Atmospheric Transport Research Articles

Heavy Metals in Surface Sediment of Plateau Lakes in Tibet, China: Occurrence, Risk Assessment, and Potential Sources.

Tibetan Plateau lakes have high ecological value and play a crucial role in maintaining ecological balance. This research aimed to study the pollution characteristics, ecological risk, and potential sources of eight heavy metals (As, Cd, Cr, Cu, Hg, Ni, Pb, and Zn) in the surface sediments of 12 Tibetan Plateau lakes. The results of the toxicity risk index (TRI) showed that only Gongzhu Tso (28.09) and La' ang Tso (20.25) had heavy metals that could pose a very high risk of toxicity to aquatic organisms. Hg posed the highest potential ecological risk to aquatic organisms. Based on the results of multiple analyses, we inferred that the contents of Cr, Cu, Hg, and Ni in sediments of Tibetan lakes were influenced by industrial and agricultural development; Cd, Pb, and Zn were influenced by transport and atmospheric transport; and As was derived from geothermal activity and rock weathering.

Distributions of PAHs, NPAHs, OPAHs, BrPAHs, and ClPAHs in air, bulk deposition, soil, and water in the Shandong Peninsula, China: Urban-rural gradient, interface exchange, and long-range transport

A systematic study of the movement of PAHs (Polycyclic aromatic hydrocarbons) and their derivatives through air, soil, and water is key to understanding the exchange and transport mechanisms of these pollutants in the environment and for ultimately improving environmental quality. PAHs and their derivatives, such as nitrated PAHs (NPAHs), oxygenated PAHs (OPAHs), brominated PAHs (BrPAHs) and chlorinated PAHs (ClPAHs), were analyzed in air, bulk deposition, soil, and water samples collected from urban, rural, field, and background sites on the eastern coast of China. The goal was to investigate and discuss their spatiotemporal variations, exchange fluxes, and transport potential. The concentrations of PAHs and their derivatives in the air and bulk deposition displayed distinct seasonal patterns, with higher concentrations observed during the winter and spring and lower concentrations during the summer and autumn. NPAHs exhibited the opposite trend. Significant urban-rural gradients were observed for most of the PAHs and their derivatives. According to the air-soil fugacity calculations, 2–3 ring PAHs, BrPAHs, and ClPAHs were found to volatilize from the soil into the air, while 4–7 ring PAHs, OPAHs, and NPAHs deposited from the air into the soil. The air-water fugacity of the PAHs and their derivatives indicated that surface water was an important source for the ambient atmosphere in Qingdao. The characteristic travel distances (CTDs) and persistence (Pov) for atmospheric transport were much lower than that for the water samples, which may be due to the longer half-lives of PAHs and their derivatives in water. NPAHs and ClPAHs with long transport distances and strong persistence in water could lead to a significant impact on marine pollution.

Phases in fine volcanic ash

Volcanic ash emissions impact atmospheric processes, depositional ecosystems, human health, and global climate. These effects are sensitive to the size and composition of the ash; however, datasets describing the constituent phases over size ranges relevant for atmospheric transport and widely distributed impacts are practically nonexistent. Here, we present results of X-ray diffraction measurements on size-separated fractions of 40 ash samples from VEI 2–6 eruptions. We characterize changes in phase fractions with grainsize, tectonic setting, and whole-rock SiO2. For grainsizes < 45 μm, average fractions of crystalline silica and surface salts increased while glass and iron oxides decreased with respect to the bulk sample. Samples from arc and intraplate settings are distinguished by feldspar and clinopyroxene fractions (determined by different crystallization sequences) which, together with glass, comprise 80–100% of most samples. We provide a dataset to approximate glass-free proportions of major crystalline phases; however, glass fractions are highly variable. To tackle this, we describe regressions between glass and major crystal phase fractions that help constrain the major phase proportions in volcanic ash with limited a priori information. Using our dataset, we find that pore-free ash density is well-estimated as a function of the clinopyroxene + Fe-oxide fraction, with median values of 2.67 ± 0.01 and 2.85 ± 0.03 g/cm3 for intraplate and arc samples, respectively. Finally, we discuss effects including atmospheric transport and alteration on modal composition and contextualize our proximal airfall ash samples with volcanic ash cloud properties. Our study helps constrain the atmospheric and environmental budget of the phases in fine volcanic ash and their effect on ash density, integral to refine our understanding of the impact of explosive volcanism on the Earth system from single eruptions to global modeling.

