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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

The missing base molecules in atmospheric acid–base nucleation

Abstract Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid–base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles. Here we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass spectrometers. We demonstrate that forming (H2SO4)1(amine)1 is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of (H2SO4)1(amine)1 is a major pathway for the initial growth of H2SO4 clusters. The proposed mechanism is very consistent with measured new particle formation in urban Beijing, in which dimethylamine is the key base for H2SO4 nucleation while other bases such as ammonia may contribute to the growth of larger clusters. Our findings further underline the fact that strong amines, even at low concentrations and when undetected in the smallest clusters, can be crucial to particle formation in the planetary boundary layer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Mechanism of Microseismic Generation During Hydraulic Fracturing - With Evidence From HFTS 2 Observations

The objective of this study is to understand how microseismic events are generated during hydraulic fracturing, as well as the role of geomechanical conditions (i.e., stress and mechanical stratigraphy) in this process. In the industry, microseismic event clouds have been generally used as an “outer-boundary” of the “stimulated reservoir volume” (SRV). However, by comparing with other surveillance data (Low frequency Distributed Acoustic Sensing, or LF-DAS strain) in the Hydraulic Fracturing Test Site (HFTS) 2 experiment, we show that this assumption is fundamentally flawed. The HFTS 2 data has three unique observations that have not been commonly observed in other datasets: 1. Due to influence of offset pad depletion, microseismic data shows that hydraulic fractures from the child well can propagate over 3000 feet into the depleted low stress zone. 2. By comparing microseismic and horizontal fiber LF-DAS strain data, we observe that microseismic event cloud does not necessarily reflect the created hydraulic fracture volume. Particularly, the extent of microseismic event clouds near heel stages are much shorter than what is shown with LF-DAS strain data. 3. Microseismic event magnitudes are larger in the depleted regions. Through geomechanical analysis, we demonstrate that the “bedding-plane-slip” model is likely the mechanism for microseismic generation during hydraulic fracturing. Furthermore, this model successfully explains the above field observations from HFTS 2 experiment. We also provide a quantitative relationship connecting the microseismic event magnitude with fracture width increment and layer mechanical property contrast.

58 GEOSCIENCES↗
DOE OSTI2022

Interpretation of HFTS 2 Microseismic Data Using Bedding-Plane-Slip Mechanism

Summary The objective of this study is to understand how microseismic events are generated during hydraulic fracturing, as well as the role of geomechanical conditions (i.e., stress and mechanical stratigraphy) in this process. In the industry, microseismic event clouds have been generally used as an “outer boundary” of the “stimulated reservoir volume” (SRV). However, by comparing with other surveillance data (low-frequency distributed acoustic sensing, or LF-DAS, strain) in the Hydraulic Fracturing Test Site (HFTS) 2 experiment, we show that this assumption is fundamentally flawed. The HFTS 2 data have three unique observations that have not been commonly observed in other datasets: (1) Due to the influence of offset pad depletion, microseismic data show that hydraulic fractures from the child well can propagate over 3,000 ft into the depleted low-stress zone. (2) By comparing microseismic and horizontal fiber LF-DAS strain data, we observe that the microseismic event cloud does not necessarily reflect the created hydraulic fracture volume. Particularly, the extent of microseismic event clouds near heel stages is much shorter than what is shown with LF-DAS strain data. (3) Microseismic event magnitudes are larger in the depleted regions. Through geomechanical analysis, we demonstrate that the “bedding-plane-slip” model is likely the mechanism for microseismic generation during hydraulic fracturing. This model successfully explains the above field observations from the HFTS 2 experiment. We also provide a quantitative relationship connecting the microseismic event magnitude with fracture width increment and layer mechanical property contrast.

