The 50 most-cited articles in Journal of Geophysical Research Atmospheres, 2021

Abstract A new methodology is developed to construct a global (60°S–60°N) long‐term (2000–2019) high‐resolution (∼10‐km h) mesoscale convective system (MCS) database by tracking MCS jointly using geostationary satellite infrared brightness temperature ( T b ) and precipitation feature (PF) characteristics from the Integrated Multi‐satellitE Retrievals for GPM precipitation data sets. Independent validation shows that the satellite‐based MCS data set is able to reproduce important MCS statistics derived from ground‐based radar network observations in the United States and China. We show that by carefully considering key PF characteristics in addition to T b signatures, the new method significantly improves upon previous T b ‐only methods in detecting MCSs in the midlatitudes for all seasons. Results show that MCSs account for over 50% of annual total rainfall across most of the tropical belt and in selected regions of the midlatitudes, with a strong seasonality over many regions of the globe. The tracking database allows Lagrangian aspects such as MCS lifetime and translational speed…

Abstract The Antarctic ice sheet (AIS) is sensitive to short‐term extreme meteorological events that can leave long‐term impacts on the continent's surface mass balance (SMB). We investigate the impacts of atmospheric rivers (ARs) on the AIS precipitation budget using an AR detection algorithm and a regional climate model (Modèle Atmosphérique Régional) from 1980 to 2018. While ARs and their associated extreme vapor transport are relatively rare events over Antarctic coastal regions (∼3 days per year), they have a significant impact on the precipitation climatology. ARs are responsible for at least 10% of total accumulated snowfall across East Antarctica (localized areas reaching 20%) and a majority of extreme precipitation events. Trends in AR annual frequency since 1980 are observed across parts of AIS, most notably an increasing trend in Dronning Maud Land; however, interannual variability in AR frequency is much larger. This AR behavior appears to drive a significant portion of annual snowfall trends across East Antarctica, while controlling the interannual variability of…

Abstract Drought events occur more frequently under recent climate change. Generally, meteorological drought is the fuse of hydrological drought; thus, it is important to understand the characteristics of meteorological drought and its propagation to hydrological drought for early warning. Taking the Pearl River Basin (PRB) in China as study area, this study adopted K‐means cluster analysis method to divide the PRB into subregions with similar precipitation characteristics. Then, standardized precipitation index and standardized runoff index were used to analyze the characteristics of meteorological drought and hydrological drought, respectively, and the maximum Pearson correlation coefficient was used to determine the drought propagation time (DPT) between these two types of drought. Moreover, the link between meteorological drought and hydrological drought was explored based on continuous wavelet transform and cross wavelet transform. The results revealed that: the PRB has experienced severe meteorological and hydrological droughts since early 2000s, and hydrological drought was…

Abstract We present emission measurements of volatile organic compounds (VOCs) for western U.S. wildland fires made on the NSF/NCAR C‐130 research aircraft during the Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE‐CAN) field campaign in summer 2018. VOCs were measured with complementary instruments onboard the C‐130, including a proton‐transfer‐reaction time‐of‐flight mass spectrometer (PTR‐ToF‐MS) and two gas chromatography (GC)‐based methods. Agreement within combined instrument uncertainties (<60%) was observed for most co‐measured VOCs. GC‐based measurements speciated the isomeric contributions to selected PTR‐ToF‐MS ion masses and generally showed little fire‐to‐fire variation. We report emission ratios (ERs) and emission factors (EFs) for 161 VOCs measured in 31 near‐fire smoke plume transects of 24 specific individual fires sampled in the afternoon when burning conditions are typically most active. Modified combustion efficiency (MCE) ranged from 0.85 to 0.94. The measured campaign‐average total VOC EF was 26.1 ± 6.9 g kg −1 ,…

, secondary organic aerosols SOA) in different parts of the world in response to modified emissions of primary pollutants during the COVID-19 pandemic. We quantify the respective effects of the reductions in NOx and in volatile organic carbon (VOC) emissions, which, in most cases, affect oxidants in opposite ways. Using model simulations, we show that the level of NOx has been reduced by typically 40% in China during February 2020 and by similar amounts in many areas of Europe and North America in mid-March to mid-April 2020, in good agreement with space and surface observations. We show that, relative to a situation in which the emission reductions are ignored and despite the calculated increase in hydroxyl and peroxy radicals, the ozone concentration increased only in a few NOx-saturated regions (northern China, northern Europe, and the US) during the winter months of the pandemic when the titration of this molecule by NOx was reduced. In other regions, where ozone is NOx-controlled, the concentration of ozone decreased. SOA concentrations decrease in response to the concurrent…

Abstract Understanding lowermost stratosphere (LMS) ozone variability is an important topic in the trends and climate assessment communities because of feedbacks among changing temperature, dynamics, and ozone. LMS evaluations are usually based on satellite observations. Free tropospheric (FT) ozone assessments typically rely on profiles from commercial aircraft. Ozonesonde measurements constitute an independent data set encompassing both LMS and FT. We used Southern Hemisphere Additional Ozonesondes (SHADOZ) data (5.8°N–14°S) from 1998 to 2019 in the Goddard Multiple Linear Regression model to analyze monthly mean FT and LMS ozone changes across five well‐distributed tropical sites. Our findings: (a) both FT (5–15 km) and LMS (15–20 km) ozone trends show marked seasonal variability. (b) All stations exhibit FT ozone increases in February‐May (up to 15%/decade) when the frequency of convectively driven waves have changed. (c) After May, monthly ozone changes are both positive and negative, leading to mean trends of +(1–4)%/decade, depending on station. (d) LMS ozone losses reach…

The Atmospheric River (AR) Tracking Method Intercomparison Project (ARTMIP) is a community effort to systematically assess how the uncertainties from AR detectors (ARDTs) impact our scientific understanding of ARs. This study describes the ARTMIP Tier 2 experimental design and initial results using the Coupled Model Intercomparison Project (CMIP) Phases 5 and 6 multi-model ensembles. We show that AR statistics from a given ARDT in CMIP5/6 historical simulations compare remarkably well with the MERRA-2 reanalysis. In CMIP5/6 future simulations, most ARDTs project a global increase in AR frequency, counts, and sizes, especially along the western coastlines of the Pacific and Atlantic oceans. We find that the choice of ARDT is the dominant contributor to the uncertainty in projected AR frequency when compared with model choice. These results imply that new projects investigating future changes in ARs should explicitly consider ARDT uncertainty as a core part of the experimental design.