Characteristics of clustered heavy precipitation events at Northeast China and associated atmospheric circulations

AbstractHeavy precipitation events can exert greater impact than general precipitation on the economy, ecology, and people’s livelihoods. Based on CN05.1 daily precipitation data and the NCEP/NCAR global daily reanalysis dataset, this study analyzes the characteristics of clustered heavy precipitation (CHP) events during summer in Northeast China (NEC) during 1961–2020, with consideration of associated atmospheric circulations and moisture transport. Results indicate that CHP events occurred mainly during midsummer, especially in July. Both the frequency and the intensity of CHP events decrease after the mid-1970s, increase after the early 1980s, and then diminish again after the 2000s. The CHP events occur in association with an anomalous lower-tropospheric cyclone centered over NEC, northward and westward shifts of the western North Pacific subtropical high in the middle troposphere, and northward shift of an intensified westerly jet in the upper troposphere, in conjunction with strengthened local convective motion. Additionally, the net moisture budget begins to increase 2 days before the occurrence of CHP and peaks 6 h earlier than the CHP. Further results indicate that net moisture influx across the southern boundary of NEC made a dominant contribution to the net moisture budget. The results of this study have importance regarding the prediction of CHP events over NEC.

Dynamic prediction of spatial dose rate distribution during nuclear severe accidents by means of active machine learning and mobile sensors

The prediction of atmospheric dispersion of nuclear material is crucial to support emergency response during nuclear accidents, due to the potential severity and far-reaching consequences of such accidents. This importance is particularly evident in the context of severe accidents, like the incident that occurred at the Fukushima Daiichi Nuclear Power Plant (NPP). NPP are commonly supported by atmospheric dispersion systems (ADS), which estimate the spatial dose rates distribution, referred to as the dose rate map (DRM), by means of physical model simulations, including source term (ST), wind fields, atmospheric transport and diffusion, and dose calculations. However, it is well-known that a real accident scenario may differ from those modeled especially under severe conditions, and this fact may lead to erroneous predictions resulting in poor or catastrophic decision making. Aiming to minimize this problem, several efforts have been made to improve predictions based on field measurements, such as inverse problems and other methods to correct/adjust ST parameters. Such methods, however, complement the physical model calculations. This paper proposes a novel approach to predict DRM at ground level, based only upon field measurements (avoiding execution of physical model simulations). The idea is to dynamically adapt a set of mobile sensors (for example monitoring drones swarm) to follow the radioactive plume. To achieve this, an active machine learning (AML) approach was developed based on Gaussian process regression (GRP) and swarm intelligence. To test the approach, computational experiments using realistic simulated data (generated on the ADS simulator of a Brazilian NPP) has been used. As result, DRMs have been reproduced with good qualitative (visual) representation and satisfactory quantitative metrics. The average correlation coefficient between predicted and real DRMs was approximately 0.72 (ranging from 0.64 to 0.97 during plume evolution), demonstrating to be a promising approach to predict DRMs.

The Hydrologic Cycle and Atmospheric Rivers in CESM2 Simulations of the Last Glacial Maximum

AbstractProxy reconstructions and model simulations of precipitation during Earth's glacial periods suggest that the locations and mechanisms of atmospheric moisture transport have changed considerably during Earth's past. We investigate the hydroclimate of the Last Glacial Maximum (LGM) using simulations with the Community Earth System Model, with a focus on the extratropics and the influence of atmospheric rivers (ARs), a key driver of modern‐day moisture transport globally. Mean and extreme precipitation increase significantly over southwestern Patagonia, Iberia, and southwestern North America—mid‐latitude regions affected by ARs in the modern climate—despite overall decreases elsewhere. In each, the associated moisture transport changes are different, with increased transport and AR activity mainly occurring in the North Atlantic. The overall LGM response is dominated by the response to ice sheets, with other forcings causing additional cooling and drying over the extratropics and a strong decrease of moisture transport over the subpolar North Atlantic.

