Physical Processes In Atmosphere Research Articles

Coupling Mesoscale Budget Components to Large-Eddy Simulations for Wind-Energy Applications

To simulate the airflow through a wind farm across a wide range of atmospheric conditions, microscale models (e.g., large-eddy simulation, LES, models) have to be coupled with mesoscale models, because microscale models lack the atmospheric physical processes to represent time-varying local forcing. Here we couple mesoscale model outputs to a LES solver by applying mesoscale momentum- and temperature-budget components from the Weather Research and Forecasting model to the governing equations of the Simulator fOr Wind Farm Applications model. We test whether averaging the budget components affects the LES results with regard to quantities of interest to wind energy. Our study focuses on flat terrain during a quiescent diurnal cycle. The simulation results are compared with observations from a 200-m tall meteorological tower and a wind-profiling radar, by analyzing time series, profiles, rotor-averaged quantities, and spectra. While results show that averaging reduces the spatio-temporal variability of the mesoscale momentum-budget components, when coupled with the LES model, the mesoscale bias (in comparison with observations of wind speed and direction, and potential temperature) is not reduced. In contrast, the LES technique can correct for shear and veer. In both cases, however, averaging the budget components shows no significant impact on the mean flow quantities in the microscale and is not necessary when coupling mesocale budget components to the LES model.

Understanding ozone pollution in the Yangtze River Delta of eastern China from the perspective of diurnal cycles

Ozone (O3) pollution has aroused increasing attention in China in past years, especially in the Yangtze River Delta (YRD), eastern China. Ozone and its precursors generally feature different diurnal patterns, which is closely related to atmospheric physical and chemical processes. This work aims to shed more light on the causes of ozone pollution from the perspective of the diurnal patterns. Hundreds of ozone pollution days (with maximum hourly O3 concentration over 100 ppb) during 2013–2017 were identified and then clustered into 4 typical types according to the diurnal variation patterns. We found that ozone pollution in Shanghai was particularly severe when anthropogenic pollutant mixed with biogenic volatile organic compounds (BVOCs) under the prevailing southwesterly wind in summer. The reason could be attributed to the spatial disparities of ozone sensitivity regime in YRD: VOC-limited regime around in the urban area and NOx-limited regime in the rural forest regions in the southern and southwest. The transition of sensitivity regimes along south/southwest wind tended to promote the photochemical production of ozone, making daily O3 pollution time exceeding 6 h of the day. In addition, ozone peak concentration in Shanghai was highly dependent on the evolution of sea-land breezes (SLBs). Earlier sea breeze associated with approaching typhoon in the West Pacific caused less cloud (−25%) and more solar radiation (11%) in YRD, which subsequently led to a rapid increase of O3 concentration in the morning and a deteriorated ozone pollution during noon and the afternoon. This study highlights the importance of observation-based processes understanding in air quality studies.

Tropical Atlantic Mixed Layer Buoyancy Seasonality: Atmospheric and Oceanic Physical Processes Contributions

This study investigates the physical processes controlling the mixed layer buoyancy using a regional configuration of an ocean general circulation model. Processes are quantified by using a linearized equation of state, a mixed-layer heat, and a salt budget. Model results correctly reproduce the observed seasonal near-surface density tendencies. The results indicate that the heat flux is located poleward of 10° of latitude, which is at least three times greater than the freshwater flux that mainly controls mixed layer buoyancy. During boreal spring-summer of each hemisphere, the freshwater flux partly compensates the heat flux in terms of buoyancy loss while, during the fall-winter, they act together. Under the seasonal march of the Inter-tropical Convergence Zone and in coastal areas affected by the river, the contribution of ocean processes on the upper density becomes important. Along the north Brazilian coast and the Gulf of Guinea, horizontal and vertical processes involving salinity are the main contributors to an upper water change with a contribution of at least twice as much the temperature. At the equator and along the Senegal-Mauritanian coast, vertical processes are the major oceanic contributors. This is mainly due to the vertical gradient of temperature at the mixed layer base in the equator while the salinity one dominates along the Senegal-Mauritania coast.