Abstract Overestimation of precipitation frequency and duration while underestimating intensity, that is, the “drizzling” bias, has been a long‐standing problem of global climate models. Here we explore this issue from the perspective of precipitation partitioning. We found that most models in the Climate Model Intercomparison Project Phase 5 (CMIP5) have high convective‐to‐total precipitation (PC/PR) ratios in low latitudes. Convective precipitation has higher frequency and longer duration but lower intensity than non‐convective precipitation in many models. As a result, the high PC/PR ratio contributes to the “drizzling” bias over low latitudes. The PC/PR ratio and associated “drizzling” bias increase as model resolution coarsens from 0.5° to 2.0°, but the resolution's effect weakens as the grid spacing increases from 2.0° to 3.0°. Some of the CMIP6 models show reduced “drizzling” bias associated with decreased PC/PR ratio. Thus, more reasonable precipitation partitioning, along with finer model resolution should alleviate the “drizzling” bias within current climate models.

Abstract The absorption Ångström exponent (AAE) describes the spectral dependence of light absorption by aerosols. AAE is typically used to differentiate between different aerosol types for example., black carbon, brown carbon, and dust particles. In this study, the variation of AAE was investigated mainly in fresh aerosol emissions from different fuel and combustion types, including emissions from ships, buses, coal‐fired power plants, and residential wood burning. The results were assembled to provide a compendium of AAE values from different emission sources. A dual‐spot aethalometer (AE33) was used in all measurements to obtain the light absorption coefficients at seven wavelengths (370–950 nm). AAE470/950 varied greatly between the different emission sources, ranging from −0.2 ± 0.7 to 3.0 ± 0.8. The correlation between the AAE470/950 and AAE370‐950 results was good (R2 = 0.95) and the mean bias error between these was 0.02. In the ship engine exhaust emissions, the highest AAE470/950 values (up to 2.0 ± 0.1) were observed when high sulfur content heavy fuel oil was used,…

Abstract An observationally constrained time series of historical aerosol effective radiative forcing (ERF) from 1750 to 2019 is developed in this study. We find that the time history of aerosol ERFs diagnosed in CMIP6 models exhibits considerable variation and explore how the time history of aerosol forcing influences the probability distributions of present‐day aerosol forcing and emergent metrics such as climate sensitivity. Using a simple energy balance model, trained on CMIP6 climate models and constrained by observed near‐surface warming and ocean heat uptake, we derive estimates for the historical aerosol forcing. We find 2005–2014 mean aerosol ERF to be −1.1 (−1.8 to −0.5) W m −2 relative to 1750. Assuming recently published historical emissions from fossil fuel and industrial sectors and biomass burning emissions from SSP2‐4.5, aerosol ERF in 2019 is −0.9 (−1.5 to −0.4) W m −2 . There is a modest recovery in aerosol forcing (+0.025 W m −2 decade −1 ) between 1980 and 2014. This analysis also gives a 5%–95% range of equilibrium climate sensitivity of 1.8°C –5.1°C (best…

Abstract Four previously identified patterns of meso‐scale cloud organization in the trades — called Sugar , Gravel , Flowers , and Fish — are studied using long‐term records of ground‐based measurements, satellite observations and reanalyzes. A deep neural network trained to detect these patterns is applied to satellite imagery to identify periods during which a particular pattern is observed over the Barbados Cloud Observatory. Surface‐based remote sensing at the observatory is composited and shows that the patterns can be distinguished by differences in cloud geometry. Variations in total cloudiness among the patterns are dominated by variations in cloud‐top cloudiness. Cloud amount near cloud base varies little. Each pattern is associated with a distinct atmospheric environment whose characteristics are traced back to origins that are not solely within the trades. Sugar air‐masses are characterized by weak winds and of tropical origin. Fish are driven by convergence lines originating from synoptical disturbances. Gravel and Flowers are most native to the trades, but distinguish…

Abstract Controls on pristine aerosol over the Southern Ocean (SO) are critical for constraining the strength of global aerosol indirect forcing. Observations of summertime SO clouds and aerosols in synoptically varied conditions during the 2018 SOCRATES aircraft campaign reveal novel mechanisms influencing pristine aerosol‐cloud interactions. The SO free troposphere (3–6 km) is characterized by widespread, frequent new particle formation events contributing to much larger concentrations (≥1,000 mg −1 ) of condensation nuclei (diameters > 0.01 μm) than in typical sub‐tropical regions. Synoptic‐scale uplift in warm conveyor belts and sub‐polar vortices lifts marine biogenic sulfur‐containing gases to free‐tropospheric environments favorable for generating Aitken‐mode aerosol particles (0.01–0.1 μm). Free‐tropospheric Aitken particles subside into the boundary layer, where they grow in size to dominate the sulfur‐based cloud condensation nuclei (CCN) driving SO cloud droplet number concentrations ( N d ∼ 60–100 cm −3 ). Evidence is presented for a hypothesized Aitken ‐ buffering…

