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Atmospheric simulation chambers continue to be indispensable tools for research in the atmospheric sciences. Insights from chamber studies are integrated into atmospheric chemical transport models, which are used for science-informed policy decisions. However, a centralized data management and access infrastructure for their scientific products had not been available in the United States and many parts of the world. ICARUS (Integrated Chamber Atmospheric data Repository for Unified Science) is an open access, searchable, web-based infrastructure for storing, sharing, discovering, and utilizing atmospheric chamber data [https://icarus.ucdavis.edu]. ICARUS has two parts: a data intake portal and a search and discovery portal. Data in ICARUS are curated, uniform, interactive, indexed on popular search engines, mirrored by other repositories, version-tracked, vocabulary-controlled, and citable. ICARUS hosts both legacy data and new data in compliance with open access data mandates. Targeted data discovery is available based on key experimental parameters, including organic reactants and mixtures that are managed using the PubChem chemical database, oxidant information, nitrogen oxide (NOx) content, alkylperoxy radical (RO2) fate, seed particle information, environmental conditions, and reaction categories. A discipline-specific repository such as ICARUS with high amounts of metadata works to support the evaluation and revision of atmospheric model mechanisms, intercomparison of data and models, and the development of new model frameworks that can have more predictive power in the current and future atmosphere. The open accessibility and interactive nature of ICARUS data may also be useful for teaching, data mining, and training machine learning models.

Abstract: We report on a multiyear set of airborne field campaigns (2005–16) off the California coast to examine aerosols, clouds, and meteorology, and how lessons learned tie into the upcoming NASA Earth Venture Suborbital (EVS-3) campaign: Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE; 2019–23). The largest uncertainty in estimating global anthropogenic radiative forcing is associated with the interactions of aerosol particles with clouds, which stems from the variability of cloud systems and the multiple feedbacks that affect and hamper efforts to ascribe changes in cloud properties to aerosol perturbations. While past campaigns have been limited in flight hours and the ability to fly in and around clouds, efforts sponsored by the Office of Naval Research have resulted in 113 single aircraft flights (>500 flight hours) in a fixed region with warm marine boundary layer clouds. All flights used nearly the same payload of instruments on a Twin Otter to fly below, in, and above clouds, producing an unprecedented dataset. We provide here i) an overview of statistics of aerosol, cloud, and meteorological conditions encountered in those campaigns and ii) quantification of model-relevant metrics associated with aerosol–cloud interactions leveraging the high data volume and statistics. Based on lessons learned from those flights, we describe the pragmatic innovation in sampling strategy (dual-aircraft approach with combined in situ and remote sensing) that will be used in ACTIVATE to generate a dataset that can advance scientific understanding and improve physical parameterizations for Earth system and weather forecasting models, and for assessing next-generation remote sensing retrieval algorithms.

Approximately 3 billion people worldwide cook with solid fuels, such as wood, charcoal, and agricultural residues. These fuels, also used for residential heating, are often combusted in inefficient devices, producing carbonaceous emissions. Between 2.6 and 3.8 million premature deaths occur as a result of exposure to fine particulate matter from the resulting household air pollution (Health Effects Institute, 2018a; World Health Organization, 2018). Household air pollution also contributes to ambient air pollution; the magnitude of this contribution is uncertain. Here, we simulate the distribution of the two major health-damaging outdoor air pollutants (PM2:5 and O3) using state-of-thescience emissions databases and atmospheric chemical transport models to estimate the impact of household combustion on ambient air quality in India. The present study focuses on New Delhi and the SOMAARTH Demographic, Development, and Environmental Surveillance Site (DDESS) in the Palwal District of Haryana, located about 80 km south of New Delhi. The DDESS covers an approximate population of 200 000 within 52 villages. The emissions inventory used in the present study was prepared based on a national inventory in India (Sharma et al., 2015, 2016), an updated residential sector inventory prepared at the University of Illinois, updated cookstove emissions factors from Fleming et al. (2018b), and PM2:5 speciation from cooking fires from Jayarathne et al. (2018). Simulation of regional air quality was carried out using the US Environmental Protection Agency Community Multiscale Air Quality modeling system (CMAQ) in conjunction with the Weather Research and Forecasting modeling system (WRF) to simulate the meteorological inputs for CMAQ, and the global chemical transport model GEOS-Chem to generate concentrations on the boundary of the computational domain. Comparisons between observed and simulated O3 and PM2:5 levels are carried out to assess overall airborne levels and to estimate the contribution of household cooking emissions.