Spatial Characteristics of Heat Extremes in South Korea from the Climatological Mean Perspective

We investigated the spatial characteristics of heat extremes in South Korea from the climatological mean perspective. A heat extreme was defined as a day when the daily maximum temperature was higher than 33 °C. According to our analyses, the eastern area of the Sobaek and Taebaek mountain ranges (hereafter called the eastern district) is significantly more exposed to heat extremes compared to other areas. The onset date and total number of days of annual heat extremes in the eastern district are approximately 13 days earlier and 3 days higher than those in the western district on average, respectively. Likewise, the annual mean of daily maximum temperatures during heat extreme days are approximately 0.25 °C higher. This larger exposure to heat extremes in the eastern district appears to be attributable to the Föhn phenomenon, which is likely induced by the dominant southwesterly monsoon during the early-to-peak summer. In contrast, differences in the ending dates of annual heat extremes are not noticeable between the eastern and western districts, when the southerly winds are dominant. Our analyses suggest that heat extremes in South Korea cannot be understood by a simple function of latitude, but in conjunction with atmospheric physical processes.

Multi-scale processes in severe haze events in China and their interactions with aerosols: Mechanisms and progresses

<p indent=0mm>Severe haze events occur frequently in China, characterized by exceedingly high concentration of fine particulate matter (smaller than <sc>2.5 µm,</sc> or PM_2.5). These extremes are caused by synthetic physical-chemical processes, including emissions, chemical formation, planetary boundary layer processes, regional circulation, weather and climate. These processes are multi-scales, ranging from nanometers to thousands of kilometers. The complex interplays among these processes make it more difficult to understand the formation of severe haze events, which also influences model development and weather forecast. Here, we review the contributions of dominant mechanisms in severe haze events, especially their roles in temporal oscillations of PM_2.5 concentrations, and discuss the interplays among these atmospheric multi-scale processes. Previous studies indicate that: (1) Secondary aerosols become the dominant components in aerosols. Heterogeneous aqueous reactions play important roles in gas-to-particle conversion, especially in the late haze period; (2) PM_2.5 owns extensive temporal oscillations (on daily, weekly, to monthly timescales), which are caused by multi-scale processes; (3) high aerosols in China have already influenced photochemistry, boundary layer, weather and climate processes. The complex interplays among aerosols and the above processes make it more difficult to unravel the causes, mechanisms, and trends for haze pollution. In the future, the following issues should be considered: cooperative observations of aerosols, gas pollutants, photochemistry, and meteorological variables should be strengthened, especially their vertical distribution in the troposphere; multidisciplinary research should be strengthened, especially among atmospheric physics, chemistry, weather and climate; and model simulations related to the interplays among aerosols and atmospheric physical and chemical processes should be strengthened.

Earth’s Climate Does Not Depend on Variations in Cosmic Rays and Cloud Coverage

The hypothesis put forward by Svensmark and Friis-Christensen (1997), Svensmark (2007), Svensmark et al. (2017), and Stozhkov et al. (2017) assumes while completely ignoring the influence of quasi-200-year variation in TSI by ~0.4% (Shapiro et al., 2011; Egorova et al., 2018) that the increased penetrating by the galactic cosmic ray flux of the lower layers of the Earth’s atmosphere during the Grand Solar Minimum causes only an increase in cloud formation and the TSI reflected back into space. However, without calculating the changes in the global average annual energy balance between the Earth and space (Е0), the authors of the hypothesis argue that this effect will lead to a long-term negative average of the Earth’s annual energy budget and to climate cooling up to a Little Ice Age. The hypothesis also completely ignores all subsequent changes in atmospheric physical processes associated with increasing cloud coverage: the increased reflection and absorption of thermal radiation from the Earth’s surface and of solar radiation reflected from the Earth’s surface, the narrowing of atmospheric transparency windows, and the enhanced greenhouse effect. These processes compensate for the cooling. Our assessment shows that the changes in the global average annual energy balance between the Earth and space before and after a 2% increase in cloud coverage in the lower atmosphere have a difference of almost zero: E1 – E0 ≈ 0. The potential increase in cloud coverage causes virtually no variations in the global average annual energy balance between the Earth and space and has no effect on climate change (cooling).

