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DOE OSTI2024

Aircraft Measurements from a U.S. Western Wildfire Demonstrating Day and Night Differences in the Chemical Composition and Optical Properties of Biomass Burning Aerosols and Their Atmospheric Evolution

The composition and transformations of biomass burning aerosols (BBA) have been measured onboard the NOAA Twin Otter research aircraft during the Fire Influence on Regional to Global Environments and Air Quality field study. Here, we analyze real-time aerosol mass spectrometry measurements across three flights during the afternoon, late afternoon, and night of August 28, 2019, for one midsized wildfire. Analysis of several metrics showed that the aerosol composition and optical properties varied depending on the burning conditions at the fire zone and the time of day the BBA was emitted, with substantial variations in the available sunlight. The total aerosol mass loadings were dominated by organic components with a much smaller contribution from inorganic species. A gradual buildup of organic material was observed during the afternoon as the plume aged, indicating the condensation of photochemically formed low-volatility oxidized organic compounds. Highly hygroscopic ammonium nitrate was the main inorganic component, suggesting potential water content in BBA particles and the likelihood of their aqueous-phase reactivity. Depletions of particle-phase NO 3 – and Cl – relative to carbon monoxide were observed in the late afternoon and nighttime plumes, respectively, aligning with known gas-particle partitioning thermodynamics and the heterogeneous chemistry of dissolved nitrate and chloride. The wavelength-dependent light absorption by aerosol species was higher for the plume sampled at night and showed no significant changes with plume age, despite observed trends in composition and mass downwind. These differences in particle composition and optical properties demonstrate that the processes involved in BBA aging are not uniform for the same wildfire over the course of the day and depend highly on when the BBA was emitted, as well as the burning phase at the emissions source.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Impacts of anthropogenic aerosols on fog in North China Plain

Fog poses a sever environmental problem in the North China Plain (NCP), China, which has been witnessing increases anthropogenic emission since the early 1980s. Here, this work first uses the WRF/Chem model coupled with the local anthropogenic emissions to simulate and evaluate a severe fog event occurring in NCP. Comparison of the simulations against observations shows that WRF/Chem well reproduces the general features of temporal evolution of PM 2.5 mass concentration, fog spatial distribution, visibility, and vertical profiles of temperature, water vapor content and relative humidity in the planetary boundary layer throughout the whole period of the fog event. Sensitivity studies are then performed with five different levels of anthropogenic emission as model inputs to systematically examine the comprehensive impacts of aerosols on fog microphysical, macrophysical, radiative, and dynamical properties. The results show that as aerosol concentration increases, fog droplet number concentration and liquid water content all increase nonlinearly; but effective radius decreases. Macrophysical properties (fog fraction, fog duration, fog height, and liquid water path) also increase nonlinearly with increasing aerosol concentration, with rates of changes smaller than microphysical properties. Further analysis reveals distinct aerosol effects on thermodynamic and dynamical conditions during different stages of fog evolution: increasing aerosols invigorate fog formation and development by enhancing longwave-induced instability, fog droplet condensation accompanying latent heat release, and thus turbulence, but delay fog dissipation by reducing surface solar radiation, surface sensible and latent heat fluxes, and thus suppressing turbulence during the dissipation stage.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Note: Real time optical sensing of alpha-radiation emitting radioactive aerosols based on solid state nuclear track detector

A sensitive radioactive aerosols sensor has been designed and developed. Its design guidance is based on the need for a low operational cost and reliable measurements to provide daily aerosol monitoring. The exposure of diethylene-glycol bis (allylcarbonate) to radiation causes modification of its physico-chemical properties like surface roughness and reflectance. In the present study, optical sensor based on the reflectance measurement has been developed with an aim to monitor real time presence of alpha radioactive aerosols emitted from thorium nitrate hydrate. The results shows that the fabricated sensor can detect 0.0157 kBq to 0.1572 kBq of radio activity by radioactive aerosols generated from (Th(NO{sub 3}){sub 4} ⋅ 5H{sub 2}O) at 0.1 ml/min flow rate. The proposed instrument will be helpful to monitor radioactive aerosols in/around a nuclear facility, building construction sites, mines, and granite polishing factories.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

