Examining the Climate Effects of a Regional Nuclear Weapons Exchange Using a Multiscale Atmospheric Modeling Approach.
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The bulk aerosol emissions excited by externally focused femtosecond laser filaments are characterized using time-resolved plasma imaging and spectroscopy. Images of N 2 and N 2 + plasma fluorescence are used to characterize the filament dimensions. Emission profiles from bulk Sr aerosols are studied, showing that several localized emission regions in the filament begin to develop for lower repetition rates and higher pulse energies. Plasma temperature and electron density profiles are determined using particle emissions along the length of short- and long-focused filaments, and results are compared for on-axis and side-collected spectra. The use of on-axis collection enables the sampling of light emitted over the entire length of the filament; however, the necessary back-propagation of light makes on-axis collection susceptible to self-absorption as the optical path is extended through the filament plasma column formed in bulk aerosols.
Global economic development and urbanization during the past two decades have driven the increases in demand of personal and commercial vehicle fleets, especially in developing countries, which has likely resulted in changes in year-to-year vehicle tailpipe emissions associated with aerosols and trace gases. However, long-term trends of impacts of global gasoline and diesel emissions on air quality and human health are not clear. In this study, we employ the Community Earth System Model in conjunction with the newly developed Community Emissions Data System as anthropogenic emission inventory to quantify the long-term trends of impacts of global gasoline and diesel emissions on ambient air quality and human health for the period of 2000–2015. Global gasoline and diesel emissions contributed to regional increases in annual mean surface PM 2.5 (particulate matter with aerodynamic diameters ≤2.5 μm) concentrations by up to 17.5 and 13.7 µg m –3 , and surface ozone (O 3 ) concentrations by up to 7.1 and 7.2 ppbv, respectively, for 2000–2015. However, we also found substantial declines of surface PM 2.5 and O 3 concentrations over Europe, the US, Canada, and China for the same period, which suggested the co-benefits of air quality and human health from improving gasoline and diesel fuel quality and tightening vehicle emissions standards. Globally, we estimate the mean annual total PM 2.5- and O 3 -induced premature deaths are 139 700–170 700 for gasoline and 205 200–309 300 for diesel, with the corresponding years of life lost of 2.74–3.47 and 4.56–6.52 million years, respectively. Diesel and gasoline emissions create health-effect disparities between the developed and developing countries, which are likely to aggravate afterwards.
The Raman lidar at the ARM Climate Research Facility (ACRF) Southern Great Plains (SGP) Central Facility (SGPRL) is an active, ground-based laser remote sensing instrument that measures height and time resolved profiles of water vapor mixing ratio and several cloud- and aerosol-related quantities. The system is a non-commercial custom-built instrument developed by Sandia National Laboratories specifically for the ARM Program. It is fully computer automated, and will run unattended for many days following a brief (~5-minute) startup period. The self-contained system (requiring only external electrical power) is housed in a climate-controlled 8’x8’x20’ standard shipping container.
Emerging coronaviruses are a global public health threat because of the potential for person-to-person transmission and high mortality rates. Middle East respiratory syndrome coronavirus (MERS-CoV) emerged in 2012, causing lethal respiratory disease in $\gg$35% of cases. Primate models of coronavirus disease are needed to support development of therapeutics, but few models exist that recapitulate severe disease. For initial development of a MERS-CoV primate model, 12 African green monkeys were exposed to 10 3 , 10 4 , or 10 5 PFU target doses of aerosolized MERS-CoV. We observed a dose-dependent increase of respiratory disease signs, although all 12 monkeys survived for the 28-day duration of the study. This study describes dosedependent effects of MERS-CoV infection of primates and uses a route of infection with potential relevance to MERSCoV transmission. Aerosol exposure of African green monkeys might provide a platform approach for the development of primate models of novel coronavirus diseases.
