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The atmospheric deposition of mercury (Hg) occurs via several mechanisms, including dry and wet scavenging by precipitation events. In an effort to understand the atmospheric cycling and seasonal depositional characteristics of Hg, wet deposition samples were collected for approximately 5 years at 17 selected GMOS monitoring sites located in the Northern and Southern hemispheres in the framework of the Global Mercury Observation System (GMOS) project. Total mercury (THg) exhibited annual and seasonal patterns in Hg wet deposition samples. Interannual differences in total wet deposition are mostly linked with precipitation volume, with the greatest deposition flux occurring in the wettest years. This data set provides a new insight into baseline concentrations of THg concentrations in precipitation worldwide, particularly in regions such as the Southern Hemisphere and tropical areas where wet deposition as well as atmospheric Hg species were not investigated before, opening the way for future and additional simultaneous measurements across the GMOS network as well as new findings in future modeling studies.

Long-range transport of biogenic emissions from the coast of Antarctica, precipitation scavenging, and cloud processing are the main processes that influence the observed variability in Southern Ocean (SO) marine boundary layer (MBL) condensation nuclei (CN) and cloud condensation nuclei (CCN) concentrations during the austral summer. Airborne particle measurements on the HIAPER GV from north–south transects between Hobart, Tasmania, and 62∘ S during the Southern Ocean Clouds, Radiation Aerosol Transport Experimental Study (SOCRATES) were separated into four regimes comprising combinations of high and low concentrations of CCN and CN. In 5 d HYSPLIT back trajectories, air parcels with elevated CCN concentrations were almost always shown to have crossed the Antarctic coast, a location with elevated phytoplankton emissions relative to the rest of the SO in the region south of Australia. The presence of high CCN concentrations was also consistent with high cloud fractions over their trajectory, suggesting there was substantial growth of biogenically formed particles through cloud processing. Cases with low cloud fraction, due to the presence of cumulus clouds, had high CN concentrations, consistent with previously reported new particle formation in cumulus outflow regions. Measurements associated with elevated precipitation during the previous 1.5 d of their trajectory had low CCN concentrations indicating CCN were effectively scavenged by precipitation. A coarse-mode fitting algorithm was used to determine the primary marine aerosol (PMA) contribution, which accounted for <20 % of CCN (at 0.3 % supersaturation) and cloud droplet number concentrations. Vertical profiles of CN and large particle concentrations (Dp>0.07 µm) indicated that particle formation occurs more frequently above the MBL; however, the growth of recently formed particles typically occurs in the MBL, consistent with cloud processing and the condensation of volatile compound oxidation products. CCN measurements on the R/V Investigator as part of the second Clouds, Aerosols, Precipitation, Radiation and atmospheric Composition Over the southeRn Ocean (CAPRICORN-2) campaign were also conducted during the same period as the SOCRATES study. The R/V Investigator observed elevated CCN concentrations near Australia, likely due to continental and coastal biogenic emissions. The Antarctic coastal source of CCN from the south, CCN sources from the midlatitudes, and enhanced precipitation sink in the cyclonic circulation between the Ferrel and polar cells (around 60∘ S) create opposing latitudinal gradients in the CCN concentration with an observed minimum in the SO between 55 and 60∘ S. The SOCRATES airborne measurements are not influenced by Australian continental emissions but still show evidence of elevated CCN concentrations to the south of 60∘ S, consistent with biogenic coastal emissions. In addition, a latitudinal gradient in the particle composition, south of the Australian and Tasmanian coasts, is apparent in aerosol hygroscopicity derived from CCN spectra and aerosol particle size distribution. The particles are more hygroscopic to the north, consistent with a greater fraction of sea salt from PMA, and less hygroscopic to the south as there is more sulfate and organic particles originating from biogenic sources in coastal Antarctica.