Abstract Coupled Model Intercomparison Project Phase 6 (CMIP6) models are analyzed using an established cloud clustering methodology. This enables a comparison of cloud representation in models and observations. The simulation of stratocumulus clouds over the Southern Ocean is shown to have changed substantially from earlier generation models. The CMIP6 models analyzed show stratocumulus clouds now occur more often in simulations than in International Satellite Cloud Climatology Project (ISCCP) observations, but are not bright enough compared to Clouds and the Earth's Radiant Energy System (CERES) data. This is in contrast to the “too few, too bright” problem, which has characterized prior model simulations of stratocumulus clouds, particularly over the Southern Ocean. The cloud clusters also enable the calculation of mean and compensating shortwave cloud radiative effect (SW CRE) errors from model data. The compensating errors are shown to be much larger than mean errors suggesting the CMIP6 models still have much to improve in their cloud representation. A statistically…

Abstract This paper describes and evaluates physical parameterizations accounting for the effect of rooftop mitigation strategies (RMSs) on the urban environment, in the context of the mesoscale model Weather Research and Forecasting (WRF). Through the new implementation, the sensitivity of near‐surface air temperature and building energy consumption to different RMSs is evaluated by means of numerical simulations in idealized urban areas, for typical summer and winter conditions. Rooftop mitigation strategies considered include cool roofs, green roofs, and rooftop photovoltaic panels. The reference case simulations are performed assuming buildings made by bricks, with roof composed of clay tiles. Results indicate that near‐surface air temperature is reduced by cool and green roofs during summer: cool roofs are the most efficient in decreasing air temperature, followed by irrigated green roofs. Photovoltaic panels, instead, induce a temperature increase during daytime and a small decrease during nighttime. Cool roofs reveal to be the most efficient strategy in reducing the energy…

Abstract Methanol is the second‐most abundant organic gas in the remote atmosphere after methane, but its sources are poorly understood. Here, we report a global budget of methanol constrained by observations from the ATom aircraft campaign as implemented in the GEOS‐Chem global atmospheric chemistry model. ATom observations under background marine conditions can be fit in the model with a surface ocean methanol concentration of 61 nM and a methanol yield of 13% from the newly implemented CH 3 O 2 + OH reaction. While terrestrial biogenic emissions dominate the global atmospheric methanol budget, secondary production from CH 3 O 2 + OH and CH 3 O 2 + CH 3 O 2 accounts for 29% of the total methanol source, and makes up the majority of methanol in the background marine atmosphere sampled by ATom. Net emission from the ocean is comparatively minor, particularly because of rapid deposition from the marine boundary layer. Aged anthropogenic and pyrogenic plumes sampled in ATom featured large methanol enhancements to constrain the corresponding sources. Methanol enhancements in pyrogenic…

Abstract In this study, we applied a cyclone tracking algorithm to multiple reanalyses and categorized the detected cyclones based on season, intensity, and sea ice state to provide an Arctic cyclone climatology with emphasis on cyclone‐sea ice interactions over the Arctic Ocean and adjacent waters. Our study period is from 1979 to 2015 and the reanalyses we are using are ERA‐Interim, ERA5, and CFSR. As for our intensity variable, we use Accumulated Cyclone Energy (ACE), which has commonly been used as an intensity metric in the tropics but has not been utilized for high latitudes before. ACE has the advantage that it relates the cyclone intensity to the kinetic energy of the cyclone and therefore better represents the cyclone impact/interaction with the surface. We performed comparisons with the other more commonly used intensity metrics to assess the use of the ACE metric in the Arctic. Our main findings include increased cyclone counts with higher trends toward the end of the study period. Cold season cyclone counts were also found to be related to decreased sea ice concentration…

Abstract A comprehensive record (WHV2020) of explosive volcanic eruptions in the last 11,000 years is reconstructed from the West Antarctica Ice Sheet Divide deep ice core (WDC). The chronological list of 426 large volcanic eruptions in the Southern Hemisphere and the low latitudes during the Holocene are of the highest quality of all volcanic records from ice cores, owing to the high‐resolution chemical measurement of the ice core and the exceptionally accurate WDC timescale. No apparent trend is found in the frequency (number of eruptions per millennium) of volcanic eruptions, and the number of eruptions in the most recent millennium (1,000–2,000 CE) is only slightly higher than the average in the last 11 millennia. The atmospheric aerosol mass loading of climate‐impacting sulfur, estimated from measured volcanic sulfate deposition, is dominated by explosive eruptions with extraordinarily high sulfur mass loading. Signals of three major volcanic eruptions are detected in the second half of the 17th century (1700–1600) BCE when the Thera volcano in the eastern Mediterranean was…

Abstract Particulate air pollution is one of the most important environmental issues confronting China, especially in northern cities during winter. The Fenwei Plain has been designated as one of the three key regions for air pollution control, replacing the Pearl River Delta (PRD) region in 2018. On average, the annual mass concentrations of PM2.5, PM10, SO2, and NO2 in the Fenwei Plain were the highest of the three key regions, which also include the Beijing‐Tianjin‐Hebei (BTH) region (the “2 + 26” region) and the Yangtze River Delta (YRD). In terms of major air pollutants, PM2.5, PM10, SO2, and NO2 at 11 typical cities in the Fenwei Plain exceeded the second level of Chinese National Ambient Air Quality Standards, most often in winter. Here, the characteristics of airborne particulate matter in the Fenwei Plain are presented, and source apportionments for PM2.5 and PM2.5 as associated chemical species are reviewed. The causes of severe particulate matter air pollution during wintertime in this region are summarized, and several recommendations for improving local air quality are…

Abstract The limited number of nitrogen dioxide (NO 2 ) surface measurements calls for the development of highly accurate approaches to estimating surface NO 2 concentrations. In this study, we leverage a new satellite instrument, the TROPOspheric Monitoring Instrument (TROPOMI), along with other predictor variables, to estimate daily surface NO 2 concentrations over Texas in 2019. We use the deep convolutional neural network (Deep‐CNN), an advanced deep learning algorithm, to obtain estimates and achieve a correlation coefficient ( R ) of 0.91, an index of agreement (IOA) of 0.95, and a mean absolute bias (MAB) of 1.75 ppb in surface NO 2 estimation. Additionally, we leverage a novel approach, shapley additive explanations (SHAP), to describe how Deep‐CNN understands each predictor variable. The SHAP results show that the Deep‐CNN model has an advanced understanding of the data set, revealing that TROPOMI closely captures levels of NO 2 . In addition, we show the superiority of our Deep‐CNN model at estimating surface NO 2 over other well‐known machine learning and regression…