Proxima Centauri b is not a transiting exoplanet

Abstract We report Spitzer Space Telescope observations during predicted transits of the exoplanet Proxima Centauri b. As the nearest terrestrial habitable-zone planet we will ever discover, any potential transit of Proxima b would place strong constraints on its radius, bulk density, and atmosphere. Subsequent transmission spectroscopy and secondary-eclipse measurements could then probe the atmospheric chemistry, physical processes, and orbit, including a search for biosignatures. However, our photometric results rule out planetary transits at the 200 ppm level at 4.5 $\mu$m, yielding a 3σ upper radius limit of 0.4 R⊕ (Earth radii). Previous claims of possible transits from optical ground- and space-based photometry were likely correlated noise in the data from Proxima Centauri’s frequent flaring. Our study indicates dramatically reduced stellar activity at near-to-mid infrared wavelengths, compared to the optical. Proxima b is an ideal target for space-based infrared telescopes, if their instruments can be configured to handle Proxima’s brightness.

Metatranscriptomic exploration of microbial functioning in clouds

Clouds constitute the uppermost layer of the biosphere. They host diverse communities whose functioning remains obscure, although biological activity potentially participates to atmospheric chemical and physical processes. In order to gain information on the metabolic functioning of microbial communities in clouds, we conducted coordinated metagenomics/metatranscriptomics profiling of cloud water microbial communities. Samples were collected from a high altitude atmospheric station in France and examined for biological content after untargeted amplification of nucleic acids. Living microorganisms, essentially bacteria, maintained transcriptional and translational activities and expressed many known complementary physiological responses intended to fight oxidants, osmotic variations and cold. These included activities of oxidant detoxification and regulation, synthesis of osmoprotectants/cryoprotectants, modifications of membranes, iron uptake. Consistently these energy-demanding processes were fueled by central metabolic routes involved in oxidative stress response and redox homeostasis management, such as pentose phosphate and glyoxylate pathways. Elevated binding and transmembrane ion transports demonstrated important interactions between cells and their cloud droplet chemical environments. In addition, polysaccharides, potentially beneficial for survival like exopolysaccharides, biosurfactants and adhesins, were synthesized. Our results support a biological influence on cloud physical and chemical processes, acting notably on the oxidant capacity, iron speciation and availability, amino-acids distribution and carbon and nitrogen fates.

A survey of the atmospheric physical processes key to the onset of Arctic sea ice melt in spring

September sea ice concentration (SIC) is found to be most sensitive to the early melt onset over the East Siberian Sea and Laptev Sea (73°–84°N, 90°–155°) in the Arctic, a region defined here as the area of focus (AOF). The areal initial melt date for a given year is marked when sea ice melting extends beyond 10% of the AOF size. With this definition, four early melting years (1990, 2012, 2003, 1991) and four late melting years (1996, 1984, 1983, 1982) were selected. The impacts and feedbacks of atmospheric physical and dynamical variables on the Arctic SIC variations were investigated for the selected early and late melting years based on the NASA MERRA-2 reanalysis. The sea ice melting tends to happen in a shorter period of time with larger magnitude in late melting years, while the melting lasts longer and tends to be more temporally smooth in early melting years. The first major melting event in each year has been further investigated and compared. In the early melting years, the positive Arctic Oscillation (AO) phase is dominant during springtime, which is accompanied by intensified atmospheric transient eddy activities in the Arctic and enhanced moisture flux convergence in the AOF and consequently enhanced northward transport of moist and warm air. As a result, positive anomalies of air temperature, precipitable water vapor (PWV) and/or cloud fraction and cloud water path were found over the AOF, increasing downward longwave radiative flux at the surface. The associated warming effect further contributes to the initial melt of sea ice. In contrast, the late melt onset is usually linked to the negative AO phase in spring accompanied with negative anomalies of PWV and downward longwave flux at the surface. The increased downward shortwave radiation during middle to late June plays a more important role in triggering the melting, aided further by the stronger than normal cloud warming effects.

Interactive 3D Visual Analysis of Atmospheric Fronts.