Atmospheric nitrogen deposition modulates carbon sequestration by terrestrial ecosystems via nitrogen‐carbon interactions. The intertwined chemical and physical processes in nitrogen deposition and subsequent nitrogen‐carbon interactions pose challenges for Earth system model (ESM) in quantifying them. Here, we combine 30‐year nitrogen wet deposition measurements (1980–2014) with Coupled Model Intercomparison Project Phase 6 (CMIP6) simulations to disentangle the nitrogen wet deposition variabilities across different scales. We show that observed decadal trends in nitrogen deposition can be reproduced by ESMs for the United States and Europe, but diverge in East Asia. Models generally fail to capture nitrogen deposition seasonality, with distinct driving factors of model errors for different nitrogen forms. The incorrect ammonia emission seasonality explains the bias in reduced nitrogen deposition, whereas precipitation scavenging and nitrogen oxides chemical oxidation collectively determine the seasonal bias of oxidized nitrogen deposition. Our results can facilitate the informed assessment of nitrogen‐carbon‐climate interactions under changing human activities.

In response to increasing production and application volumes, organophosphate esters (OPEs) have emerged as pervasively detected contaminants in various environmental media, with concentrations often exceeding those of traditional organic contaminants. Despite the recognition of the atmosphere's important role in dispersing OPEs and a substantial number of studies quantifying OPEs in air, investigations into atmospheric phase distribution processes are rare. Using measurements of OPEs in the atmospheric gas and particle phase, in precipitation, and in surface water collected in southern Canada, we explored the seasonal concentration variability, gas–particle partitioning behaviour, precipitation scavenging, and air–water equilibrium status of OPEs. Whereas consistent seasonal trends were not observed for OPE concentrations in precipitation or atmospheric particles, gas phase concentrations of several OPEs were elevated during the summer in suburban Toronto and at two remote sites on Canada's eastern and western coast. Apparent enthalpies of air–surface exchange fell mainly within or slightly above the range of air–water and air–octanol enthalpies of exchange, indicating the influence of local air–surface exchange processes and/or seasonally variable source strength. While many OPEs were present with a notable fraction in both the gas and particle phase, no clear relationship with compound volatility was apparent, although there was a tendency for higher particle-bound fractions at a lower temperature. High precipitation scavenging ratios for OPEs measured at the two coastal sites are consistent with low air–water partitioning ratios and the association with particles. Although beset by large uncertainties, air–water equilibrium calculations suggest net deposition of gaseous OPEs from the atmosphere to the Salish Sea and the St. Lawrence River and St. Lawrence Estuary. The measured seasonal concentration variability is likely less a reflection of temperature-driven air–surface exchange and instead indicates that more OPEs enter or are formed in the atmosphere in summer. More research is needed to better understand the atmospheric gas–particle partitioning behaviour of the OPEs and how it may be influenced by transformation reactions.

Atmospheric aerosols are of great climatic and environmental importance due to their effects on the Earth’s radiative energy balance and air quality. Aerosol concentrations are strongly influenced by rainfall via wet removal. Global climate models have been used to quantify their climate and health effects. However, they commonly suffer from a well-known problem of ‘too much light rain and too little heavy rain’. The impact of simulated rainfall intensities on aerosol burden at the global scale is still unclear. Here we show that rainfall intensity has profound impacts on aerosol burden, and light rain has a disproportionate control on it. By improving the representation of convection, the light-rain (1–20 mm d −1 ) frequency in two state-of-the-art global climate models is reduced. As a result, the aerosol burden is increased globally, especially over the tropics and subtropics, by as much as 0.3 in aerosol optical depth in tropical rain belts. It is attributed to the dominant contribution of light rain to the accumulated wet removal by its frequent occurrence despite its weak intensity. The implication of these findings is that understanding the nature of aerosol scavenging by rainfall is critical to aerosol–climate interaction and its impact on climate. Light rain plays a disproportionate role in aerosol wet removal, according to improved simulations on rain intensity and frequency in global climate models.