Downwind gas condensate volatiles affect phytoplankton communities

We investigated the effects of volatile organic carbons (VOCs) evaporated from gas condensate on the cyanobacteria Synechococcus sp. WH8103, the diatom Asterionellopsis glacialis, and the dinoflagellate Alexandrium minutum. We used custom algal incubation chambers enabling only the gas condensate-derived VOCs to interact with the cell cultures via an atmospheric bridge, without direct contact with the hydrocarbon oil. The exposure to gas condensate VOCs reduced the abundance, growth rate, and photosynthetic efficiency of Synechococcus sp. WH8103. Thiobarbituric acid reactive substances (TBARS) assays hint at oxidative damage to the chloroplasts and/or the thylakoid membranes in this organism. A.glacialis abundance, physiological state and growth rates remained unchanged, whereas A.minutum abundance and photosynthetic efficiency increased relative to their respective controls. Our results demonstrate that the effects of a gas condensate formed due to an oil spill will not be restricted to the polluted area, but may be prominent in downwind locations through atmospheric transport.

Sedimentary records of contaminant inputs in Frobisher Bay, Nunavut

Contaminants, such as polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs), heavy metals, and per and polyfluoroalkyl substances (PFASs), primarily reach the Arctic through long-range atmospheric and oceanic transport. However, local sources within the Arctic also contribute to the levels observed in the environment, including legacy sources and new sources that arise from activities associated with increasing commercial and industrial development. The City of Iqaluit in Frobisher Bay, Nunavut (Canada), has seen rapid population growth and associated development during recent decades yet remains a site of interest for ocean protection, where Inuit continue to harvest country food. In the present study, seven dated marine sediment cores collected in Koojesse Inlet near Iqaluit, and from sites in inner and outer Frobisher Bay, respectively, were analyzed for total mercury (THg), major and trace elements, PAHs, PCBs, and PFASs. The sedimentary record in Koojesse Inlet shows a period of Aroclor 1260-like PCB input concurrent with military site presence in the 1950–60s, followed by decades of input of pyrogenic PAHs, averaging about ten times background levels. Near-surface sediments in Koojesse Inlet also show evidence of transient local-source inputs of THg and PFASs, and recycling or continued slow release of PCBs from legacy land-based sources. Differences in PFAS congener composition clearly distinguish the local sources from long-range transport. Outside Koojesse Inlet but still in inner Frobisher Bay, 9.2 km from Iqaluit, sediments showed evidence of both local source (PCB) and long-range transport. In outer Frobisher Bay, an up-core increase in THg and PFASs in sediments may be explained by ongoing inputs of these contaminants from long-range transport. The context for ocean protection and country food harvesting in this region of the Arctic clearly involves both local sources and long-range transport, with past human activities leaving a long legacy insofar as levels of persistent organic pollutants are concerned.

An optimisation method to improve modelling of wet deposition in atmospheric transport models: applied to FLEXPART v10.4

Abstract. Wet deposition plays a crucial role in the removal of aerosols from the atmosphere. Yet, large uncertainties remain in its implementation in atmospheric transport models, specifically in the parameterisation schemes that are often used. Recently, a new wet deposition scheme was introduced in FLEXPART. The input parameters for its wet deposition scheme can be altered by the user and may be case-specific. In this paper, a new method is presented to optimise the wet scavenging rates in atmospheric transport models such as FLEXPART. The optimisation scheme is tested in a case study of aerosol-attached 137Cs following the Fukushima Daiichi nuclear power plant accident. From this, improved values for the wet scavenging input parameters in FLEXPART are suggested.

Microplastics in Freshwater Ecosystems of India: Current Trends and Future Perspectives.

