident. The objective of this study is to design and develop a more robust tool to rapidly evaluate hazard transport conditions and to perform risk analysis, while still maintaining an intuitive and user-friendly interface. Methods: HYSPLIT calculates forward and backward trajectories of particles based on wind speed, wind direction, and the corresponding location, timestamp, and Pasquill stability classes of the regions of the atmosphere in terms of the wind speed, the amount of solar radiation, and the fractional cloud cover. The computed particle transport trajectories, combined with the online Proton Transfer Reaction-Mass Spectrometry (PTR-MS) data (https://figshare.com/articles/dataset/ARL_Data_from_PROS_station_at_Hanford_site/19993964), can be used to identify and quantify the sources and affected area of the hazardous chemicals' emission using the potential source distribution function (PSDF). PSDF is an improved statistical function based on the well-known potential source contribution function (PSCF) in establishing the air pollutant source and receptor relationship. Performing this analysis requires a range of meteorological and pollutant concentration measurements to be statistically meaningful. The existing HYSPLIT graphical user interface (GUI) does not easily permit computations of trajectories of a dataset of meteorological data in high temporal frequency. To improve the performance of HYSPLIT computations from a large dataset and enhance risk analysis of the accidental release of material at risk, a geospatial risk analysis tool (GRAT-GUI) is created to allow large data sets to be processed instantaneously and to provide ease of visualization. Results: The GRAT-GUI is a native desktop-based application and can be run in any Windows 10 system without any internet access requirements, thus providing a secure way to process large meteorological datasets even on a standalone computer. GRAT-GUI has features to import, integrate, and convert meteorological data with various formats for hazardous chemical emission source identification and risk analysis as a self-explanatory user interface. The tool is available at https://figshare.com/articles/software/GRAT/19426742.

Parameter Optimization and Development of Mini Infrared Lidar for Atmospheric Three-Dimensional Detection.

In order to conduct more thorough research on the structural characteristics of the atmosphere and the distribution and transmission of atmospheric pollution, the use of remote sensing technology for multi-dimensional detection of the atmosphere is needed. A light-weight, low-volume, low-cost, easy-to-use and low-maintenance mini Infrared Lidar (mIRLidar) sensor is developed for the first time. The model of lidar is established, and the key optical parameters of the mIRLidar are optimized through simulation, in which wavelength of laser, energy of pulse laser, diameter of telescope, field of view (FOV), and bandwidth of filter are included. The volume and weight of the lidar system are effectively reduced through optimizing the structural design and designing a temperature control system to ensure the stable operation of the core components. The mIRLidar system involved a 1064 nm laser (the pulse laser energy 15 µJ, the repetition frequency 5 kHz), a 100 mm aperture telescope (the FOV 1.5 mrad), a 0.5 nm bandwidth of filter and an APD, where the lidar has a volume of 200 mm × 200 mm × 420 mm and weighs about 13.5 kg. It is shown that the lidar can effectively detect three-dimensional distribution and transmission of aerosol and atmospheric pollution within a 5 km detection range, from Horizontal, scanning and navigational atmospheric measurements. It has great potential in the field of meteorological research and environmental monitoring.

Gaseous elemental mercury and its evasion fluxes in the marine boundary layer of the marginal seas of the northwestern Pacific: Results from two cruises in September-December 2019.

There are many questions regarding the behavior of mercury in the sea-atmosphere system of the northwestern Pacific. Continuous underway measurements of atmospheric gaseous elemental mercury (GEM) and measurements of sea-air GEM evasion fluxes were carried out in the marginal seas of northwestern Pacific from the South China Sea to the Sea of Okhotsk in fall-winter 2019. The median GEM concentration (1.1 ng/m3) was lower than both the background value and the averages previously observed in these areas. A latitudinal gradient of atmospheric GEM and GEM evasion fluxes with maximum values at southern latitudes was found. The following areas have been identified as potential source areas: the Kurill area of the Pacific Ocean Northeast China, Korean Peninsula, and the territory from the southwest coast of the Yellow Sea to the south of Indochina. Seasonal variations were observed in the Sea of Japan and East China Sea with higher GEM concentrations in winter than in fall. Our data and analysis of published data showed significant relationships between GEM evasion fluxes, latitude and sea surface temperature (SST). It seems that on a global scale, along with the GEM gradient between water and atmosphere, SST is the most significant parameter for sea-air GEM evasion fluxes.