Dust aerosols have a wide size distribution from less than 0.1 to over 100 μm and dominate Earth's atmospheric aerosol mass. However, most Earth system models (ESMs) inadequately represent dust aerosols larger than 10 μm in diameter, limiting the accuracy of the simulated dust cycle and climate impacts. Here, we introduce a new modeling framework that captures the full observed size distribution of dust aerosols, incorporating recent advances into a mineral-resolved version of the Community ESM, while addressing known issues in previous versions. Comprehensive evaluation against diverse observations of bulk dust and component minerals demonstrates that the model reproduces the observed dust cycle across particle sizes. Incorporating the previously unrepresented large-dust fractions substantially alters dust budget estimates, highlighting potential changes in simulated climate impacts and underscoring the importance of comprehensive size-resolved dust modeling. Despite these advancements, uncertainties persist. Our results indicate that a size-dependent reduction in settling velocity is required to reproduce the observed dust size distribution downwind of source regions. Specifically, in the new model, the gravitational settling velocity of dust particles larger than 10 μm in diameter must be reduced by as much as 85% to achieve agreement with observations. This empirical reduction serves as a constraint on physics-based models of dust settling. Future developments should address misrepresented physical processes that hinder accurate modeling of the large dust aerosol transport. Expanding observational data sets covering the full-size distribution is also essential to better constrain the dust cycle and improve the representation of dust optical properties and climate effects.
Abstract Clouds, crucial for understanding climate, begin with droplet formation from aerosols, but observations of this fleeting activation step are lacking in the atmosphere. Here we use a time-gated time-correlated single-photon counting lidar to observe cloud base structures at decimeter scales. Results show that the air–cloud interface is not a perfect boundary but rather a transition zone where the transformation of aerosol particles into cloud droplets occurs. The observed distributions of first-arriving photons within the transition zone reflect vertical development of a cloud, including droplet activation and condensational growth. Further, the highly resolved vertical profile of backscattered photons above the cloud base enables remote estimation of droplet concentration, an elusive but critical property to understanding aerosol–cloud interactions. Our results show the feasibility of remotely monitoring cloud properties at submeter scales, thus providing much-needed insights into the impacts of atmospheric pollution on clouds and aerosol-cloud interactions that influence climate.
To evaluate the exposure potential of infectious aerosols containing SARS-CoV-2 in an office building setting, synthetic test aerosols were used to experimental study airborne particle transmission in a multizone small office test building at the Oak Ridge National Laboratory. Nine measurement points in a single zone using active aerosol impactors report that the coefficient of variation of the time-averaged concentration is <10% in two campaigns and < 15% in one campaign, so a nearly well-mixed condition was noted. To understand the effect of HVAC system operation on the dynamic concentration of aerosols in office spaces, an aerosol transport model that includes factors such as outside air (OA) ratio, filtration, return air fraction, transport loss in air ducts, and particle deposition has been developed. The results of model fitting demonstrate strong agreement with experimental data. Overall, our investigation finds the return air fraction effects outweigh other mechanisms for the aerosol recirculation in this study, and the impact of air change rate (ACR) is more important than the small particle deposition for aerosol removal. Because ACR dominates the aerosol transport, the full model can be simplified to just one factor, the ACR, while maintaining an acceptable representation of the experimental data.
Abstract Pyrocumulonimbus (PyroCb) clouds have a complex origin dependent on fire dynamics and meteorological conditions. When a pyrocumulonimbus cloud develops and is maintained over a period of time, it can inject significant aerosol into the troposphere and lower stratosphere, resulting in a longer‐term (months to years) occurrence of aerosol in the stratosphere. In this work, we investigate the British Columbia wildfires on 12–13 August 2017 using a multi‐scale simulation framework. We use the output of a physics‐based wildfire model (FIRETEC) with parameterized energy, particle, and gas emissions to drive the upper atmospheric aerosol mass injection within a regional cloud resolving model (HIGRAD). We demonstrate that vertical motions produced by latent heat release of the condensation of ice and cloud particles within the PyroCbs induce another 5 km of lifting of the simulated aerosol plume. Primary black carbon and organic aerosols (OAs) alone may not be enough to explain the observed aerosol burden, thus we show that secondary OA produced via condensation of gases by the fires, ash, and possibly dust can enhance lofted aerosol mass. A simulation with all emission mechanisms active, driven by the observed fuel load and environmental conditions, reasonably reproduces an aerosol profile inferred from observational data.