Microplastics (MPs)-i.e., plastic particles less than 5 mm in length-are becoming a growing environmental concern due to their potential ecotoxicological impacts on aquatic ecosystems. In India, MPs contamination is a significantly growing problem due to increased plastic production as well as its low rate of recycling. As a result, MPs research work in India has gained considerable attention in the last two decades. The objective of this study is to conduct a comprehensive review of the existing scientific literature on MPs in freshwater ecosystems (e.g., lakes and rivers) of India. A bibliographical search was used to conduct the literature review across a number of databases including ScienceDirect, Google Scholar, and ResearchGate. We found that in comparison to the marine ecosystem the source, transport, and fate of MPs in freshwater ecosystems of India are still underexplored, and we found only 18 relevant papers. This review work reveals that there is no standard procedure for separating MPs from water and sediment samples, and as a result, comparing the results was a challenging task. The larger MPs (>500 μm) in water and sediments were identified most commonly using the attenuated total reflection (ATR) Fourier Transform Infrared (FTIR) spectroscopy technique (ATR-FTIR), whereas smaller-sized MPs (<500 μm) were identified using FTIR fitted with a confocal microscope, also known as μ-FTIR imaging or chemical imaging. We found that white-colored fibers and fragments of polypropylene (PP), polyethylene terephthalate (PET), and polyethylene (PE) were the most common polymer types in the freshwater ecosystems of India. Although research on MPs in freshwater ecosystems of India has gained momentum over the past decade, the literature review reveals a limited understanding of the impact of MPs' weathering patterns, the role of biofouling, and the role of water hyacinths on freshwater ecosystem services in India. Furthermore, the fluxes of MPs to the Indian oceans are not constrained, and atmospheric transport in high-altitude mountains, which have already been made fragile by climate change, has not been fully investigated. This study, therefore, calls for additional assessments of MPs in freshwater ecosystems-particularly in the central parts of India.

Linearity of the Climate System Response to Raising and Lowering West Antarctic and Coastal Antarctic Topography

Abstract A hierarchy of general circulation models (GCMs) is used to investigate the linearity of the response of the climate system to changes in Antarctic topography. Experiments were conducted with a GCM with either a slab ocean or fixed SSTs and sea ice, in which the West Antarctic ice sheet (WAIS) and coastal Antarctic topography were either lowered or raised in an idealized way. Additional experiments were conducted with a fully coupled GCM with topographic perturbations based on an ice-sheet model in which the WAIS collapses. The response over the continent is the same in all model configurations and is mostly linear. In contrast, the response has substantial nonlinear elements over the Southern Ocean that depend on the model configuration and are due to feedbacks with sea ice, ocean, and clouds. The atmosphere warms near the surface over much of the Southern Ocean and cools in the stratosphere over Antarctica, whether topography is raised or lowered. When topography is lowered, the Southern Ocean surface warming is due to strengthened southward atmospheric heat transport and associated enhanced storminess over the WAIS and the high latitudes of the Southern Ocean. When topography is raised, Southern Ocean warming is more limited and is associated with circulation anomalies. The response in the fully coupled experiments is generally consistent with the more idealized experiments, but the full-depth ocean warms throughout the water column whether topography is raised or lowered. These results indicate that ice sheet–climate system feedbacks differ depending on whether the Antarctic ice sheet is gaining or losing mass. Significance Statement Throughout Earth’s history, the Antarctic ice sheet was at times taller or shorter than it is today. The purpose of this study is to investigate how the atmosphere, sea ice, and ocean around Antarctica respond to changes in ice sheet height. We find that the response to lowering the ice sheet is not the opposite of the response to raising it, and that in either case the ocean surface near the continent warms. When the ice sheet is raised, the ocean warming is related to circulation changes; when the ice sheet is lowered, the ocean warming is from an increase in southward atmospheric heat transport. These results are important for understanding how the ice sheet height and local climate evolve together through time.