Abstract Deliberately blocking out a small portion of the incoming solar radiation would cool the climate. One such approach would be injecting SO 2 into the stratosphere, which would produce sulfate aerosols that would remain in the atmosphere for 1–3 years, reflecting part of the incoming shortwave radiation. The cooling produced by the aerosols can offset the warming produced by increased greenhouse gas (GHG) concentrations, but it would also affect the climate differently, leading to residual differences compared to a climate not affected by either. Many climate model simulations of geoengineering have used a uniform reduction of the incoming solar radiation as a proxy for stratospheric aerosols, both because many models are not designed to adequately capture relevant stratospheric aerosol processes, and because a solar reduction has often been assumed to capture the most important differences between how stratospheric aerosols and GHG would affect the climate. Here we show that dimming the sun does not produce the same surface climate effects as simulating aerosols in the…

Abstract Surface processes in high latitudes play an important role in global climate and thus understanding the physics of these systems is critical for improving climate projections. The characterization of the stable water isotopologue flux between the surface and the atmosphere offers the potential to constrain parameterizations of these physical surface exchange processes in numerical models. In addition, observations of isotopologue surface fluxes allow the evaluation of surface fluxes as a process influencing the formation of the climate signal retrieved from ice core isotopologue records. Here, we present a record of stable water isotopologue surface fluxes measured in‐situ in the accumulation zone of the Greenland Ice Sheet at the East Greenland Ice Core Project site. We measured isotopologue fluxes above the snow surface directly by combining high‐frequency eddy covariance measurements with low‐frequency isotopologue measurements from a cavity ring‐down spectrometer (CRDS). We developed a method to correct for the high‐frequency loss of the CRDS by combining humidity…

Abstract To investigate the chemical compositions, sources, and aging processes of submicron particles (PM1), a comprehensive field campaign was conducted in Guangzhou urban area of China during the autumn (October–November) of 2018. The average mass concentration of PM1 was 35.6 ± 20.8 µg m−3, which was mainly contributed by organic aerosols (OA, 42%), then followed by sulfate (25%) and inorganic nitrate (11%). The inorganic nitrate was found to be the main driving component (up to ∼50%) to account for the fast increase of PM1 during the polluted periods of Guangzhou autumn. The promotion effects of sulfate, aerosol liquid water content, and particles acidity on nitrate formation were systematically discussed. Source apportionment results showed 72% of OA in Guangzhou autumn was contributed by secondary OA (SOA), and 28% of primary OA (POA), including vehicle emission related hydrocarbon‐like OA (HOA, 16%), nitrogen‐containing OA (NOA, 3%) and cooking OA (COA, 8%). To explore the aging processes of OA, the dynamic variations of OA and its oxidation level as a function of ambient…

Abstract The Western North Atlantic Ocean (WNAO) is a complex land‐ocean‐atmosphere system that experiences a broad range of atmospheric phenomena, which in turn drive unique aerosol transport pathways, cloud morphologies, and boundary layer variability. This work, Part 2 of a 2‐part paper series, provides an overview of the atmospheric circulation, boundary layer variability, three‐dimensional cloud structure, and precipitation over the WNAO; the companion paper (Part 1) focused on chemical characterization of aerosols, gases, and wet deposition. Seasonal changes in atmospheric circulation and sea surface temperature explain a clear transition in cloud morphologies from small shallow cumulus clouds, convective clouds, and tropical storms in summer, to stratus/stratocumulus and multilayer cloud systems associated with winter storms. Synoptic variability in cloud fields is estimated using satellite‐based weather states, and the role of postfrontal conditions (cold‐air outbreaks) in the development of stratiform clouds is further analyzed. Precipitation is persistent over the ocean,…

Abstract Aerosol deposition is a major source of soluble Fe in open oceans, affecting marine biogeochemistry and primary production. However, Fe fractional solubility, a key parameter in estimating deposition fluxes of soluble aerosol Fe, is still highly uncertain. Abundance and fractional solubility of aerosol Fe in fine (<1 μm) and coarse (>1 μm) particles was measured at Qingdao (a coastal city in northern China) in November‐December 2019. Average concentrations of total and soluble Fe were found to be 798 ± 466 and 7.7 ± 14.5 ng/m3 in coarse particles, and 801 ± 534 and 7.3 ± 7.6 ng/m3 in fine particles. Fe solubility was significantly lower in coarse particles (average: 0.80 ± 1.03%) than fine particles (average 1.29 ± 1.41%). Compared to clean days, total Fe concentration was substantially increased during dust and haze days; however, Fe solubility was significantly reduced in dust days and elevated in haze days. Acid processing significantly enhanced Fe solubility in both fine and coarse particles, and the contribution of primary emission to Fe solubility enhancement was…

Abstract Wildfires in the western United States are large sources of particulate matter, and the area burned by wildfires is predicted to increase in the future. Some particles released from wildfires can affect cloud formation by serving as ice‐nucleating particles (INPs). INPs have numerous impacts on cloud radiative properties and precipitation development. Wildfires are potentially important sources of INPs, as indicated from previous measurements, but their abundance in the free troposphere has not been quantified. The Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen campaign sampled free tropospheric immersion‐freezing INPs from smoke plumes near their source and downwind, along with widespread aged smoke. The results indicate an enhancement of INPs in smoke plumes relative to out‐of‐plume background air, but the magnitude of enhancement was both temperature and fire dependent. The majority of INPs were inferred to be predominately organic in composition with some contribution from biological sources at modest super cooling, and contributions…