Engineering↗
DOE OSTI2021

Mass accommodation and gas–particle partitioning in secondary organic aerosols: dependence on diffusivity, volatility, particle-phase reactions, and penetration depth

Abstract. Mass accommodation is an essential process for gas–particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as being incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface–bulk exchange, it can be important for viscous semi-solid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas–particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective mass accommodation coefficient αeff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particle-phase reaction rate coefficient. Application of αeff in the traditional Fuchs–Sutugin approximation of mass-transport kinetics at the gas–particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (kinetic multilayer model of gas–particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Model for Simulating Aerosol Interactions and Chemistry, MOSAIC; Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semi-solid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in the case of low-volatility compounds, whereas it can decrease by several orders of magnitude in the case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs–Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient, regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models. While kinetic limitations may not be critical for partitioning into liquid SOA particles in the planetary boundary layer (PBL), the effects are likely important for amorphous semi-solid or glassy SOA in the free and upper troposphere (FT–UT) as well as in the PBL at low relative humidity and low temperature.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Boundary Layer Structures Over the Northwest Atlantic Derived From Airborne High Spectral Resolution Lidar and Dropsonde Measurements During the ACTIVATE Campaign

The Planetary Boundary Layer height (PBLH) is essential for studying PBL and ocean-atmosphere interactions. Marine PBL is usually defined to include a mixed layer (ML) and a capping inversion layer. The ML height (MLH) estimated from the measurements of aerosol backscatter by a lidar was usually compared with PBLH determined from radiosondes/dropsondes in the past, as the PBLH is usually similar to MLH in nature. However, PBLH can be much greater than MLH for decoupled PBL. Here, in this study, we evaluate the retrieved MLH from an airborne lidar (HSRL-2) by utilizing 506 co-located dropsondes during the ACTIVATE field campaign over the Northwest Atlantic from 2020 to 2022. First, we define and determine the MLH and PBLH from the temperature and humidity profiles of each dropsonde, and find that the MLH values from HSRL-2 and dropsondes agree well with each other, with a coefficient of determination of 0.66 and median difference of 18 m. In contrast, the HSRL-2 MLH data do not correspond to dropsonde-derived PBLH, with a median difference of -47 m. Therefore, we modify the current operational and automated HSRL-2 wavelet-based algorithm for PBLH retrieval, decreasing the median difference significantly to -8 m. Further data analysis indicates that these conclusions remain the same for cases with higher or lower cloud fractions, and for decoupled PBLs. These results demonstrate the potential of using HSRL-2 aerosol backscatter data to estimate both marine MLH and PBLH and suggest that lidar-derived MLH should be compared with radiosonde/dropsonde-determined MLH (not PBLH) in general.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

African dust transported to Barbados in the wintertime lacks indicators of chemical aging

The chemical processing (“aging”) of mineral dust is thought to increase dust light-scattering efficiency, cloud droplet activation, and nutrient solubility. However, the extent of African dust aging during long-range transport to the western Atlantic is poorly understood. Here, we explore African dust aging in wintertime samples collected from Barbados when dust is transported at lower altitudes. Ion chromatography (IC) analysis indicates that the mass concentrations of bulk nitrate, sulfate, and oxalate increase, relative to background conditions, when African dust reaches Barbados after transatlantic transport, indicating dust aging. However, aerosol mixing-state analysis from computer-controlled scanning electron microscopy with energy dispersive X-ray spectroscopy (CCSEM/EDX) indicates that approximately 67 % of dust particles are internally mixed with sea salt, while only about 26 % of dust particles contain no internally mixed components. SEM/EDX elemental mapping and time-of-flight secondary ion mass spectrometry (TOF-SIMS) reveals that within internally mixed dust and sea salt particles, only sea salt components contain signs of aging as indicated by the loss of chloride and acquisition of nitrate and/or sulfate. Our results suggest that chemical aging may only modestly increase the solubility of nutrients in African dust during long-range transport. Because most dust that we measured was internally mixed with sea salt, chemical aging is not necessarily required to increase the hygroscopicity of dust, at least in the lower boundary layer. Further, our findings have implications for understanding the release of halogens from sea salts, which may be enhanced in internally mixed dust and sea salt particles.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Evaluation of Techniques for Vegetation Removal from UAV-Based Photogrammetric DSM near WIPP Land Withdrawal Act Boundary, NM

