Atmospheric Chemistry and Physics

Future African aerosol emissions, and therefore air pollution levels and health outcomes, are uncertain and understudied. Understanding the future health impacts of pollutant emissions from this region is crucial. Here, this research gap is addressed by studying the range in the future health impacts of aerosol emissions from Africa in the Shared Socioeconomic Pathway (SSP) scenarios, using the UK Earth System Model version 1 (UKESM1), along with human health concentration-response functions. The effects of Africa following a high-pollution aerosol pathway are studied relative to a low-pollution control, with experiments varying aerosol emissions from industry and biomass burning...

Mobile sources are responsible for a substantial controllable portion of the reactive organic carbon (ROC) emitted to the atmosphere, especially in urban environments of the United States. We update existing methods for calculating mobile source organic particle and vapor emissions in the United States with over a decade of laboratory data that parameterize the volatility and organic aerosol (OA) potential of emissions from on-road vehicles, nonroad engines, aircraft, marine vessels, and locomotives. We find that existing emission factor information from Teflon filters combined with quartz filters collapses into simple relationships and can be used to reconstruct the complete volatility distribution of ROC emissions...

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes...

The fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4) is conducting a diagnostic intercomparison and evaluation of deposition simulated by regional-scale air quality models over North America and Europe. In this study, we analyze annual AQMEII4 simulations performed with the Community Multiscale Air Quality Model (CMAQ) version 5.3.1 over North America. These simulations were configured with both the M3Dry and Surface Tiled Aerosol and Gas Exchange (STAGE) dry deposition schemes available in CMAQ...

Recently, volatile chemical products (VCPs) have been increasingly recognized as important precursors for secondary organic aerosol (SOA) and ozone in urban areas. However, their atmospheric chemistry, physical transformation, and their impact on climate, environment and human health remain poorly understood. Here, the yields and chemical composition at the molecular level of gas and particle phase products originating from the photooxidation of one of these VCPs, benzyl alcohol (BnOH), is reported. The SOA was generated in the presence of seed aerosol from nebulized ammonium sulfate solution in a 14...

Volatile chemical products (VCPs) and other non-combustion-related sources have become important for urban air quality, and bottom-up calculations report emissions of a variety of functionalized compounds that remain understudied and uncertain in emissions estimates. Using a new instrumental configuration, we present online measurements of oxygenated organic compounds in a U.S. megacity over a 10-day wintertime sampling period, when biogenic sources and photochemistry were less active. Measurements were conducted at a rooftop observatory in upper Manhattan, New York City, USA using a Vocus chemical ionization time-of-flight mass spectrometer with ammonium (NH4 + ) as the reagent ion operating at 1 Hz...

Airborne aerosols reduce surface solar radiation through light scattering and absorption (aerosol direct effects, ADEs), influence regional meteorology, and further affect atmospheric chemical reactions and aerosol concentrations. The inhibition of turbulence and the strengthened atmospheric stability induced by ADEs increases surface primary aerosol concentration, but the pathway of ADE impacts on secondary aerosol is still unclear. In this study, the online coupled meteorological and chemistry model (WRF-CMAQ; Weather Research and Forecasting-Community Multiscale Air Quality) with integrated process analysis was applied to explore how ADEs affect secondary aerosol formation through changes in atmospheric dynamics and photolysis processes...

The COVID-19 pandemic created an extreme natural experiment in which sudden changes in human behavior and economic activity resulted in significant declines in nitrogen oxide (NO x ) emissions, immediately after strict lockdowns were imposed. Here we examined the impact of multiple waves and response phases of the pandemic on nitrogen dioxide (NO2 ) dynamics and the role of meteorology in shaping relative contributions from different emission sectors to NO2 pollution in post-pandemic New York City. Long term (> 3...

The Arctic is a climatically sensitive region that has experienced warming at almost 3 times the global average rate in recent decades, leading to an increase in Arctic greenness and a greater abundance of plants that emit biogenic volatile organic compounds (BVOCs). These changes in atmospheric emissions are expected to significantly modify the overall oxidative chemistry of the region and lead to changes in VOC composition and abundance, with implications for atmospheric processes. Nonetheless, observations needed to constrain our current understanding of these issues in this critical environment are sparse...