TAMU TRACER: Targeted Mobile Measurements to Isolate the Impacts of Aerosols and Meteorology on Deep Convection

Difficulty in using observations to isolate the impacts of aerosols from meteorology on deep convection often stems from inability to resolve the spatiotemporal variations in the environment serving as the storm’s inflow region. During the DOE TRacking Aerosol Convection interactions ExpeRiment (TRACER) in June-September 2022, a Texas A&M University (TAMU) team conducted a mobile field campaign to characterize the meteorological and aerosol variability in airmasses that serve as inflow to convection across the ubiquitous mesoscale boundaries associated with the sea- and bay-breezes in the Houston, Texas, region. These boundaries propagate inland over the fixed DOE Atmospheric Radiation Measurement (ARM) sites. However, convection occurs on either or both the continental or maritime sides or along the boundary. The maritime and continental airmasses serving as convection inflow may be quite distinct, with different meteorological and aerosol characteristics that fixed-site measurements cannot simultaneously sample. Thus, a primary objective of TAMU TRACER was to provide mobile measurements similar to those at the fixed sites, but in the opposite airmass across these moving mesoscale boundaries. TAMU TRACER collected radiosonde, lidar, aerosol, cloud condensation nuclei (CCN), and ice nucleating particle (INP) measurements on 29 enhanced operations days covering a variety of maritime, continental, outflow, and pre-frontal airmasses. This paper summarizes the TAMU TRACER deployment and measurement strategy, instruments, available datasets, and provides sample cases highlighting differences between these mobile measurements and those made at the ARM sites. We also highlight the exceptional TAMU TRACER undergraduate student participation in high impact learning activities through forecasting and field deployment opportunities.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Tropical Pacific Ocean Dynamical Response to Short-Term Sulfate Aerosol Forcing

Abstract The large-scale and long-term climate impacts of anthropogenic sulfate aerosols consist of Northern Hemisphere cooling and a southward shift of the tropical rain belt. On interannual time scales, however, the response to aerosols is localized with a sizable imprint on local ocean–atmosphere interaction. A large concentration of anthropogenic sulfates over Asia may impact ENSO by modifying processes and interactions that generate this coupled ocean–atmosphere variability. Here, we use climate model experiments with different degrees of ocean–atmosphere coupling to study the tropical Pacific response to an abrupt increase in anthropogenic sulfates. These include an atmospheric general circulation model (GCM) coupled to either a full-ocean GCM or a slab-ocean model, or simply forced by climatology of sea surface temperature. Comparing the responses helps differentiate between the fast atmospheric and slow ocean-mediated responses, and highlights the role of ocean–atmosphere coupling in the latter. We demonstrate the link between the Walker circulation and the equatorial Pacific upper-ocean dynamics in response to increased sulfate aerosols. The local surface cooling due to sulfate aerosols emitted over the Asian continent drives atmospheric subsidence over the equatorial west Pacific. The associated anomalous circulation imparts westerly momentum to the underlying Pacific Ocean, leading to an El Niño–like upper-ocean response and a transient warming of the east equatorial Pacific Ocean. The oceanic adjustment eventually contributes to its decay, giving rise to a damped oscillation of the tropical Pacific Ocean in response to abrupt anthropogenic sulfate aerosol forcing.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Moving beyond the Aerosol Climatology of WRF-Solar: A Case Study over the North China Plain