Atmospheric Moisture Transport Associated with Precipitation in Present and Simulated Future Climates

Abstract Precipitation and the atmospheric moisture budget are analyzed for 40-yr periods of recent and future climate simulated by the 10 CMIP6 models from which the vertically integrated moisture flux data are available. This allows new assessments of this important atmospheric transport, which can typically only be approximated. Seasonal climatological fields are compared with those from the ERA5 reanalysis. Using the four-season average M skill score for the globe, precipitation from the 10 models is similar in skill to that from a further 25 models. The scores for six moisture variables, including flux and its convergence, demonstrate global skill for each model. The 10-model average fields have better skill than any individual model. Changes are calculated for 2040–79 under the SSP5-8.5 forcing scenario. The focus is on the 10-model average scaled as a projection of change for a global warming of 2°C. The changes in precipitation, temperature, and pressure in each season are largely consistent with those from the larger ensemble. The changes in flux, convergence, water column, and winds at three levels are presented. The role of convergence in balancing precipitation changes over many land regions is evident. Flux, convergence, and precipitation are shown in detail for selected cases, including central North America, the South American monsoon, southern Africa in summer, southern South America in winter, Europe in summer, and both polar regions. Typically, flux is enhanced, but the associated convergence may shift. The production of the vertically integrated flux vector as a standard output from climate models is supported.

Evaluation of Simulated CO2 Point Source Plumes from High-Resolution Atmospheric Transport Model

Coal-fired power plants, as major anthropogenic CO2 emission sources, constitute one of the largest contributors to global greenhouse gas emissions. Accurately calculating the dispersion process of CO2 emissions from these point sources is crucial, as it will aid in quantifying CO2 emissions using remote sensing measurements. Employing the Lagrangian Particle Dispersion Theory Model (LPDTM), our study involves modeling CO2 diffusion from point sources. Firstly, we incorporated high-resolution DEM (Digital Elevation Model) and artificial building elements obtained through the Adaptive Deep Learning Location Matching Method, which is involved in CO2 simulation. The accuracy of the results was verified using meteorological stations and aircraft measurements. Additionally, we quantitatively analyzed the influence of terrain and artificial building characteristics on high spatial resolution atmospheric CO2 diffusion simulations, revealing the significance of surface characteristics in dispersion modeling. To validate the accuracy of the LPDTM in high-resolution CO2 diffusion simulation, a comparative experiment was conducted at a power plant in Yangzhou, Jiangsu Province, China. The simulated result was compared with observation from aerial flights, yielding the R2 (Correlation Coefficient) of 0.76, the RMSE (Root Mean Square Error) of 0.267 ppm, and the MAE (Mean Absolute Error) of 0.2315 ppm for the comparison of 73 pixels where the plume intersected with flight trajectories. The findings demonstrate a high level of consistency between the modeled CO2 point source plume morphology and concentration quantification and the actual observed outcomes. This study carried out a quantitative assessment of the influence of surface features on high-resolution atmospheric CO2 point source diffusion simulations, resulting in an enhanced accuracy of the simulated CO2 concentration field. It offers essential technological and theoretical foundations for the accurate quantification of anthropogenic CO2 emissions using top-down approaches.

Smoke emissions from biomass burning in Central Mexico and their impact on air quality in Mexico City: May 2019 case study

Smoke emissions from biomass burning considerably influence regional and local air quality. Many natural wildfires and agricultural burns occur annually in Central Mexico during the hot, dry season (March to May), potentially leading to air quality problems. Nevertheless, the impact of these biomass burning emissions on Mexico City's air quality has not been investigated in depth. This study examines a severely deteriorated air quality case from 11 to 16 May 2019, during which fine particle concentrations (PM2.5) exceeded the 99th percentile of the available official dataset (2005–2019). Specifically, this work aims to highlight the role of fires and regional pollution in the severe episode observed in Mexico City, identifying the fires that were the sources of regional pollution, the type of fuel burned in those fires, and the dominant atmospheric transport pattern. Biomass burning emissions were calculated for different land cover types using satellite data from the Visible Infrared Imaging Radiometer Suite (VIIRS) and the Moderate-Resolution Imaging Spectroradiometer (MODIS). PM2.5 increased by a factor of 2 at some monitoring sites, and ozone concentration increased to 40 % in Mexico City during the poor air quality episode. Our results indicate that over 50 % of the fire activity observed during the 2019 fire season was concentrated in May in Central Mexico. The burning activity was mainly seen over shrubland and forest between 10 and 15 May. Moreover, the fire radiative power analysis indicates that most energy was associated with burning shrubland and forests. Organic carbon emissions were estimated highest on 14 and 15 May, coinciding with the largest number of fires. Back trajectory analysis indicates that enhanced concentration of air pollutants in Mexico City originated from biomass burning detected in neighboring states: Guerrero, Michoacán, and the State of Mexico. Smoke from fires on the specific vegetation cover was advected into Mexico City and contributed to the bad air quality episode. Further meteorological analysis evidenced that the fire intensity and emissions were worsened by low humidity and the late onset of the rainy season in Central Mexico.