Abstract Here, we present a multi‐season study of ice‐nucleating particles (INPs) active via the immersion freezing mechanism, which took place in north‐central Argentina, a worldwide hotspot for mesoscale convective storms. INPs were measured untreated, after heating to 95°C, and after hydrogen peroxide digestion. No seasonal cycle of INP concentrations was observed. Heat labile INPs, which we define as “biological” herein, dominated the population active at −5 to −20°C, while non‐heat‐labile organic INPs (decomposed by peroxide) dominated at lower temperatures, from −20 to −28°C. Inorganic INPs (remaining after peroxide digestion), were minor contributors to the overall INP activity. Biological INP concentration active around −12°C peaked during rain events and under high relative humidity, reflecting emission mechanisms independent of the background aerosol concentration. The ratio of non‐heat‐labile organic and inorganic INPs was generally constant, suggesting they originated from the same source, presumably from regional arable topsoil based on air mass histories. Single…

Abstract According to atmospheric modeling and satellite observations, cold fronts can cause trans‐regional transport (TRT) of haze particles from the North China Plain (NCP) to Yangtze River Delta (YRD) in winter. However, compositions and aging of haze aerosols during the TRT have not been studied. We showed the TRT PM2.5 dominated by organic matter (OM) (30%) and secondary inorganic ions (36%) in the NCP and 29% and 60% in the YRD. Following the TRT, abundant spherical primary OM particles (i.e., tarballs) (71% by number) mainly from residential coal burning in rural areas of the NCP unexpectedly occurred in the YRD. The inert tarballs display similar sizes (∼300 nm) and O/C ratios (∼0.15), but the mixture of nitrate, sulfate, and secondary OM as the coatings completely convert the hydrophobic tarballs into hydrophilic ones in the TRT. The aging and transport of tarballs from the NCP to YRD further indicate that the TRT not only brought various trace gases (e.g., CO, SO2, NOx, and VOCs) but also carried large numbers of nanosized primary particles (e.g., tarball, metal, fly ash,…

The Western North Atlantic Ocean (WNAO) and adjoining East Coast of North America are of great importance for atmospheric research and have been extensively studied for several decades. This broad region exhibits complex meteorological features and a wide range of conditions associated with gas and particulate species from many sources regionally and other continents. As Part 1 of a 2-part paper series, this work characterizes quantities associated with atmospheric chemistry, including gases, aerosols, and wet deposition, by analyzing available satellite observations, ground-based data, model simulations, and reanalysis products. Part 2 provides insight into the atmospheric circulation, boundary layer variability, three-dimensional cloud structure, properties, and precipitation over the WNAO domain. Key results include spatial and seasonal differences in composition along the North American East Coast and over the WNAO associated with varying sources of smoke and dust and meteorological drivers such as temperature, moisture, and precipitation. Spatial and seasonal variations of…

Abstract Currently available evapotranspiration (ET) products have not provided us with an accurate estimation for global irrigated land area. Thermal energy balance (EB) model has the potential to solve this problem. The accurate estimation of aerodynamic resistances is a major complication in most remote sensing ET models. An EB model using a column canopy‐air turbulent heat diffusion method was developed to more realistically depict dynamic changes in aerodynamic resistance. In order to estimate global ET and land surface fluxes for all weather conditions, Moderate Resolution Imaging Spectroradiometer (MODIS) Aqua and Terra land surface temperature fields were combined and a nearest‐evaporative‐fraction gap‐filling method was merged into the EB model. A global ET product covering the period 2003–2017 was produced using the EB model. By combining thermal and optional information from MODIS satellites and surface meteorological forcing data from ERA‐Interim reanalysis data, the EB model provides a 5 × 5 km resolution estimate of daily ET without spatio‐temporal gaps at the global…

Abstract Regional ozone (O3) pollution is influenced by a combination of anthropogenic sources and biogenic volatile organic compounds (BVOC) emitted from vegetation. Under the influence of warming climate and projected expansion of urban green space, O3 pollution may get worse, especially during heat waves (HWs). However, HW‐induced changes in BVOC and subsequent effects on regional O3 pollution have not been adequately assessed. In this study, we used the Weather Research and Forecasting‐Community Multi‐scale Air Quality models to investigate the formation of a typical O3 episode and quantify the O3 response to BVOC in the Pearl River Delta during a HW in 2017. The results showed that the rate of increase of O3 during the HW was 27.1 µg m−3 °C−1, reflecting the rapid O3 formation under high temperature. Compared with the non‐HW (NHW), gas‐phase chemistry and vertical transport were dominant contributors to O3 formation. Sensitivity experiments indicate that the contribution of BVOC to ground‐level O3 formation in Pearl River Delta was up to 42.1 μg m−3 because BVOC emissions in HW…

Abstract Here, we define weather regimes in the East Antarctica—Southern Ocean sector based on daily anomalies of 700 hPa geopotential height derived from ERA5 reanalysis during 1979–2018. Most regimes and their preferred transitions depict synoptic‐scale disturbances propagating eastwards off the Antarctic coastline. While regime sequences are generally short, their interannual variability is strongly driven by the polarity of the Southern Annular Mode (SAM). Regime occurrences are then intersected with atmospheric rivers (ARs) detected over the same region and period. ARs are equiprobable throughout the year, but clearly concentrate during regimes associated with a strong atmospheric ridges/blockings on the eastern part of the domain, which act to channel meridional advection of heat and moisture from the lower latitudes towards Antarctica. Both regimes and ARs significantly shape climate variability in Antarctica. Regimes favorable to AR occurrences are associated with anomalously warm and humid conditions in coastal Antarctica and, to a lesser extent, the hinterland parts of the…