Atmospheric fronts play a central role in meteorology, as the boundaries between different air masses and as fundamental features of extra-tropical cyclones. They appear in numerous conceptual model depictions of extra-tropical weather systems. Conceptually, fronts are three-dimensional surfaces in space possessing an innate structural complexity, yet in meteorology, both manual and objective identification and depiction have historically focused on the structure in two dimensions. In this work, we -a team of visualization scientists and meteorologists- propose a novel visualization approach to analyze the three-dimensional structure of atmospheric fronts and related physical and dynamical processes. We build upon existing approaches to objectively identify fronts as lines in two dimensions and extend these to obtain frontal surfaces in three dimensions, using the magnitude of temperature change along the gradient of a moist potential temperature field as the primary identifying factor. We introduce the use of normal curves in the temperature gradient field to visualize a frontal zone (i.e., the transitional zone between the air masses) and the distribution of atmospheric variables in such zones. To enable for the first time a statistical analysis of frontal zones, we present a new approach to obtain the volume enclosed by a zone, by classifying grid boxes that intersect with normal curves emanating from a selected front. We introduce our method by means of an idealized numerical simulation and demonstrate its use with two real-world cases using numerical weather prediction data.

Size-resolved effective density of submicron particles during summertime in the rural atmosphere of Beijing, China

Particle density is an important physical property of atmospheric particles. The information on high time-resolution size-resolved particle density is essential for understanding the atmospheric physical and chemical aging processes of aerosols particles. In the present study, a centrifugal particle mass analyzer (CPMA) combined with a differential mobility analyzer (DMA) was deployed to determine the size-resolved effective density of 50 to 350nm particles at a rural site of Beijing during summer 2016. The measured particle effective densities decreased with increasing particle sizes and ranged from 1.43 to 1.55g/cm3, on average. The effective particle density distributions were dominated by a mode peaked at around 1.5g/cm3 for 50 to 350nm particles. Extra modes with peaks at 1.0, 0.8, and 0.6g/cm3 for 150, 240, and 350nm particles, which might be freshly emitted soot particles, were observed during intensive primary emissions episodes. The particle effective densities showed a diurnal variation pattern, with higher values during daytime. A case study showed that the effective density of Aitken mode particles during the new particle formation (NPF) event decreased considerably, indicating the significant contribution of organics to new particle growth.

Recent research progress and perspective of characteristics of ambient bioaerosols during hazy pollution in China

Since the haze event occurred in many areas of central and eastern China in 2013, haze pollution has become one of the most important environmental issues and has attracted more and more attention from government, industry circle, scholars and the general public in China. Haze pollution is characterized by atmospheric particular matter (PM) being one of the top pollutants. A large number of studies have been conducted to investigate the chemical components of atmospheric PM during haze pollution, while little is known about the biological components and characteristics of PM in the atmosphere, especially during haze pollution. Biological particles in the atmosphere, generally defined as bioaerosols, are airborne particles or large molecules carrying living organisms or released from living organisms (e.g., bacteria, fungi, viruses, pollen, bacterial endotoxins and mycotoxins, etc.). Bioaerosols not only pose potential risks on air quality and human health, but also have direct effects on the alteration of global climate and atmospheric physical and chemical processes. Up to now, however, the concentration and size distribution, diversity, and abundance of different types of bioaerosols as well as their temporal and spatial variability are not well characterized on hazy days. Moreover, due to the changeable community structure, flexible biological activity and comprehensive influential factors, the knowledge involving how haze pollution affects bioaerosols, to what extent it affects, and the influence mechanism is still unclear so far. Therefore, this review first has presented an overview of the state of bioaerosol research during haze pollution, including concentration level, size distribution and community structure of microorganisms in bioaerosols. Subsequently, the current understanding and open questions have been emphatically discussed concerning the characteristics of bioaerosols at different air pollution levels and effects of air pollution on airborne microbes. Finally, we suggest that the following research activities should be pursued in future studies of bioaerosols during haze pollution: (1) It is extremely urgent to develop and establish uniform standardized sampling and identification criterion to better judge and measure the numerous monitoring data from different researchers. It is also essential to develop advanced, sensitive, real-time and online detection techniques to quantify the biological properties of bioaerosols. (2) The nationwide field monitoring of bioaerosols covering more climate types and pollution levels at various time scales should be carried out to obtain more comprehensive data for fully understanding the temporal and spatial variability of bioaerosols and its influential factors. Some other meteorological influential factors (e.g., boundary-layer height, atmospheric extreme temperature, extreme wind speed, and atmospheric pressure, etc.), and pollution factors such as the concentration of heavy metal and polycyclic aromatic hydrocarbon (PAHs) in PM should be taken into account to deeply understand the effect of haze pollution on bioaerosols. (3) Current studies have shown that many gaseous and particulate pollutants are related to the concentration of bioaerosols. However, little is known about the influence mechanisms of pollutants. Therefore, in addition to field monitoring, it is also necessary to design and conduct the laboratory experiment of smog chamber to determine the influence mechanism of each single environmental factor or pollution factor on bioaerosols. (4) In addition to different degrees of haze pollution, there are different kinds of haze pollution including the formation of haze by photochemical reaction in summer and liquid phase reaction at high RH in winter. Therefore, it is also essential to examine the distribution and variation of bioaerosols during different haze formation processes in order to improve our understanding of haze pollution effects on bioaerosols. (5) It is necessary to develop a biological source-tracking technology based on the bioaerosol species and community composition to reveal the possible sources of bioaerosols during haze episodes.