Morphological features and water solubility of iron in aged fine aerosol particles over the Indian Ocean

Abstract. Atmospheric transport of iron (Fe) in fine anthropogenic aerosol particles is an important route of soluble Fe supply from continental areas to remote oceans. To elucidate Fe properties of aerosol particles over remote oceans, we collected atmospheric aerosol particles over the Indian Ocean during the RV Hakuho Maru KH-18-6 cruise. After aerosol particles were collected using a cascade impactor, particles of 0.3–0.9 µm aerodynamic diameter on the sample stage were analyzed using transmission electron microscopy (TEM) with an energy-dispersive X-ray spectrometry analyzer. The particle shape and composition indicated that most particles collected north of the Equator were composed mainly of ammonium sulfate. Regarding the particle number fraction, 0.6 %–3.0 % of particles contained Fe, which mostly co-existed with sulfate. Of those particles, 26 % of Fe occurred as metal spheres, often co-existing with Al or Si, regarded as fly ash; 14 % as mineral dust; and 7 % as iron oxide aggregates. Water dialysis analyses of TEM samples indicated Fe in spherical fly ash as being almost entirely insoluble and Fe in other morphological-type particles as being partly soluble (65 % Fe mass on average). Global model simulations mostly reproduced observed Fe mass concentrations in particulate matter with a diameter of less than 2.5 µm (PM2.5) collected using a high-volume air sampler, including their north–south contrast during the cruise. In contrast, a marked difference was found between the simulated mass fractions of Fe mineral sources and the observed Fe types. For instance, the model underestimated anthropogenic aluminosilicate (illite and kaolinite) Fe contained in matter such as fly ash from coal combustion. Our observations revealed multiple shapes and compositions of Fe minerals in particles over remote ocean areas and further suggested that their solubilities after aging processes differ depending on their morphological and mineral types. Proper consideration of such Fe types at their sources is necessary for accurately estimating atmospheric Fe effects on marine biological activity.

The vertical distribution of 27 elements in bottom sediments reflects the modern history of the hypersaline lagoon

Knowledge of the distribution of various elements in the bottom vertical cores helps to assess current levels and to reconstruct the history of a water body. There is little to no bioturbation of bottom sediments in hypersaline lagoons/lakes, and vertical distribution of elements in the sediments is not distorted. The vertical distribution of 27 elements was studied in one of the Crimean hypersaline marine lakes. Their determination was carried out in layers one centimeter thick, which were taken from a depth of 1 cm to 28 cm. Using the technogenic radionuclide 90Sr, the time intervals when various layers of bottom sediments were formed had been previously determined. The concentrations of most elements, as well as their ratio, changed quasi-cyclically. For most of the elements for which such changes were noted, the maximum peak values were in the layers that formed in 1976 and 2006. The authors concluded from this that there appears to be a natural rhythm with a period of about 30 years. Not only a concentration of technogenic radionuclide 90Sr but also Mo, Ba, Tl, Sb, Se, and Ag reacted strongly to the accident at the Chernobyl nuclear power plant in 1986 due to atmospheric fallout and transportation of elements via the Dnieper river waters through the North Crimean Canal.