Numerical weather prediction (NWP), when accessible, is a crucial input to short-term solar power forecasting. WRF-Solar, the first NWP model specifically designed for solar energy applications, has shown promising predictive capability. Nevertheless, few attempts have been made to investigate its performance under high aerosol loading, which attenuates incoming radiation significantly. The North China Plain is a polluted region due to industrialization, which constitutes a proper testbed for such investigation. Here, in this paper, aerosol direct radiative effect (DRE) on three surface shortwave radiation components (i.e., global, beam, and diffuse) during five heavy pollution episodes is studied within the WRF-Solar framework. Results show that WRF-Solar overestimates instantaneous beam radiation up to 795.3 W m -2 when the aerosol DRE is not considered. Although such overestimation can be partially offset by an underestimation of the diffuse radiation of about 194.5 W m -2 , the overestimation of the global radiation still reaches 160.2 W m -2 . This undesirable bias can be reduced when WRF-Solar is powered by Copernicus Atmosphere Monitoring Service (CAMS) aerosol forecasts, which then translates to accuracy improvements in photovoltaic (PV) power forecasts. This work also compares the forecast performance of the CAMS-powered WRF-Solar with that of the European Centre for Medium-Range Weather Forecasts model. Under high aerosol loading conditions, the irradiance forecast accuracy generated by WRF-Solar increased by 53.2% and the PV power forecast accuracy increased by 6.8%.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

ARM Aerosol Measurement Science Group Strategic Planning Workshop 2017

The Aerosol Measurement Science Group (AMSG) was tasked with evaluating the status of the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Climate Research Facility’s existing aerosol instrumentation, measurement strategies, and data products in the context of ARM and Atmospheric System Research (ASR) science directions and the current and future needs of ARM data users. A workshop comprising the AMSG members and external experts in aerosol measurements was convened in February 2017 to delineate specific measurements and efforts in data product development that would align the ARM aerosol program investments well with the needs of the scientific community. Topics of discussion in the workshop included priority measurements and instrumentation to be deployed at the range of ARM sites, physical system configurations that impact the character of observables and quality of observations, calibration strategies, overarching deployment strategies for aerosol observing systems (AOS), and communication about and accessibility of data. This report provides an account of workshop discussions and prioritized recommendations for ARM supported activities that will bring measurements to quality and science-ready data products relevant to the ASR and larger science community.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Aerosol Inlets for a Mid-Sized Uncrewed Aerial System (UAS)

The purpose of this technical report is to document the efforts to design and test two inlet systems for aerosol sampling suitable for deployment on a medium-sized fixed-wing Uncrewed Aerial System (UAS). This work, which was supported by the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) user facility, was conducted at the Pacific Northwest National Laboratory (PNNL) for the ARM Aircraft Facility (AAF) starting in November 2017. The current work is a part of AAF efforts to instrument the ArcticShark (a mid-sized UAS owned and operated by the AAF) for atmospheric research and develop a scientific payload for deployment on a similar-sized UAS with minimal adaptation and integration. An aerosol inlet system is necessary to sample and transport ambient air sample to the scientific instrumentation with minimal distortions to the aerosols. Two isokinetic aerosol inlets were designed: the first is a simple passive system for a single instrument suitable to be installed in a wing pylon; the second is a system with active control designed to sample and distribute air among several heterogeneous instruments and to provide basic humidity control of the air sample so that the measured aerosol parameters should correspond to “dry” conditions (a common requirement). Both systems could be easily adapted for deployment on another platform and/or with a different set of instrumentation. Several conducted flight tests showed that the inlets’ performance met our design goals.

42 ENGINEERING↗

DOE OSTI2022

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

SCILLA Secondary Aerosol Volume Concentration Airborne Data

This data set contains secondary aerosol volume concentration in cubic micrometers per cubic centimeter (um^3/cm^3). The aerosol was generated in an oxidation flow reactor (OFR) and its volume concentration measured with a scanning mobility particle sizer (SMPS). Both components were designed and built at the University of California Riverside. Ambient particles were removed with a Teflon filter upstream of the OFR and then pure ammonium sulfate particles were added to create a stable aerosol surface area on which low-volatility oxidation products condense. High concentrations of hydroxyl radical (OH) formed inside the OFR accelerate the oxidative chemistry that would typically occur over a period of several days in the atmosphere, resulting in the production of secondary aerosol from precursor gases present in the ambient air. Concentrations of added ozone and water vapor were controlled to produce the desired and approximately constant level of photochemical aging. The reactor temperature was controlled, while the pressure was not, and was always slightly lower than that of the sampled outside air. Sampled air was pulled from above the Naval Postgraduate School’s (NPS) Twin Otter aircraft through a rear-facing, ¼” OD PFA Teflon tube. The sample stream was split between the OFR and several gas analyzers (NOx, CO, O3, and H2O). Though not contained in these files, data from an aerosol mass spectrometer intermittently operated downstream of the OFR are also available.