Complex terrain experiments in the New European Wind Atlas.

The New European Wind Atlas project will create a freely accessible wind atlas covering Europe and Turkey, develop the model chain to create the atlas and perform a series of experiments on flow in many different kinds of complex terrain to validate the models. This paper describes the experiments of which some are nearly completed while others are in the planning stage. All experiments focus on the flow properties that are relevant for wind turbines, so the main focus is the mean flow and the turbulence at heights between 40 and 300 m. Also extreme winds, wind shear and veer, and diurnal and seasonal variations of the wind are of interest. Common to all the experiments is the use of Doppler lidar systems to supplement and in some cases replace completely meteorological towers. Many of the lidars will be equipped with scan heads that will allow for arbitrary scan patterns by several synchronized systems. Two pilot experiments, one in Portugal and one in Germany, show the value of using multiple synchronized, scanning lidar, both in terms of the accuracy of the measurements and the atmospheric physical processes that can be studied. The experimental data will be used for validation of atmospheric flow models and will by the end of the project be freely available.This article is part of the themed issue ‘Wind energy in complex terrains’.

Potential predictability sources of the 2012 U.S. drought in observations and a regional model ensemble

AbstractThe 2012 drought was the most severe and extensive summertime U.S. drought in half a century with substantial economic loss and impacts on food security and commodity prices. A unique aspect of the 2012 drought was its rapid onset and intensification over the Southern Rockies, extending to the Great Plains during late spring and early summer, and the absence of known precursor large‐scale patterns. Drought prediction therefore remains a major challenge. This study evaluates relationships among snow, soil moisture, and precipitation to identify sources of potential predictability of the 2012 summer drought using observations and a Weather Research and Forecasting model multiphysics ensemble experiment. Although underestimated in intensity, the drought signal is robust to the way atmospheric physical processes are represented in the model. For the Southern Rockies, soil moisture exhibits stronger persistence than precipitation in observations and the ensemble experiment. Correlations between winter/spring snowmelt and concurrent and following season soil moisture, and between soil moisture and concurrent and following season precipitation, in both observations and the model ensemble, suggest potential predictability beyond 1 and 2 month lead‐time reside in the land surface conditions for apparent flash droughts such as the 2012 drought.

Are atmospheric updrafts a key to unlocking climate forcing and sensitivity?

Abstract. Both climate forcing and climate sensitivity persist as stubborn uncertainties limiting the extent to which climate models can provide actionable scientific scenarios for climate change. A key, explicit control on cloud–aerosol interactions, the largest uncertainty in climate forcing, is the vertical velocity of cloud-scale updrafts. Model-based studies of climate sensitivity indicate that convective entrainment, which is closely related to updraft speeds, is an important control on climate sensitivity. Updraft vertical velocities also drive many physical processes essential to numerical weather prediction.Vertical velocities and their role in atmospheric physical processes have been given very limited attention in models for climate and numerical weather prediction. The relevant physical scales range down to tens of meters and are thus frequently sub-grid and require parameterization. Many state-of-science convection parameterizations provide mass fluxes without specifying vertical velocities, and parameterizations that do provide vertical velocities have been subject to limited evaluation against what have until recently been scant observations. Atmospheric observations imply that the distribution of vertical velocities depends on the areas over which the vertical velocities are averaged. Distributions of vertical velocities in climate models may capture this behavior, but it has not been accounted for when parameterizing cloud and precipitation processes in current models.New observations of convective vertical velocities offer a potentially promising path toward developing process-level cloud models and parameterizations for climate and numerical weather prediction. Taking account of the scale dependence of resolved vertical velocities offers a path to matching cloud-scale physical processes and their driving dynamics more realistically, with a prospect of reduced uncertainty in both climate forcing and sensitivity.