Experiments in the Pi Convection‐Cloud Chamber conducted by systematically changing the diameter of injected dry aerosol particles while holding the temperature difference constant demonstrate that dry diameter strongly influences the onset of haze‐dominated conditions. Two factors contribute: the system becomes water‐limited, resulting in reduction of supersaturation by growing aerosol particles to the activation diameter; and the activation process becomes kinetically limited. Dry aerosol diameter exerts a strong influence on activation time, with a power‐law exponent of 9/2. Kinetically limited activation occurs when the ratio of the activation and droplet residence times is greater than unity. The findings demonstrate that a haze‐dominated state, where cloud formation is suppressed, can be achieved not only with weak supersaturation forcing and high aerosol concentration but also with large, hygroscopic aerosol particles. These results have implications for cloud formation in polluted environments, fog development near the ocean, and hygroscopic cloud seeding.
The Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) was an international scientific expedition into the central Arctic sea ice to study the changing atmosphere-ice-ocean system and its key physical, chemical, and biological processes in a way that will support improved understanding and modeling of Arctic climate. The US Department of Energy’s Atmospheric Research Measurement (ARM) Program operated its second ARM Mobile Facility (AMF2) as a major contribution to the expedition, and the Atmospheric System Research (ASR) program supported this project to maximize the success of DOE’s involvement in MOSAiC. This project has enabled the successful collection of data through support of field operations plans, in-field operational implementation, oversight of real-time data quality, and representing DOE’s interests within the broader international MOSAiC endeavor. The project has promoted scientific research by facilitating and leading a number of efforts to develop value-added products that will support research, including products related to aerosol properties, trace gases, cloud properties, snowfall, the surface energy budget, and a merged product designed for model assessment. These products and related analyses have also contributed to numerous scientific publications on related themes as well as direct model evaluation. Lastly, the project has engaged in a great deal of communication and outreach activities that help to publicize and promote both MOSAiC and DOE’s specific contribution to a broad audience that includes the scientific community, program management, policy makers, and the general public.
Convective clouds play an important role in Earth’s climate system and are a known source of extreme weather. Gaps in our understanding of convective vertical motions, microphysics, and precipitation across a full range of aerosol and meteorological regimes continue to limit our ability to predict the occurrence and intensity of these cloud systems. To improve predictability, the National Science Foundation (NSF) sponsored a large field experiment entitled “Experiment of Sea Breeze Convection, Aerosols, Precipitation, and Environment (ESCAPE).” ESCAPE took place between 30 May and 30 September 2022 in the vicinity of Houston, Texas, because this area frequently experiences isolated deep convection that interacts with the region’s mesoscale circulations and its range of aerosol conditions. ESCAPE focused on collecting observations of isolated deep convection through innovative sampling and developing novel analysis techniques. This included the deployment of two research aircraft, the National Research Council of Canada Convair-580 and the Stratton Park Engineering Company Learjet, which combined conducted 24 research flights from 30 May to 17 June. On the ground, three mobile X-band radars and one mobile Doppler lidar truck equipped with soundings were deployed from 30 May to 28 June. From 1 August to 30 September 2022, a dual-polarization C-band radar was deployed and operated using a novel, multisensor agile adaptive sampling strategy to track the entire life cycle of isolated convective clouds. Analysis of the ESCAPE observations has already yielded preliminary findings on how aerosols and environmental conditions impact the convective life cycle.
Background: Humans emit approximately 30 million microbial cells per hour into their immediate vicinity. However, sampling of aerosolized microbial taxa (aerobiome) remains largely uncharacterized due to the complexity and limitations of sampling techniques, which are highly susceptible to low biomass and rapid sample degradation. Recently, there has been an interest in developing technology that collects naturally occurring water from the atmosphere, even within the built environment. Here, we analyze the feasibility of indoor aerosol condensation collection as a method to capture and analyze the aerobiome. Methods: Aerosols were collected via condensation or active impingement in a laboratory setting over the course of 8 h. Microbial DNA was extracted from collected samples and sequenced (16S rRNA) to analyze microbial diversity and community composition. Dimensional reduction and multivariate statistics were employed to identify significant (p < 0.05) differences in relative abundances of specific microbial taxa observed between the two sampling platforms. Results: Aerosol condensation capture is highly efficient with a yield greater than 95% when compared to expected values. Compared to air impingement, aerosol condensation showed no significant difference (ANOVA, p > 0.05) in microbial diversity. Among identified taxa, Streptophyta and Pseudomonadales comprised approximately 70% of the microbial community composition. Conclusion: The results suggest that condensation of atmospheric humidity is a suitable method for the capture of airborne microbial taxa reflected by microbial community similarity between devices. Future investigation of aerosol condensation may provide insight into the efficacy and viability of this new tool to investigate airborne microorganisms.