Abstract Studies of wintertime air quality in the North China Plain (NCP) show that particulate‐nitrate pollution persists despite rapid reduction in NOx emissions. This intriguing NOx‐nitrate relationship may originate from non‐linear nitrate‐formation chemistry, but it is unclear which feedback mechanisms dominate in NCP. In this study, we re‐interpret the wintertime observations of 17O excess of nitrate (∆17O(NO3−)) in Beijing using the GEOS‐Chem (GC) chemical transport model to estimate the importance of various nitrate‐production pathways and how their contributions change with the intensity of haze events. We also analyze the relationships between other metrics of NOy chemistry and [PM2.5] in observations and model simulations. We find that the model on average has a negative bias of −0.9‰ and −36% for ∆17O(NO3−) and [Ox,major] (≡ [O3] + [NO2] + [p‐NO3−]), respectively, while overestimating the nitrogen oxidation ratio ([NO3−]/([NO3−] + [NO2])) by +0.12 in intense haze. The discrepancies become larger in more intense haze. We attribute the model biases to an overestimate of…

Abstract As the buffer layer between the atmosphere and permafrost, the active layer is vulnerable to climate change. The variation in the active layer thickness (ALT) has important effects on surface energy balance, ecosystem, hydrological cycle, vegetation cover, and engineering construction in permafrost regions. The goal of this study is to discuss the active layer variation under different shared socioeconomic pathways (SSPs) for specific warming levels and to reveal the potential interactions between the ALT and the associated driving factors in typical hydrological basins. We revised the Stefan solution using the edaphic factor and the thawing index calculated by multimodel data from the Coupled Model Intercomparison Project Phase 6 to estimate the variation in the ALT. During 2015 to 2100, the ALT will increase by 14 cm (SSP1‐2.6), 43 cm (SSP2‐4.5), and 1.44 m (SSP5‐8.5), with average increase rates of 2.5 cm/decade, 5.8 cm/decade, and 17.5 cm/decade, respectively. The rates of increase of the ALT in the Hexi basin, Inner basin, Mekong basin, Yangtze basin, and Yellow basin…

Abstract During summer, the Southern Ocean is largely unaffected by anthropogenic emissions, which makes this region an ideal place to investigate marine natural aerosol sources and processes. A better understanding of natural aerosol is key to constrain the preindustrial aerosol state and reduce the aerosol radiative forcing uncertainty in global climate models. We report the concentrations of gaseous sulfuric acid, iodic acid, and methanesulfonic acid (MSA) together with a characterization of new particle formation (NPF) events over a large stretch of the Southern Ocean. Measurements were conducted on board the Russian icebreaker Akademik Tryoshnikov from January to March 2017. Iodic acid is characterized by a particular diurnal cycle with reduced concentration around noon, suggesting a lower formation yield when solar irradiance is higher. Gaseous MSA does not have a diurnal cycle and measured concentrations in gas and condensed phase are compatible with this species being primarily produced via heterogeneous oxidation of dimethyl sulfide and subsequent partitioning into the gas…

Abstract Atmospheric river (AR) and its impact on monsoon rainfall in East Asia are investigated by considering their month‐to‐month variations during the East Asian summer monsoon (EASM). The AR in the EASM, defined as an anomalously enhanced plume‐like water vapor transport, frequently forms over eastern China, Korea and western Japan. However, its characteristics vary from the early (June‐July) to the late (August‐September) period of the EASM. In the early EASM, AR is typically characterized by a quasi‐stationary monsoon southwesterly along the northern boundary of the western North Pacific subtropical high (WNPSH), which is further intensified by a migrating extratropical cyclone in the north. In contrast, the late‐EASM AR, which is less frequent than the early EASM AR, is primarily organized by a migrating extratropical cyclone. The quasi‐stationary monsoon southwesterly is less influential as the northern boundary of the WNPSH shifts northward, being decoupled from the subtropical ocean. Both the early‐ and late‐EASM ARs contribute substantially to monsoon rainfall,…

Abstract Black carbon (BC) aerosols strongly absorb the solar radiation, affecting the regional and global climate through direct and indirect radiative forcing. The optical properties of BC are critical factors to estimate their radiative forcing. However, the optical absorption of BC is still under controversy partially due to the weakness in quantifying their complex morphology and mixing structures. Although a Discrete Dipole Approximation (DDA) can calculate optical properties of fine particles with arbitrary shapes, an appropriate definition of realistic BC shape models for optical simulation is essentially required. Here we present a novel Electron‐Microscope‐to‐BC‐Simulation (EMBS) tool to construct realistic BC shape models with various morphology and mixing structures for optical calculation using DDA. The optical properties of BC particles with different particle morphology, coating thickness, and embedded fraction (F) are estimated based on electron microscope. We find that absorption enhancement (Eabs) of the realistic irregular model is larger than that of the present…

Abstract We present a new version of the HIgh Altitude Mechanistic general Circulation Model (HIAMCM) with specified dynamics. We utilize a spectral method that nudges only the large‐scale flow to MERRA‐2 reanalysis. The nudged HIAMCM simulates gravity waves (GWs) down to horizontal wavelengths of about 200 km from the troposphere to the thermosphere like the free‐running model, including the generation of secondary and tertiary GWs. Case studies show that the simulated large‐scale GWs are consistent with those in the reanalysis, while the medium‐scale GWs compare well with observations in the northern winter 2016 stratosphere from the Atmospheric InfraRed Sounder (AIRS). GWs having wavelengths larger than about 1,350 km can be described with the nonlinear balance equation. The GWs relevant in the stratosphere, however, have smaller scales and require a different approach. We propose that the GW amplification due to kinetic energy transfer from the large‐scale flow combined with GW potential energy flux convergence helps to identify the mesoscale GW sources due to spontaneous…

Abstract Understanding of groundwater recharge and associated hydrological processes is important for sustainable management and utilization of water resources, especially in the monsoon regions. However, few systematic studies have been conducted on the spatiotemporal variation of groundwater recharge. In this study, stable isotopes of precipitation and groundwater were used to explore the spatiotemporal variation of groundwater recharge in the lower reaches of the Poyang Lake Basin of China, a region affected by the interplay of different monsoons. The results indicated that isotopic values (δ2H and δ18O) of precipitation exhibited obvious seasonal variations, higher in winter and lower in summer, controlled by different monsoons. The stable isotopes of groundwater also presented distinct seasonal variations, revealing the dominant influence of seasonal precipitation, but they had different characteristics in space. In the northern study area and Rao and Xin Basins, the isotopic signatures of groundwater showed the shift to lower values in summer and higher values in winter,…