Aerosols influence the Earth's radiative balance through direct interactions with radiation and by affecting cloud properties. Anthropogenic aerosols have led to cooling during the industrial era through aerosol–cloud interactions (ACI), including aerosol effects on cloud microphysical properties and the subsequent adjustments. However, large uncertainties remain in Earth system models (ESMs) regarding the magnitude of this cooling. In part, ESMs substantially disagree on cloud properties, thermodynamics, the hydrological cycle, and general circulation. Reanalysis provides a useful avenue for exploring the impact of ACI on clouds and radiation because its atmosphere is forced to match realistic conditions through the assimilation of observations. Here, we explore the impact of ACI on clouds in the GiOcean reanalysis – the first to incorporate aerosol-cloud interactions. We contrast variables important for ACI between GiOcean and satellite observations and develop 2-dimensional lookup tables of ACI for both using a source-sink budget perspective to attribute the changes in cloud droplet number (Nd) and liquid water path (LWP) to aerosol and meteorology. A compositing analysis using lookup tables shows that GiOcean captures key aspects of aerosol–cloud–precipitation interactions, including (1) activation of aerosol into cloud droplets, (2) effective precipitation scavenging of Nd, (3) suppression of precipitation by high Nd in regions with heavy aerosol emissions. In contrast, satellite observations do not exhibit clear patterns for processes (2) and (3). Random Forest analysis shows that interannual variability in Nd and LWP over the Northern Hemisphere ocean in GiOcean is primarily driven by precipitation, consistent with satellite observations.

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 µm normalized by the enhancement of carbon monoxide above background (PM2.5/ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December–February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM2.5/ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM2.5/ΔCO was most sensitive to increases in APT up to 5 mm (−0.044 µg m−3 ppbv−1 mm−1) and less sensitive to increases in APT over 5 mm. While anthropogenic PM2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210Pb submicron aerosol tracer and its gaseous precursor 222Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222Rn tracer emissions contribute most to surface 210Pb concentrations at Bermuda in winter (∼ 75 %–80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.

Measurements at high-Arctic sites (Alert, Nunavut, and Mt. Zeppelin, Svalbard) during the years 2011 to 2013 show a strong and similar annual cycle in aerosol number and size distributions. Each year at both sites, the number of aerosols with diameters larger than 20 nm exhibits a minimum in October and two maxima, one in spring associated with a dominant accumulation mode (particles 100 to 500 nm in diameter) and a second in summer associated with a dominant Aitken mode (particles 20 to 100 nm in diameter). Seasonal-mean aerosol effective diameter from measurements ranges from about 180 in summer to 260 nm in winter. This study interprets these annual cycles with the GEOS-Chem-TOMAS global aerosol microphysics model. Important roles are documented for several processes (new-particle formation, coagulation scavenging in clouds, scavenging by precipitation, and transport) in controlling the annual cycle in Arctic aerosol number and size. Our simulations suggest that coagulation scavenging of interstitial aerosols in clouds by aerosols that have activated to form cloud droplets strongly limits the total number of particles with diameters less than 200 nm throughout the year. We find that the minimum in total particle number in October can be explained by diminishing new-particle formation within the Arctic, limited transport of pollution from lower latitudes, and efficient wet removal. Our simulations indicate that the summertime-dominant Aitken mode is associated with efficient wet removal of accumulation-mode aerosols, which limits the condensation sink for condensable vapours. This in turn promotes new-particle formation and growth. The dominant accumulation mode during spring is associated with build up of transported pollution from outside the Arctic coupled with less-efficient wet-removal processes at colder temperatures. We recommend further attention to the key processes of new-particle formation, interstitial coagulation, and wet removal and their delicate interactions and balance in size-resolved aerosol simulations of the Arctic to reduce uncertainties in estimates of aerosol radiative effects on the Arctic climate.