Constraints on simulated past Arctic amplification and lapse rate feedback from observations

Abstract. The Arctic has warmed more rapidly than the global mean during the past few decades. The lapse rate feedback (LRF) has been identified as being a large contributor to the Arctic amplification (AA) of climate change. This particular feedback arises from the vertically non-uniform warming of the troposphere, which in the Arctic emerges as strong near-surface and muted free-tropospheric warming. Stable stratification and meridional energy transport are two characteristic processes that are evoked as causes for this vertical warming structure. Our aim is to constrain these governing processes by making use of detailed observations in combination with the large climate model ensemble of the sixth Coupled Model Intercomparison Project (CMIP6). We build on the result that CMIP6 models show a large spread in AA and Arctic LRF, which are positively correlated for the historical period of 1951–2014. Thus, we present process-oriented constraints by linking characteristics of the current climate to historical climate simulations. In particular, we compare a large consortium of present-day observations to co-located model data from subsets that show a weak and strong simulated AA and Arctic LRF in the past. Our analyses suggest that the vertical temperature structure of the Arctic boundary layer is more realistically depicted in climate models with weak (w) AA and Arctic LRF (CMIP6/w) in the past. In particular, CMIP6/w models show stronger inversions in the present climate for boreal autumn and winter and over sea ice, which is more consistent with the observations. These results are based on observations from the year-long Multidisciplinary Drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition in the central Arctic, long-term measurements at the Utqiaġvik site in Alaska, USA, and dropsonde temperature profiling from aircraft campaigns in the Fram Strait. In addition, the atmospheric energy transport from lower latitudes that can further mediate the warming structure in the free troposphere is more realistically represented by CMIP6/w models. In particular, CMIP6/w models systemically simulate a weaker Arctic atmospheric energy transport convergence in the present climate for boreal autumn and winter, which is more consistent with fifth generation reanalysis of the European Centre for Medium-Range Weather Forecasts (ERA5). We further show a positive relationship between the magnitude of the present-day transport convergence and the strength of past AA. With respect to the Arctic LRF, we find links between the changes in transport pathways that drive vertical warming structures and local differences in the LRF. This highlights the mediating influence of advection on the Arctic LRF and motivates deeper studies to explicitly link spatial patterns of Arctic feedbacks to changes in the large-scale circulation.

Long-term trends in inorganic aerosol chemical composition and chemistry at an urban and rural site in the northeastern US

Atmospheric nitrate and sulfate are major inorganic particulate matter components that impact human and ecosystem health and air quality. Over the last several decades, emissions of the precursor gases, nitrogen oxides (NOx = NO + NO2) and sulfur dioxide (SO2), have dramatically decreased in the US in response to federal regulations. However, the response in concentrations of particulate nitrate (pNO3) and sulfate (pSO4) have not followed predictions due to complex non-linear chemistry feedbacks that may differ amongst environments (i.e., urban vs. rural). In this study, we explored the long-term response of particle chemistry for urban and rural environments in southern New England, a region historically impacted by NOx and SO2 emissions. Particulate matter (PM10) samples collected via the same method from 2005 to 2015 at urban and rural locations in Rhode Island were analyzed for their major inorganic components, and air mass trajectories and statistical analysis were used to identify source regions over time. Our results indicated a significant urban-rural aerosol chemical composition gradient for sampling locations within 40 km. Over time, as anthropogenic influences have decreased, the relative contribution of marine and crustal sources has increased greatly, impacting fine and coarse particle chemistry in recent years. Total mass concentrations of chemical species, particularly anthropogenic pSO4 and particulate ammonium (pNH4), have shown dramatic decreases over the ten years at both the urban and rural sites; however, pNO3 concentration increased by 95 % and 57 % in the urban and rural sites, respectively, despite significant NOx emission reductions. Our results demonstrate that changes in chemical mechanisms due to the decrease in SO2 emissions contributed to decreases in pNH4, along with enhanced pNO3 concentration. Furthermore, the change in SO2 emissions has significantly impacted the atmospheric lifetime and transport distance of pNH4, favoring more localized contributions in recent years.