Abstract Urban areas generally have higher near‐surface air temperature and lower air humidity than rural areas. Little is known about how heat stress, the combined effect of high air temperature and high humidity on human physiology, will be affected by future urban land expansion. Here we use a mesoscale numerical weather prediction model to examine the effects of urban land expansion from 2000 to 2050 on heat stress (measured as wet‐bulb globe temperature, WBGT) in the urban areas of China, India, and Nigeria, which are projected to account for one‐third of global urban population growth through 2050. Our results show that urban expansion slightly reduces heat stress during the day (∼0.2°C) but substantially intensifies it at night, by ∼1°C on average and by up to 2–3°C in five mega‐urban regions (MURs). These effects exist with or without climate change induced by rising concentrations of greenhouse gases (GHGs). Installing cool roofs—an urban heat island mitigation measures—can reduce the daytime WBGT by 0.5–1°C, partially offsetting the heat stress conditions caused by…

Abstract Climate models exhibit major radiative biases over the Southern Ocean owing to a poor representation of mixed‐phase clouds. This study uses the remote‐sensing dataset from the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean (MARCUS) campaign to assess the ability of the Weather Research and Forecasting (WRF) model to reproduce frontal clouds off Antarctica. It focuses on the modeling of thin mid‐level supercooled liquid water layers which precipitate ice. The standard version of WRF produces almost fully glaciated clouds and cannot reproduce cloud top turbulence. Our work demonstrates the importance of adapting the ice nucleation parameterization to the pristine austral atmosphere to reproduce the supercooled liquid layers. Once simulated, droplets significantly impact the cloud radiative effect by increasing downwelling longwave fluxes and decreasing downwelling shortwave fluxes at the surface. The net radiative effect is a warming of snow and ice covered surfaces and a cooling of the ocean. Despite improvements in our simulations, the local…

Abstract Biomass burning (BB) produces large quantities of carbonaceous aerosol (black carbon and organic aerosol, BC and OA, respectively), which significantly degrade air quality and impact climate. BC absorbs radiation, warming the atmosphere, while OA typically scatters radiation, leading to cooling. However, some OA, termed brown carbon (BrC), also absorbs visible and near UV radiation; although, its properties are not well constrained. We explore three aircraft campaigns from important BB regions with different dominant fuel and fire types (Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen [WE‐CAN] in the western United States and ObseRvations of Aerosols above CLouds and their intEractionS and Cloud‐Aerosol‐Radiation Interactions and Forcing for Year downwind of southern Africa) and compare them with simulations from the global chemical transport model, GEOS‐Chem using GFED4s. The model generally captures the observed vertical profiles of carbonaceous BB aerosol concentrations; however, we find that BB BC emissions are underestimated in…

Abstract Tropical gravity wave activity is investigated using measurements of momentum fluxes gathered during Strateole‐2 superpressure balloon flights. The data set consists of eight balloon flights performed in the deep tropics from November 2019 to February 2020. The flights lasted for 2–3 months each, and in‐situ meteorological data were collected every 30 s. The relation between gravity waves and deep convection is investigated using geostationary satellite data from the NOAA/NCEP GPM_MERGIR satellite data product, at 1 h resolution. The amplitude of gravity wave momentum fluxes shows a clear dependence on the distance to the nearest convective system, with a strong decay as distance to convection increases. The largest momentum‐flux values (> mPa) are only found less than 200 km away from deep convection. The sensitivity of the wave flux to distance from convection is stronger for high frequency gravity waves (periods shorter than 60 min). Lower frequency waves tend to a non‐zero, background value away from convection, supporting some background value in gravity‐wave drag…

Abstract As one of the aridest regions in the mid‐latitudes, arid Northwest China (ANC) has scarce water resources year‐round, its annual total precipitation is mainly contributed by summer extreme precipitation events, which may also cause disastrous flash floods. However, the physical mechanism and climatic features of extreme precipitation events in ANC are not fully understood and warrant in‐depth investigations. Taking Xinjiang as an example, this study investigates the underlying mechanisms and long‐term trend of extreme precipitation events in ANC during 1961–2019 using observational and reanalysis data sets. Results suggest that summer extreme precipitation events in ANC are characterized by a zonal wave pattern with the deepening of the western Siberian trough, central Asian high, and Mongolian high. Under the effects of the zonal wave pattern, the westerly and the easterly airflows anomalously intensify and converge in ANC, transporting a large amount of water vapor from the Arctic Ocean, the Caspian Sea, the Aral Sea, the Arabian Sea, and eastern China to ANC. Meanwhile,…

Abstract Mesoscale convective systems (MCSs) have been identified as an important source of precipitation in the Tibetan Plateau (TP) region. However, the characteristics and structure of MCS‐induced precipitation are not well understood in this location. Infrared (IR) satellite imagery has been used for MCS tracking, but cirrus clouds or cold surfaces can lead to false MCS classification over mountain regions. Here, we combine brightness temperatures from IR imagery with satellite precipitation estimates from GPM IMERG and track MCSs over the TP, at the boundary of the TP (TPB), and in the surrounding lower‐elevation plains (LE), between 2000 and 2019. In most parts of LE and TPB, MCSs produced 50%–80% of the total summer precipitation (60%–90% of summer heavy precipitation), whereas MCSs over the TP account for below 10% of the total summer precipitation (10%–30% of summer heavy precipitation). Our results also show that MCSs that produce the largest amounts of heavy precipitation are characterized by longevity and large extents rather than by high intensities. These are mainly…