The Waste Isolation Pilot Plant is located within New Mexico's karst landscape and is the United States' only deep geologic radioactive waste repository which isolates transuranic waste from defense activities underground in a bedded salt formation. Characteristic karst topography in this region is made up of material (such as limestone) that can be dissolved by water over a long period of time, and includes features such as springs, surface streams, sinking streams, caves, and sinkholes. Karst features can potentially impact the integrity of the waste repository in the future and compromise WIPP's performance, particularly when coupled with incompatible land-use activities within the Land Withdrawal Act (LWA) boundary as well as increased water withdrawals outside the LWA. In order to better capture the ground surface topography to support hydrology modeling efforts, the U.S. DOE has enlisted FIU to develop a high-resolution digital elevation model (DEM). In a previous field study, a high-resolution digital surface model (DSM) of an adjacent representative site, Basin 6, was developed by photogrammetry using aerial images captured with unmanned aerial vehicles. The DSM generated was based on point clouds representing the entire landscapes, including points of terrain, vegetation and infrastructure. These above-ground features need to be removed to create a DSM/DEM with good representation of the bare ground. In recent years, many techniques including both pre- and post-processing of DSMs, were developed for vegetation removal with varied success. This research focuses on applying and comparing various vegetation removal methods using point clouds generated of the Basin 6 pilot study area. The 3D RGB-based point cloud classification using Python scripts was a modification of the procedure by Themistocleous (2019). The method using Liblas classifies the point cloud three-dimensionally, whereas the method by Themistocleous (2019) is two-dimensional. The preliminary result of the method using Liblas, however, still had a large amount of vegetation remaining compared to the Pix4D Machine Learning method. The vegetation layer remains highly visible in the DEMs processed using the vegetation indices as opposed to the Pix4D Machine Learning method, which produces a DEM where mostly bare ground is seen. Further modifications to the input parameters are required to improve the vegetation vs. bare ground classification using this approach. The next step will be to improve the method using Liblas and to also test other vegetation removal methods found in the literature review to compare them against the two described here.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Texas A&M University Mobile Facility Measurements during TRACER (Field Campaign Report)

One of the main goals of the U.S Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Tracking Aerosol Convection Interactions Experiment (TRACER) near Houston, Texas is to improve understanding of how meteorology and aerosols impact storm dynamical and microphysical processes in deep convection to better constrain and improve their model representation. The Houston area is strongly influenced by sea- and bay-breeze circulations that generate convergence and help to initiate and organize deep convection. To properly isolate and understand the roles of varied meteorological conditions and cloud condensation nuclei (CCN) and ice nucleation particles (INP) distributions in different air masses, co-located thermodynamic, kinematic, and aerosol vertical profile observations are needed. The focus of this campaign was to provide key measurements in air masses both in front of and behind sea/bay breeze fronts moving through the greater Houston area to sample the airmass heterogeneity. The overarching scientific goal of this campaign is to understand how the vertical distributions of both CCN and INP correspond to the inflow layer of deep convection in maritime, background continental, and polluted continental air masses, and how these variations influence deep convection. To fully sample the heterogeneity in both meteorological conditions and aerosols across the sea-breeze front (SBF), Texas A&M University (TAMU) deployed a InterMet 3050A 403 MHz mobile unit launching iMet-4 radiosondes and the new Rapid Onsite Atmospheric Measurement Van (ROAM-V) for aerosol sampling during the TRACER intensive operational period (IOP) from June to September 2022. The suite of instruments deployed on ROAM-V included a condensation particle counter (CPC; GRIMM Model 5.403 CPC), scanning mobility particle sizer (SMPS; TSI 3750 detector, TSI 3082 classifier, TSI 3088 neutralizer, TSI 3081A differential mobility analyzer), cloud condensation nuclei counter (Droplet Measurement Technologies CCN counter), micropulse lidar (Droplet Measurement Technologies micropulse lidar [miniMPL]), and a Davis Rotating Uniform size-cut Monitor (DRUM; DRUMAir 4-DRUM). Before sampling at each location, the latitude and longitude were recorded using the Global Positioning System (GPS) on the phone application “My Altitude”. The DRUM data were collected as part of a closely related ARM field campaign and also supported by DOE Atmospheric System Research grant DE-SC0021047. The TAMU team sampled these airmass heterogeneities by strategically choosing deployment sites in a different airmass than the ARM fixed sites in La Porte and Guy, Texas. On days when the sea/bay breeze boundary was pushing inland, the TAMU team would usually sample the airmass on the maritime side of the SBF at a coastal site in Galveston, Texas in the early afternoon (1730-1900 UTC) and then move inland ahead of the SBF to sample the airmass on the continental side during late afternoon (2030-2230). Figure 1 shows the Galveston maritime site and the array of sites for the late afternoon continental measurements.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Exploring the impact of surface topography on Rayleigh-Bénard dry convection in the Pi cloud chamber using OpenFOAM: In cylindrical and rectangular geometries