Abstract. Discontinuities in apparent hygroscopicity below and above water saturation have been observed for organic and mixed organic–inorganic aerosol particles in both laboratory studies and in the ambient atmosphere. However, uncertainty remains regarding the factors that contribute to observations of low hygroscopic growth below water saturation but enhanced cloud condensation nuclei (CCN) activity for a given aerosol population. Utilizing laboratory surrogates for oligomers in atmospheric aerosols, we explore the extent to which such discontinuities are influenced by organic component molecular mass and viscosity, non-ideal thermodynamic interactions between aerosol components, and the combination of these factors. Measurements of hygroscopic growth under subsaturated conditions and the CCN activity of aerosols comprised of polyethylene glycol (PEG) with average molecular masses ranging from 200 to 10 000 g mol−1 and mixtures of PEG with ammonium sulfate (AS) were conducted. Experimental results are compared to calculations of hygroscopic growth at thermodynamic equilibrium conducted with the Aerosol Inorganic Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model, and the potential influence of kinetic limitations on observed water uptake was further explored through estimations of water diffusivity in the PEG oligomers. Particle-phase behavior, including the prevalence of liquid–liquid phase separation (LLPS), was also modeled with AIOMFAC. Under subsaturated relative humidity (RH) conditions, we observed little variability in hygroscopic growth across PEG systems with different molecular masses; however, an increase in CCN activity with increasing PEG molecular mass was observed. This effect is most pronounced for PEG–AS mixtures, and, in fact, an enhancement in CCN activity was observed for the PEG10000–AS mixture as compared to pure AS, as evidenced by a 15 % reduction in critical activation diameter at a supersaturation of 0.8 %. We also observed a marked increase in apparent hygroscopicity for mixtures of higher molecular mass PEG and AS under supersaturated conditions as compared to subsaturated hygroscopic growth. AIOMFAC-based predictions and estimations of water diffusivity in PEG suggest that such discontinuities in apparent hygroscopicity above and below water saturation can be attributed, at least in part, to differences in the sensitivity of water uptake behavior to surface tension effects. There is no evidence that kinetic limitations to water uptake due to the presence of viscous aerosol components influenced hygroscopic growth. For the systems that display an enhancement in apparent hygroscopicity above water saturation, LLPS is predicted to persist to high RH. This indicates a miscibility gap and is likely to influence bulk-to-surface partitioning of PEG at high RH, impacting droplet surface tension and CCN activity. This work provides insight into the factors likely to be contributing to discontinuities in aerosol water-uptake behavior below and above water saturation that have been observed previously in the ambient atmosphere.

The declining trend in vehicle emissions has underscored the growing significance of volatile organic compound (VOC) emissions from volatile chemical products (VCPs). However, accurately representing VOC chemistry in simplified chemical mechanisms remains challenging due to its chemical complexity including speciation and reactivity. Previous studies have predominantly focused on VOCs from fossil fuel sources, leading to an underrepresentation of VOC chemistry from VCP sources. We developed an integrated chemical mechanism, RACM2B-VCP, that is compatible with WRF-Chem and is aimed at enhancing the representation of VOC chemistry, particularly from VCP sources, within the present urban environment. Evaluation against the Air Quality System (AQS) network data demonstrates that our model configured with RACM2B-VCP reproduces both the magnitude and spatial variability of O3 and PM 2.5 in Los Angeles. Furthermore, evaluation against comprehensive measurements of O3 and PM 2.5 precursors from the Reevaluating the Chemistry of Air Pollutants in California (RECAP-CA) airborne campaign and the Southwest Urban NO x and VOC Experiment (SUNVEx) ground site and mobile laboratory campaign confirm the model's accuracy in representing NO x and many VOCs and highlight remaining biases. Although there exists an underprediction in the total VOC reactivity of observed VOC species, our model with RACM2B-VCP exhibits good agreement for VOC markers emitted from different sectors, including biogenic, fossil fuel, and VCP sources. Through sensitivity analyses, we probe the contributions of VCP and fossil fuel emissions to total VOC reactivity and O3. Our results reveal that 52 % of the VOC reactivity and 35 % of the local enhancement of MDA8 O3 arise from anthropogenic VOC emissions in Los Angeles. Significantly, over 50 % of this anthropogenic fraction of either VOC reactivity or O3 is attributed to VCP emissions. The RACM2B-VCP mechanism created, described, and evaluated in this work is ideally suited for accurately representing ozone for the right reasons in the present urban environment where mobile, biogenic, and VCP VOCs are all important contributors to ozone formation. [ABSTRACT FROM AUTHOR]

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth's clouds is the most uncertain component of the overall global radiative forcing from preindustrial time. General circulation models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions, but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. We suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

Abstract Data from three research flights, conducted over water near the California coast, are used to investigate the boundary between stratocumulus cloud decks and clearings of different sizes. Large clearings exhibit a diurnal cycle with growth during the day and contraction overnight and a multiday life cycle that can include oscillations between growth and decay, whereas a small coastal clearing was observed to be locally confined with a subdiurnal lifetime. Subcloud aerosol characteristics are similar on both sides of the clear–cloudy boundary in the three cases, while meteorological properties exhibit subtle, yet important, gradients, implying that dynamics, and not microphysics, is the primary driver for the clearing characteristics. Transects, made at multiple levels across the cloud boundary during one flight, highlight the importance of microscale (~1 km) structure in thermodynamic properties near the cloud edge, suggesting that dynamic forcing at length scales comparable to the convective eddy scale may be influential to the larger-scale characteristics of the clearing. These results have implications for modeling and observational studies of marine boundary layer clouds, especially in relation to aerosol–cloud interactions and scales of variability responsible for the evolution of stratocumulus clearings.