Abstract Volcanic explosions are the most critical replenishing mechanism of the stratospheric aerosol Junge layer. A fresh volcanic cloud comprises mostly sulfur‐bearing gases, volcanic ash, and water vapor. It is commonly assumed that only sulfate aerosols remain in an aged volcanic cloud. Accurate simulation of the initial evolution of multicomponent fresh volcanic clouds is largely missing due to insufficient spatial resolution and a lack of relevant physics in global climate models. However, this initial stage is essential, as the vertical structure, composition, and altitude of a freshly developed volcanic cloud affect its long‐term evolution. To fill this gap, we modified a regional WRF‐Chem model to study the dispersion of a Pinatubo‐size volcanic cloud in the equatorial belt with a 25 km grid spacing explicitly accounting for the SO 2 , ash, sulfate, water vapor, and hydrometeors radiative effects. The model best reproduces the observed evolution of the Pinatubo optical depth when eruptive products are injected above the cold tropical tropopause at 17 km. During the first…

Abstract The first inventory of dust emission sources in Central Asia and northwestern China (35–50°N, 50–100°E) derived from the twice daily MODIS imagery from 2003 to 2012 is presented. A high‐resolution (1 km) dust enhancement product was generated to produce maps of dust point sources (DPS), indicating geographical locations of the observed dust emissions, and gridded data sets of dust emission frequencies. About 13,500 DPS were detected over an area of ∼5 × 106 km2, however, their distribution was uneven. The highest frequency of DPS occurred in the northern and eastern Taklimakan, in the Aralkum, and in the regions, which were not widely reported in literature before, the Balkh delta in northern Afghanistan and the pre‐Aral, from the northern Caspian coast to the Betpak‐Dala desert in Kazakhstan. South of the Aral, DPS were mainly associated with fluvial features: drying lakes, dry river beds, alluvial deposits and agricultural activity which is closely linked to water availability in this arid region. In the pre‐Aral and Balkhash‐Junggar regions, land damaged by wildfire was…

Abstract The major fraction of intermediate and semi‐volatility organic compounds (I/SVOCs) is still unresolved by traditional analyses, leaving large unresolved complex mixture (UCM) and limiting the estimation of secondary organic aerosol (SOA). This study addressed the UCM by employing two‐dimensional gas chromatography−time‐of‐flight mass spectrometry. The ratios of UCM in I/SVOCs emitted from household burning of biomass and coal were reduced to 1.0 ± 0.3% and 2.1 ± 2.0%, respectively, and these levels are one order of magnitude less than those reported in previous studies. Phenols, polycyclic aromatic hydrocarbons, and ketones made the major contribution to I/SVOCs emission factors (EFs) (65.9 ± 9.6%) for biomass burning, while amides, acids, and esters constituted the majority of EFs (56.5 ± 45.0%) for coal burning. Furthermore, SOA production can be predicted via the highly identified I/SVOCs compounds based on volatility distributions of each speciated species. These majority compounds contribute the predicted SOA production with 76.0 ± 12.7% and 82.0 ± 60.3% for biomass…

Abstract California has experienced more wildfires in recent years, resulting in huge economic losses and threatening human health. Clarifying the meteorological environments of wildfires is foundational to improving the understanding and prediction of wildfires and their impacts. Here, 1,535 California wildfires during 1984–2017 are systematically investigated. Based on two key meteorological factors—temperature and moisture anomalies—all wildfires are classified into four groups: hot‐dry, hot‐wet, cold‐dry, cold‐wet. Most (∼60%) wildfires occurred on hot‐dry days. Compositing the meteorological environments of the four groups shows that persistent high pressure and strong northeasterly wind descending from inland favor hot‐dry conditions for wildfires. Self‐organizing map analysis lends confidence in the large‐scale meteorological pattern dominating hot‐dry wildfires in California. Meteorological anomalies also influence wildfire size through their magnitudes, with moisture anomaly explaining the largest fraction (∼69%) of variability in wildfire sizes. In addition, 12.2% of…

Abstract Agricultural emissions of ammonia (NH 3 ) impact air quality, human health, and the vitality of aquatic and terrestrial ecosystems. In the UK, there are few direct policies regulating anthropogenic NH 3 emissions and development of sustainable mitigation measures necessitates reliable emissions estimates. Here, we use observations of column densities of NH 3 from two space‐based sensors (IASI and CrIS) with the GEOS‐Chem model to derive top‐down NH 3 emissions for the UK at fine spatial (∼10 km) and time (monthly) scales. We focus on March‐September when there is adequate spectral signal to reliably retrieve NH 3 . We estimate total emissions of 272 Gg from IASI and 389 Gg from CrIS. Bottom‐up emissions are 27% less than IASI and 49% less than CrIS. There are also differences in seasonality. Top‐down and bottom‐up emissions agree on a spring April peak due to fertilizer and manure application, but there is also a comparable summer July peak in the top‐down emissions that is not in the bottom‐up emissions and appears to be associated with dairy cattle farming. We estimate…

Abstract Brown Carbon (BrC) absorbs light in wavelength of 300–400 nm, and BrC molecule (BrCM) is a fundamental component responsible for aerosol radiative forcing. In this study, Fourier‐transform ion cyclotron resonance mass spectrometry (FT‐ICR MS) coupled with electrospray ionization (ESI) was used to determine methanol extracted BrCM in PM 2.5 collected in Xi'an, China. The absorption of individual BrCM was quantified through partial least square regression (PLSR) method. Results showed that 77.5% and 91.8% of winter and summer BrCMs were weak absorptive. The top BrCMs were responsible for 60.4% and 84.6%, respectively, of the absorbances in summer and winter. The nitrogen (N)‐containing organic molecules were identified to be critical components of light‐absorbing matters in both of the two seasons, outlining the significance of N chromogenesis in BrC. The top BrCMs were more closely related to ‐(O)NO 2 that originated from NO 2 engaged reactions in winter, and to ‐NH that formed in NH 3 reactions in summer. Sulfur (S)‐containing functional groups were not chromophoric while…