{"secondary aerosol concentration",aerosol_concent↗

DOE OSTI2025

BSEC Air Quality: Stationary Aerosol Composition and Mass Concentration at Baltimore

Data is 10-min average mass composition and mass concentration from the TOF-ACSM-X. TOF-ACSM-X reports fine (less than 2.5 um diameter) non-refractory aerosol, including organic aerosol, sulfate, nitrate, ammonium, and non-refractory chloride. Also reported is the elemental ratios determined for organic aerosol (O/C, H/C, and organic matter to organic carbon ratio, OM/OC). Finally, ion ratios of key ions used for identifying sources, ammonium balance, and fractional contribution of organic nitrate aerosol to total aerosol nitrate has been included.

aerosol↗

NASA NTRS2014

Near-Cloud Aerosol Properties from the 1 Km Resolution MODIS Ocean Product

This study examines aerosol properties in the vicinity of clouds by analyzing high-resolution atmospheric correction parameters provided in the MODIS (Moderate Resolution Imaging Spectroradiometer) ocean color product. The study analyzes data from a 2 week long period of September in 10 years, covering a large area in the northeast Atlantic Ocean. The results indicate that on the one hand, the Quality Assessment (QA) flags of the ocean color product successfully eliminate cloud-related uncertainties in ocean parameters such as chlorophyll content, but on the other hand, using the flags introduces a sampling bias in atmospheric products such as aerosol optical thickness (AOT) and Angstrom exponent. Therefore, researchers need to select QA flags by balancing the risks of increased retrieval uncertainties and sampling biases. Using an optimal set of QA flags, the results reveal substantial increases in optical thickness near clouds-on average the increase is 50% for the roughly half of pixels within 5 km from clouds and is accompanied by a roughly matching increase in particle size. Theoretical simulations show that the 50% increase in 550nm AOT changes instantaneous direct aerosol radiative forcing by up to 8W/m2 and that the radiative impact is significantly larger if observed near-cloud changes are attributed to aerosol particles as opposed to undetected cloud particles. These results underline that accounting for near-cloud areas and understanding the causes of near-cloud particle changes are critical for accurate calculations of direct aerosol radiative forcing.

near-cloud aerosols↗

DOE OSTI2016

Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particles that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.

spherical organic particles, Manaus pollution plum↗

DOE OSTI2016

Comparison of aerosol optical properties above clouds between POLDER and AeroCom models over the South East Atlantic Ocean during the fire season

Aerosol properties above clouds have been retrieved over the South East Atlantic Ocean during the fire season 2006 using satellite observations from POLDER (Polarization and Directionality of Earth Reflectances). From June to October, POLDER has observed a mean Above-Cloud Aerosol Optical Thickness (ACAOT) of 0.28 and a mean Above-Clouds Single Scattering Albedo (ACSSA) of 0.87 at 550nm. These results have been used to evaluate the simulation of aerosols above clouds in 5 AeroCom (Aerosol Comparisons between Observations and Models) models (GOCART, HadGEM3, ECHAM5-HAM2, OsloCTM2 and SPRINTARS). Most models do not reproduce the observed large aerosol load episodes. The comparison highlights the importance of the injection height and the vertical transport parameterizations to simulate the large ACAOT observed by POLDER. Moreover, some models overestimate the ACSSA. In accordance with recent recommendations of the black carbon refractive index, a higher prescription of the imaginary part allows a better comparison with POLDER’s ACSSA.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2016

Toward reconciling the influence of atmospheric aerosols and greenhouse gases on light precipitation changes in Eastern China