The influence of losses of organic vapors to chamber walls during secondary organic aerosol (SOA) formation experiments has recently been established. Here, the influence of such losses on simulated ambient SOA concentrations and properties is assessed in the University of California at Davis / California Institute of Technology (UCD/CIT) regional air quality model using the statistical oxidation model (SOM) for SOA. The SOM was fit to laboratory chamber data both with and without accounting for vapor wall losses following the approach of Zhang et al. (2014). Two vapor wall-loss scenarios are considered when fitting of SOM to chamber data to determine best-fit SOM parameters, one with "low" and one with "high" vapor wall-loss rates to approximately account for the current range of uncertainty in this process. Simulations were run using these different parameterizations (scenarios) for both the southern California/South Coast Air Basin (SoCAB) and the eastern United States (US). Accounting for vapor wall losses leads to substantial increases in the simulated SOA concentrations from volatile organic compounds (VOCs) in both domains, by factors of ∼2-5 for the low and ∼5-10 for the high scenarios. The magnitude of the increase scales approximately inversely with the absolute SOA concentration of the no loss scenario. In SoCAB, the predicted SOA fraction of total organic aerosol (OA) increases from ∼0.2 (no) to ∼0.5 (low) and to ∼0.7 (high), with the high vapor wall-loss simulations providing best general agreement with observations. In the eastern US, the SOA fraction is large in all cases but increases further when vapor wall losses are accounted for. The total OA/ΔCO ratio captures the influence of dilution on SOA concentrations. The simulated OA/ΔCO in SoCAB (specifically, at Riverside, CA) is found to increase substantially during the day only for the high vapor wall-loss scenario, which is consistent with observations and indicative of photochemical production of SOA. Simulated O:C atomic ratios for both SOA and for total OA increase when vapor wall losses are accounted for, while simulated H:C atomic ratios decrease. The agreement between simulations and observations of both the absolute values and the diurnal profile of the O:C and H:C atomic ratios for total OA was greatly improved when vapor wall-losses were accounted for. These results overall demonstrate that vapor wall losses in chambers have the potential to exert a large influence on simulated ambient SOA concentrations, and further suggest that accounting for such effects in models can explain a number of different observations and model-measurement discrepancies.

The prevailing treatment of secondary organic aerosol formation in atmospheric models is based on the assumption of instantaneous gas-particle equilibrium for the condensing species, yet compelling experimental evidence indicates that organic aerosols can exhibit the properties of highly viscous, semisolid particles, for which gas-particle equilibrium may be achieved slowly. The approach to gas-particle equilibrium partitioning is controlled by gas-phase diffusion, interfacial transport, and particle-phase diffusion. Here we evaluate the controlling processes and the time scale to achieve gas-particle equilibrium as a function of the volatility of the condensing species, its surface accommodation coefficient, and its particle-phase diffusivity. For particles in the size range of typical atmospheric organic aerosols (∼50-500 nm), the time scale to establish gas-particle equilibrium is generally governed either by interfacial accommodation or particle-phase diffusion. The rate of approach to equilibrium varies, depending on whether the bulk vapor concentration is constant, typical of an open system, or decreasing as a result of condensation into the particles, typical of a closed system.

Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought.

2-Methyl-3-buten-2-ol (MBO) is an important biogenic volatile organic compound (BVOC) emitted by pine trees and a potential precursor of atmospheric secondary organic aerosol (SOA) in forested regions. In the present study, hydroxyl radical (OH)-initiated oxidation of MBO was examined in smog chambers under varied initial nitric oxide (NO) and aerosol acidity levels. Results indicate measurable SOA from MBO under low-NO conditions. Moreover, increasing aerosol acidity was found to enhance MBO SOA. Chemical characterization of laboratory-generated MBO SOA reveals that an organosulfate species (C(5)H(12)O(6)S, MW 200) formed and was substantially enhanced with elevated aerosol acidity. Ambient fine aerosol (PM(2.5)) samples collected from the BEARPEX campaign during 2007 and 2009, as well as from the BEACHON-RoMBAS campaign during 2011, were also analyzed. The MBO-derived organosulfate characterized from laboratory-generated aerosol was observed in PM(2.5) collected from these campaigns, demonstrating that it is a molecular tracer for MBO-initiated SOA in the atmosphere. Furthermore, mass concentrations of the MBO-derived organosulfate are well correlated with MBO mixing ratio, temperature, and acidity in the field campaigns. Importantly, this compound accounted for an average of 0.25% and as high as 1% of the total organic aerosol mass during BEARPEX 2009. An epoxide intermediate generated under low-NO conditions is tentatively proposed to produce MBO SOA.