Neutral polyfluoroalkyl substances in the atmosphere over the northern South China Sea

Neutral Polyfluoroalkyl substances (PFASs) in the atmosphere were measured during a cruise campaign over the northern South China Sea (SCS) from September to October 2013. Four groups of PFASs, i.e., fluorotelomer alcohols (FTOHs), fluorotelomer acrylates (FTAs), fluorooctane sulfonamides (FOSAs) and fluorooctane sulfonamidoethanols (FASEs), were detected in gas samples. FTOHs was the predominant PFAS group, accounting for 95.2–99.3% of total PFASs (ΣPFASs), while the other PFASs accounted for a small fraction of ΣPFASs. The concentrations of ΣPFASs ranged from 18.0 to 109.9 pg m−3 with an average of 54.5 pg m−3. The concentrations are comparable to those reported in other marine atmosphere. Higher concentrations of ΣPFASs were observed in the continental-influenced samples than those in other samples, pointing to the substantial contribution of anthropogenic sources. Long-range transport is suggested to be a major pathway for introducing gaseous PFASs into the atmosphere over the northern SCS. In order to further understand the fate of gaseous PFASs during transport, the atmospheric decay of neutral PFASs under the influence of reaction with OH radicals and atmospheric physical processes were estimated. Concentrations of 8:2 FTOH, 6:2 FTOH and MeFBSE from selected source region to the atmosphere over the SCS after long-range transport were predicted and compared with the observed concentrations. It suggests that the reaction with OH radicals may play an important role in the atmospheric decay of PFAS during long-range transport, especially for shorted-lived species. Moreover, the influence of atmospheric physical processes on the decay of PFAS should be further considered.

Atmosphere‐ocean coupled processes in the Madden‐Julian oscillation

AbstractThe Madden‐Julian oscillation (MJO) is a convectively coupled 30–70 day (intraseasonal) tropical atmospheric mode that drives variations in global weather but which is poorly simulated in most atmospheric general circulation models. Over the past two decades, field campaigns and modeling experiments have suggested that tropical atmosphere‐ocean interactions may sustain or amplify the pattern of enhanced and suppressed atmospheric convection that defines the MJO and encourage its eastward propagation through the Indian and Pacific Oceans. New observations collected during the past decade have advanced our understanding of the ocean response to atmospheric MJO forcing and the resulting intraseasonal sea surface temperature fluctuations. Numerous modeling studies have revealed a considerable impact of the mean state on MJO ocean‐atmosphere coupled processes, as well as the importance of resolving the diurnal cycle of atmosphere‐upper ocean interactions. New diagnostic methods provide insight to atmospheric variability and physical processes associated with the MJO but offer limited insight on the role of ocean feedbacks. Consequently, uncertainty remains concerning the role of the ocean in MJO theory. Our understanding of how atmosphere‐ocean coupled processes affect the MJO can be improved by collecting observations in poorly sampled regions of MJO activity, assessing oceanic and atmospheric drivers of surface fluxes, improving the representation of upper ocean mixing in coupled model simulations, designing model experiments that minimize mean state differences, and developing diagnostic tools to evaluate the nature and role of coupled ocean‐atmosphere processes over the MJO cycle.

Review: Particle number size distributions from seven major sources and implications for source apportionment studies

Abstract The particle number size distribution (PNSD) of airborne particles not only provides us with information about sources and atmospheric processing of particles, but also plays an important role in determining regional lung dose. As a result, urban particles and their size distributions have received much attention with a rapid increase of publications in recent years. The object of this review is to synthesise and analyse existing knowledge on particles in urban environments with a focus on their number concentration and size distribution. This study briefly reviews the characterization of PNSD from seven major sources of urban particles including traffic emissions, industrial emissions, biomass burning, cooking, transported aerosol, marine aerosol and nucleation. It then discusses atmospheric physical processes such as coagulation or condensation which have a strong influence on PNSD. Finally, the implications of PNSD datasets for source modelling are briefly discussed. Based on this review, it is concluded that the concentrations, modal structures and temporal patterns of urban particles are strongly influenced by traffic emissions, which are identified as the main source of particle number in urban environments. Information derived from particle number size distributions is beginning to play an important role in source apportionment studies.