The aerosol particles serving as cloud condensation and ice nuclei contribute to key cloud processes associated with cold-air outbreak (CAO) events but are poorly constrained in climate models due to sparse observations. Here we retrieve aerosol number size distribution modes from measurements at Andenes, Norway, during the Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) and at Zeppelin Observatory, approximately 1000 km upwind from Andenes at Svalbard. During CAO events at Andenes, the sea-spray-mode number concentration is correlated with strong over-ocean winds with a mean of 8±4 cm−3 that is 71 % higher than during non-CAO conditions. Additionally, during CAO events at Andenes, the mean Hoppel minimum diameter is 6 nm smaller than during non-CAO conditions, though the estimated supersaturation is lower, and the mean number concentration of particles that likely activated in-cloud is 109±61 cm−3 with no statistically significant difference from the non-CAO mean of 99±66 cm−3. For CAO trajectories between Zeppelin Observatory and Andenes, the upwind-to-downwind change in number concentration is the largest for the accumulation mode with a mean decrease of 93±95 cm−3, likely attributable primarily to precipitation scavenging. These characteristic properties of aerosol number size distributions during CAO events provide guidance for evaluating CAO aerosol–cloud interaction processes in models.

The interaction between biomass burning aerosols and clouds remains challenging to accurately determine, in part because of difficulties using direct observations to account for influences on aerosol concentrations from precipitation scavenging and dilution due to air mass mixing and separating those signals from source contributions. The prevalence of mixing versus precipitation processes in air laden with biomass burning aerosol (BBA) in the southeast Atlantic lower free troposphere (FT) and marine boundary layer (MBL) is assessed during three observation periods (September 2016, August 2017, and October 2018) during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign. Significant sources of BBAs over the African continent combined with regional circulation patterns result in BBA-laden air flowing from the continent over the southeast Atlantic in the lower FT, then subsiding onto the semi-permanent stratocumulus cloud deck, and entraining into the MBL. This study is broken into two parts, first analyzing hydrologic histories of the BBA air in the lower FT and then carrying out a similar assessment in the underlying MBL. Both analyses leverage joint measurements of water concentration and its heavy isotope ratio, interpreted in the previously established (q, δD) phase space framework. For the lower-FT analysis, in situ observations (water concentration, water isotope ratios) in the lower FT are combined with satellite and Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), global reanalysis data into simple analytical models to constrain hydrologic histories. We find that even simple models are capable of detecting and constraining the primary processes at play, e.g., distinguishing air masses that experienced moist convection and precipitation (likely over the continent) from those that underwent dry convection and turbulent mixing. Regression of the aircraft data onto a simple model of convective detrainment is used to develop a metric of total precipitation for the in situ measurements and then compared to an aerosol metric of black carbon scavenging also derived from the in situ measurements (the ratio of black carbon to carbon monoxide, BC/CO). There is a strong correlation between the two, suggesting black carbon scavenging has been detected and partially quantified, if only in a relative manner. In comparison, weak correlation is found between BC/CO and the total water concentration itself. The above method is expanded to test for entrainment and precipitation influences on BBA concentrations in the MBL. This is more difficult than the FT analysis since signals are subtle and limited by imperfect knowledge of the water and isotope ratios of the entrained air mass at cloud top. For some of the MBLs observed during 2016 and 2018, lower cloud condensation nuclei (CCN) concentrations occur in the sub-cloud layer coincident with isotopic evidence of precipitation, indicating aerosol scavenging, but more complex models are needed to produce definitive conclusions. For the 2017 observation period, with the highest sub-cloud CCN concentrations, there is no connection between precipitation signals and CCN concentrations, likely indicating the importance of different geographic sampling and air mass history in that year. Nonetheless, these findings along with the FT analysis suggest that utilizing isotope ratio signals may be an aid in addressing cloud–aerosol challenges. Especially for the FT case, these findings support the pursuit of more complex models combined with targeted in situ data to constrain BC scavenging coefficients in a manner which can guide model parameterizations, leading to improvements in the accuracy of simulated BC concentrations and lifetimes in climate models.