Passive-tracer modelling at super-resolution with Weather Research and Forecasting – Advanced Research WRF (WRF-ARW) to assess mass-balance schemes

Abstract. Super-resolution atmospheric modelling can be used to interpret and optimize environmental observations during top-down emission rate retrieval campaigns (e.g. aircraft-based) by providing complementary data that closely correspond to real-world atmospheric pollution transport and dispersion conditions. For this work, super-resolution model simulations with large-eddy-simulation sub-grid-scale parameterization were developed and implemented using WRF-ARW (Weather Research and Forecasting - Advanced Research WRF). We demonstrate a series of best practices for improved (realistic) modelling of atmospheric pollutant dispersion at super-resolutions. These include careful considerations for grid quality over complex terrain, sub-grid turbulence parameterization at the scale of large eddies, and ensuring local and global tracer mass conservation. The study objective was to resolve small dynamical processes inclusive of spatio-temporal scales of high-speed (e.g. 100 m s−1) airborne measurements. This was achieved by downscaling of reanalysis data from 31.25 km to 50 m through multi-domain model nesting in the horizontal and grid-refining in the vertical. Further, WRF dynamical-solver source code was modified to simulate the release of passive tracers within the finest-resolution domain. Different meteorological case studies and several tracer source emission scenarios were considered. Model-generated fields were evaluated against observational data (surface monitoring network and aircraft campaign data) and also in terms of tracer mass conservation. Results indicated agreement between modelled and observed values within 5 ∘C for temperature, 1 %–25 % for relative humidity, and 1–2 standard deviations for wind fields. Model performance in terms of (global and local) tracer mass conservation was within 2 % to 5 % of model input emissions. We found that, to ensure mass conservation within the modelling domain, tracers should be released on a regular-resolution grid (vertical and horizontal). Further, using our super-resolution modelling products, we investigated emission rate estimations based on flux calculation and mass-balancing. Our results indicate that retrievals under weak advection conditions (horizontal wind speeds &lt; 5 m s−1) are not reliable due to weak correlation between the source emission rate and the downwind tracer mass flux. In this work we demonstrate the development of accurate super-resolution model simulations useful for planning, interpreting, and optimizing top-down retrievals, and we discuss favourable conditions (e.g. meteorological) for reliable mass-balance emission rate estimations.

Uncovering PM2.5 transport trajectories and sources at district within city scale

To continuously improve air quality, it is necessary to carry out fine management of air pollution prevention and control. However, research into regional transport of PM2.5 at a smaller spatial scale such as district is limited. In this study, a novel combined method was constructed to simulate and identify the regional transport trajectories and potential sources of PM2.5 concentrations at district scale, based on a hybrid model that integrates the Bayesian maximum entropy (BME) model, Weather Research and Forecast (WRF) and backward trajectory model. Take Tianjin as an example, an analysis of the transport trajectories showed that the air masses from northwest and southwest were the dominant atmospheric transport pathway in all seasons except summer. The number of transport trajectories from northwest and southwest accounted for 42.41% and 40.75% of the total number of transport trajectories. Despite the dominant wind direction in winter was northwest, it can be beneficial to atmospheric transport. This was because northwest trajectories were the long-range pathways, corresponding to fast-moving air masses that facilitate the dispersion of pollutants. On contrast, it is noteworthy that the southwest trajectories were the short-range pathways, resulting in limited diffusion and unfavorable conditions. The major potential cities that were likely contributors of PM2.5 (Weighted Concentration-Weighted Trajectory (WCWT) values greater than 40 μg m−3) were situated in the southwest. Furthermore, the inter-district transport results indicated that the primary direction of PM2.5 transport in Tianjin was also from south to north. It is critical that the current layout of Tianjin is adjusted in a timely manner through relocating or phasing out, as the majority of industrial enterprises with severe air pollution in Tianjin are located in the southern districts. This method of combining BME, WRF and backward trajectory can be used for atmospheric environment planning in other similar city and district-scale around the world. It also provides useful insights to policy makers when they formulate pollutants prevention control policies.