Overview of receptor-based source apportionment studies for speciated atmospheric mercury

Abstract. Receptor-based source apportionment studies of speciated atmospheric mercury are not only concerned with source contributions but also with the influence of transport, transformation, and deposition processes on speciated atmospheric mercury concentrations at receptor locations. Previous studies applied multivariate receptor models including principal components analysis and positive matrix factorization, and back trajectory receptor models including potential source contribution function, gridded frequency distributions, and concentration–back trajectory models. Combustion sources (e.g., coal combustion, biomass burning, and vehicular, industrial and waste incineration emissions), crustal/soil dust, and chemical and physical processes, such as gaseous elemental mercury (GEM) oxidation reactions, boundary layer mixing, and GEM flux from surfaces were inferred from the multivariate studies, which were predominantly conducted at receptor sites in Canada and the US. Back trajectory receptor models revealed potential impacts of large industrial areas such as the Ohio River valley in the US and throughout China, metal smelters, mercury evasion from the ocean and the Great Lakes, and free troposphere transport on receptor measurements. Input data and model parameters specific to atmospheric mercury receptor models are summarized and model strengths and weaknesses are also discussed. Multivariate models are suitable for receptor locations with intensive air monitoring because they require long-term collocated and simultaneous measurements of speciated atmospheric Hg and ancillary pollutants. The multivariate models provide more insight about the types of Hg emission sources and Hg processes that could affect speciated atmospheric Hg at a receptor location, whereas back trajectory receptor models are mainly ideal for identifying potential regional Hg source locations impacting elevated Hg concentrations. Interpretation of the multivariate model output to sources can be subjective and challenging when speciated atmospheric Hg is not correlated with ancillary pollutants and when source emissions profiles and knowledge of Hg chemistry are incomplete. The majority of back trajectory receptor models have not accounted for Hg transformation and deposition processes and could not distinguish between upwind and downwind sources effectively. Ensemble trajectories should be generated to take into account the trajectory uncertainties where possible. One area of improvement that applies to all the receptor models reviewed in this study is the greater focus on evaluating the accuracy of the models at identifying potential speciated atmospheric mercury sources, source locations, and chemical and physical processes in the atmosphere. In addition to receptor model improvements, the data quality of speciated atmospheric Hg plays an equally important part in producing accurate receptor model results.

Modeling of HCHO and CHOCHO at a semi-rural site in southern China during the PRIDE-PRD2006 campaign

Abstract. HCHO and CHOCHO are important trace gases in the atmosphere, serving as tracers of VOC oxidations. In the past decade, high concentrations of HCHO and CHOCHO have been observed for the Pearl River Delta (PRD) region in southern China. In this study, we performed box model simulations of HCHO and CHOCHO at a semi-rural site in the PRD, focusing on understanding their sources and sinks and factors influencing the CHOCHO to HCHO ratio (RGF). The model was constrained by the simultaneous measurements of trace gases and radicals. Isoprene oxidation by OH radicals is the major pathway forming HCHO, followed by degradations of alkenes, aromatics, and alkanes. The production of CHOCHO is dominated by isoprene and aromatic degradation; contributions from other NMHCs are of minor importance. Compared to the measurement results, the model predicts significant higher HCHO and CHOCHO concentrations. Sensitivity studies suggest that fresh emissions of precursor VOCs, uptake of HCHO and CHOCHO by aerosols, fast vertical transport, and uncertainties in the treatment of dry deposition all have the potential to contribute significantly to this discrepancy. Our study indicates that, in addition to chemical considerations (i.e., VOC composition, OH and NOx levels), atmospheric physical processes (e.g., transport, dilution, deposition) make it difficult to use the CHOCHO to HCHO ratio as an indicator for the origin of air mass composition.