Evaluating the influence of anthropogenic-emission changes on air quality requires accounting for the influence of meteorological variability. Statistical methods such as multiple linear regression (MLR) models with basic meteorological variables are often used to remove meteorological variability and estimate trends in measured pollutant concentrations attributable to emission changes. However, the ability of these widely used statistical approaches to correct for meteorological variability remains unknown, limiting their usefulness in the real-world policy evaluations...

Aerosol-cloud interactions (ACIs) are considered to be the most uncertain driver of present-day radiative forcing due to human activities. The nonlinearity of cloud-state changes to aerosol perturbations make it challenging to attribute causality in observed relationships of aerosol radiative forcing. Using correlations to infer causality can be challenging when meteorological variability also drives both aerosol and cloud changes independently. Natural and anthropogenic aerosol perturbations from well-defined sources provide "opportunistic experiments" (also known as natural experiments) to investigate ACI in cases where causality may be more confidently inferred...

Volatile chemical products (VCPs) are commonly-used consumer and industrial items that are an important source of anthropogenic emissions. Organic compounds from VCPs evaporate on atmospherically relevant time scales and include many species that are secondary organic aerosol (SOA) precursors. However, the chemistry leading to SOA, particularly that of intermediate volatility organic compounds (IVOCs), has not been fully represented in regional-scale models such as the Community Multiscale Air Quality (CMAQ) model, which tend to underpredict SOA concentrations in urban areas...

Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. Accordingly, we jointly constrain NO x and VOC emissions using well-characterized TROPOspheric Monitoring Instrument (TROPOMI) HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline)...

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2...

We compare Community Multiscale Air Quality (CMAQ) model predictions with measured nitrous acid (HONO) concentrations in Beijing, China for December 2015. The model with the existing HONO chemistry in CMAQ severely under-estimates the observed HONO concentrations with a normalized mean bias of -97%. We revise the HONO chemistry in the model by implementing six additional heterogeneous reactions in the model: reaction of nitrogen dioxide (NO2 ) on ground surfaces, reaction of NO2 on aerosol surfaces, reaction of NO2 on soot surfaces, photolysis of aerosol nitrate, nitric acid displacement reaction, and hydrochloric acid displacement reaction...

We present in this technical note the research protocol for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This research initiative is divided into two activities, collectively having three goals: (i) to define the current state of the science with respect to representations of wet and especially dry deposition in regional models, (ii) to quantify the extent to which different dry deposition parameterizations influence retrospective air pollutant concentration and flux predictions, and (iii) to identify, through the use of a common set of detailed diagnostics, sensitivity simulations, model evaluation, and reduction of input uncertainty, the specific causes for the current range of these predictions...

The acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications for the tropospheric lifetime of air pollutants, atmospheric composition, deposition to terrestrial and oceanic ecosystems, visibility, climate, and human health...

During the 3 years of the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign, the NASA Orion P-3 was equipped with a 2D stereo (2D-S) probe that imaged particles with maximum dimension ( D ) ranging from 10 < D < 1280 μm. The 2D-S recorded supermicron-sized aerosol particles (SAPs) outside of clouds within biomass burning plumes during flights over the southeastern Atlantic off Africa's coast. Numerous SAPs with 10 < D < 1520 μm were observed in 2017 and 2018 at altitudes between 1230 and 4000 m, 1000 km from the coastline, mostly between 7-11° S...

Nitrogen oxides (NO x =NO+NO2 ) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment - 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region...

Cloud drop number concentrations ( N d ) over the western North Atlantic Ocean (WNAO) are generally highest during the winter (DJF) and lowest in summer (JJA), in contrast to aerosol proxy variables (aerosol optical depth, aerosol index, surface aerosol mass concentrations, surface cloud condensation nuclei (CCN) concentrations) that generally peak in spring (MAM) and JJA with minima in DJF. Using aircraft, satellite remote sensing, ground-based in situ measurement data, and reanalysis data, we characterize factors explaining the divergent seasonal cycles and furthermore probe into factors influencing N d on seasonal timescales...