The data set of aerosol light absorption coefficients were collected by two tricolor absorption photometers (TAP; Brechtel Model 2901) in July and August, 2022 during the TRACER field campaign at the AMF1 site in La Porte, Texas. One of the TAPs at the La Porte site was an RGB model measuring aerosol light absorption at 652, 528, 467 nm, and the other was an UV model measuring absorption at the same red and green wavelengths but at an additional UV wavelength at 365 nm. Since TAP is a filter-based optical instrument using 47-mm glass fiber filters, the output absorption coefficients are corrected for filter loading and scattering effects based on a correction scheme developed in "Comment on ‘Calibration and Intercomparison of Filter-Based Measurements of Visible Light Absorption by Aerosols’" by John A. Ogren 2010. This uploaded dataset contains both the Ogren corrected absorption coefficients (column header with “ Ogren”) and the raw absorption coefficients without the correction scheme (column header with “_ Raw”). During the field campaign, the two TAPs operated side by side with a shared inlet at a flow rate of 2 lpm. In July, no inlet impactors/cyclones were installed; however, beginning in August, a PM2.5 cyclone inlet was installed.
Atmospheric aerosols play critical roles in the Earth’s energy budget, directly by scattering or absorbing solar and terrestrial radiation and indirectly by serving as seeds (nuclei) for cloud droplet and ice crystal formation and by depositing on snow and ice surface, thereby changing the surface albedo. These effects are dependent on aerosol particle size and chemical composition and impact the hydrological cycle as well. This project provided single-particle size and chemical composition measurements across the entire annual cycle in the high Arctic and in the Alaskan Arctic during fall – winter, addressing the most significant gaps in Arctic aerosol observational data. These needs were based on recent rapid sea ice loss across the entire Arctic, as well as the major annual delays in sea ice freeze-up during fall in the Chukchi Sea and increased wintertime sea ice fracturing in the Beaufort Sea, both off the North Slope of Alaska. Two DOE Atmospheric Radiation Measurement (ARM) field campaigns were conducted for atmospheric aerosol sampling. The Aerosols during the Polar Utqiagvik Night (APUN – ‘snow on ground’ in Iñupiaq) ARM field campaign at Utqagivik, Alaska was conducted from Oct. 28 – Dec. 22, 2018. Aerosol sizing instrumentation and a single-particle mass spectrometer were successfully deployed for size-resolved number concentration measurements and measurements of individual particle size and chemical composition, respectively. These results show the influence of locally-produced sea spray aerosol, with high cloud-forming potential, due to delayed sea ice freeze-up in the fall. During the 2019‐2020 international Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition, daily atmospheric aerosol particles were collected aboard the German icebreaker Polarstern in the Central Arctic from Nov. 2019 – Oct. 2020. Sea salt aerosol and marine organics were observed year-round during MOSAiC with varying morphologies and sources. These findings are important because most Arctic models do not include a sea spray aerosol source, despite this source increasing with declining sea ice extent. In addition to collecting new samples and data, this project also conducted further analysis of previously collected single-particle chemical composition measurements within the North Slope of Alaska oil fields and at Utqiaġvik, AK, during Aug. – Sep. 2015 and 2016 field campaigns. This work resulted in the discovery of chemical reactions of oil field combustion emissions occurring within fog droplets across the North Slope of Alaska and forming secondary aerosol, showing the impact of Arctic oil field emissions beyond black carbon aerosol and greenhouse gases. In addition, the distribution of chemical species across the aerosol population within the oil fields was quantified, using these data and a previously development framework. We also presented the first ambient evidence of the collision of two atmospheric particles resulting in formation of an organic-coated ammonium sulfate particle of marine origin, which has implications for cloud formation with declining sea ice extent. Overall, this project has elucidated connections between seawater biogeochemistry, resource extraction activities, atmospheric composition, clouds, and the energy budget of the Arctic region. The results of this project are expected to improve weather and sea ice forecasting for security and development in the Arctic and beyond.