The attribution of the widely observed shifted precipitation extremes to different forcing agents represents a critical issue for understanding of changes in the hydrological cycle. To compare aerosol and greenhouse-gas effects on the historical trends of precipitation intensity, we performed AMIP-style NCAR/DOE CAM5 model simulations from 1950-2005 with and without anthropogenic aerosol forcings. Precipitation rates at every time step in CAM5 are used to construct precipitation probability distribution functions. By contrasting the two sets of experiments, we found that the global warming induced by the accumulating greenhouse gases is responsible for the changes in precipitation intensity at the global scale. However, regionally over the Eastern China, the drastic increase in anthropogenic aerosols primarily accounts for the observed light precipitation suppression since the 1950s. Here, compared with aerosol radiative effects, aerosol microphysical effect has a predominant role in determining the historical trends of precipitation intensity in Eastern China.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Broadband optical properties of biomass-burning aerosol and identification of brown carbon chromophores

The radiative effects of biomass burning aerosols on regional and global scale is substantial. Accurate modeling of the radiative effects of smoke aerosols require wavelength-dependent measurements and parameterizations of their optical properties in the UV and visible spectral ranges along with improved description of their chemical composition. To address this issue, we used a recently developed approach to retrieve the time- and spectral-dependent optical properties of ambient biomass burning aerosols between 300 and 650 nm wavelength during a regional bonfire festival in Israel. We report that during the biomass burning event, the overall absorption at 400 nm increased by about two orders of magnitude, changing the size-weighted single scattering albedo from a background level of 0.95 to 0.7. Based on the new retrieval method, we provide parameterizations of the wavelength-dependent effective complex refractive index from 350 to 650 nm for freshly emitted and aged biomass burning aerosols. In addition, PM 2.5 filter samples were collected for detailed off-line chemical analysis of the water soluble organics that contribute to light absorption. Nitrophenols were identified as the main organic species responsible for the increased absorption at 400-500 nm. These include species such as 4- nitrocatechol, 4-nitrophenol, nitro-syringol and nitro-guaiacol; oxidation-nitration products of methoxyphenols, known products of lignin pyrolysis. Our findings emphasize the importance of both primary and secondary organic aerosol from biomass burning in absorption of solar radiation and in effective radiative forcing.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Radiative and Chemical Response to Interactive Stratospheric Sulfate Aerosols in Fully Coupled CESM1(WACCM)

We present a new version of the Community Earth System Model, version 1 (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) featuring numerous improvements that are unique among earth system models. Improved horizontal resolution, dynamics, and chemistry now provide the development of an internally generated quasi-biennial oscillation, and significant improvements to temperatures and ozone throughout the stratosphere. The prognostic treatment of stratospheric sulfate aerosols is shown to represent well the evolution of stratospheric aerosol optical depth and perturbations to solar and longwave radiation following volcanic eruptions. We identify the inclusion of interactive OH chemistry as crucial to the study of aerosol formation following large inputs of SO 2 to the stratosphere. We show that depletion of OH levels within the dense SO 2 cloud in the first weeks following the June 1991 eruption of Mt. Pinatubo significantly prolonged the e-folding decay time for SO 2 oxidation to 47 days. Previous observational and model studies showing a 30-day decay time have not accounted for the large initial losses of SO 2 on ash and ice in the first 7-9 days following the eruption, and have not correctly accounted for OH depletion. The completeness of the chemistry, dynamics, and aerosol microphysics in WACCM uniquely qualify it for studies of stratospheric sulfate aerosol geoengineering.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2018

Use of an Open Port Sampling Interface Coupled to Electrospray Ionization for the On-Line Analysis of Organic Aerosol Particles

A simple design for an open port sampling interface coupled to electrospray ionization (OPSI-ESI) is presented for the analysis of organic aerosols. The design uses minimal modifications to a Bruker electrospray (ESI) emitter to create a continuous flow, self-aspirating open port sampling interface. Considerations are presented for introducing aerosol to the open port sampling interface including aerosol gas flow and solvent flow rates. The device has been demonstrated for use with an aerosol of nicotine as well as aerosol formed in the pyrolysis of biomass. Upon comparison with extractive electrospray ionization (EESI), this device has similar sensitivity with increased reproducibility by nearly a factor of three. The device has the form factor of a standard Bruker/Agilent ESI emitter and can be used without any further instrument modifications. .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