The 2022 Hunga volcanic eruption injected a significant amount of water vapor and a moderate amount of sulfur dioxide into the stratosphere, causing observable responses in the climate system. We have developed a model–observation comparison project to investigate the evolution of volcanic water and aerosols and their impacts on atmospheric dynamics, chemistry, and climate, using several state-of-the-art chemistry climate models. The project goals are (1) to evaluate the current chemistry–climate models to quantify their performance in comparison to observations and (2) to understand atmospheric responses in the Earth system after this exceptional event and investigate the potential impacts in the projected future. To achieve these goals, we designed specific experiments for direct comparisons to observations, for example from balloons and the Microwave Limb Sounder satellite instrument. Experiment 1 consists of two sets of free-running ensemble experiments from 2022 to 2031: one with fixed sea-surface temperatures and sea ice and one with coupled ocean. These experiments will help to understand the long-term evolution of water vapor and aerosols; quantify HTHH effects on stratospheric and mesospheric temperatures, dynamics, and transport; understand the impact of dynamic changes on ozone chemistry; quantify the net radiative forcings; and evaluate any surface climate impact. Experiment 2 is a nudged-run experiment from 2022 to 2023 using observed meteorology. To allow participation of more climate models with varying complexities of aerosol simulation, we include two sets of simulations in Experiment 2: Experiment 2a is designed for models with internally generated aerosol, while Experiment 2b is designed for models using prescribed aerosol surface area density. This experiment will help to analyze H 2 O and aerosol evolution, quantify the net radiative forcings, understand the impacts on mid-latitude and polar O 3 chemistry, and allow close comparisons with observations.
Mineral dust contributes to more than half of the global aerosol loading. However, the radiative impacts of dust aerosols on planetary boundary layer (PBL) structure have not been explored sufficiently. During a typical dust storm event over Tarim Basin, dust aerosols exhibit a well-mixed distribution during the daytime in spite of a shallow layer of dust particles accumulated at higher altitudes. By contrast, nocturnal dust plumes are located near the surface due to stable stratification. We demonstrate that these differentiated vertical distributions determine the spatial heterogeneity of dust loading, radiative fluxes and PBL height variations. Dust aerosols cause daytime PBL suppression and nighttime PBL promotion through modulating surface and atmospheric radiative budgets. Specifically, dust-induced cooling effect within PBL directly inhibits the daytime PBL development. PBL suppression effect is then amplified by entrainment processes resulting in excessively low PBL height, especially for dust particles below but near the PBL top. Dust plumes weaken updrafts from PBL and downdrafts of the free atmosphere, which further reduce the entrainment mixing through attenuating horizontal and vertical advection, and eventually amplify PBL suppression. At night, near-surface dust aerosols stimulate a warm and unstable lower atmosphere, generate warm advection heating and promote the PBL development. Our study highlights the importance of specifying entrainment parameters and nighttime advection activities in quantifying the dust-PBL interactions.
The goal of this project has been to understand at the process level how the interaction of aerosols and cloud microphysics may alter the cloud response to climate change from the scale of turbulence to the global scale. Atmospheric aerosols (suspended particulates) have a unique role to play in the climate system. Anthropogenic aerosols may be an air pollution hazard and degrade human health. Their presence also results in the direct scattering or absorption of sunlight, with small net impacts on climate. But aerosols are also a key part of cloud formation, as the locations on which cloud droplets and ice crystals form. Understanding these Aerosol Cloud Interactions (ACI) is a critical uncertainty for climate models, including the Energy Exascale Earth System Model (E3SM), and affects how well models like E3SM can simulate the past and future. This work aims to understand cloud microphysics as well as the interaction of aerosol forcing and cloud feedback through improving our understanding of aerosol-cloud interactions (ACI) by looking at their uncertainty in critical environments at the process level. It will also contribute to the development of E3SM. Specific goals include: first, high level analysis of Perturbed Parameter Ensemble (PPE) simulations already available from the Community Earth System Model (CESM) and E3SM. Second, detailed analysis of recent changes to temperature and the role of aerosols.