The Pi convection-cloud chamber can generate steady-state turbulence in both rectangular and cylindrical shapes via Rayleigh-Bénard convection (RBC) by maintaining warm bottom and cold top surfaces. Although most experiments in the Pi chamber were conducted in cylindrical shapes, all previous Pi chamber simulations were conducted in a rectangular shape due to the limitations of those models to discretize a cylindrical domain when using the finite difference method therein. Here, we use OpenFOAM, an open-source finite-volume-based Computational Fluid Dynamics (CFD) software package, to conduct Large-Eddy Simulation (LES) of dry RBC in the Pi chamber at high Rayleigh numbers (10 8 to 10 9 ). Results show that large-scale circulation (LSC) direction varies in the chamber with a constant side wall temperature. Imposing a slight temperature imbalance at the side wall ranging from 0.1 to 0.7 degrees can lock the LSC, aligning better with Pi chamber observations, particularly at higher Rayleigh numbers. In addition, we examine the impact of surface topography on LSC and heat transfer in RBC systems within cylindrical and rectangular shapes under varying conditions. Results show that roughing top/bottom surfaces by adding bars of a few tens millimeters height can strengthen thermal plumes and enhance temperature fluctuations in the chamber. Furthermore, we observe that different bar height configurations lead to notable changes in LSC orientation and thermal stratification, highlighting the complex interactions between surface features and convection patterns. This finding highlights how surface topography and chamber geometry affect Rayleigh-Bénard convection, improving understanding of turbulent heat transfer and atmospheric boundary-layer processes. Direct Numerical Simulations (DNS) are also conducted to validate LES results. In conclusion, while LES effectively captures qualitative behaviors seen in DNS, it tends to underestimate velocity variances near walls, illustrating a trade-off between computational efficiency and accuracy.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Undersizing of aged African biomass burning aerosol by an ultra-high-sensitivity aerosol spectrometer

The ultra-high-sensitivity aerosol spectrometer (UHSAS) differs from most other optical particle spectrometers by using a high-power infrared (IR) laser to detect small particles and reduce the sizing ambiguity due to the non-monotonicity of scattering with particle size. During the NASA ORACLES project (ObseRvations of Aerosols above CLouds and their intEractionS) over the southeast Atlantic Ocean, the UHSAS clearly undersized particles in the biomass burning plume extending from southern Africa. Since the horizontal and vertical extent of the plume was vast, the NASA P-3B research aircraft often flew through a fairly uniform biomass burning plume for periods exceeding 30 min, sufficient time to explore the details of the UHSAS response by selecting single particle sizes with a differential mobility analyzer (DMA) and passing them to the UHSAS. This was essentially an in-flight calibration of the UHSAS using the particles of interest. Two modes of responses appeared. Most particles were undersized by moderate amounts, ranging from not at all for 70 nm aerosols to 15 % for 280 nm particles. Mie scattering calculations show that composition-dependent refractive index of the particles cannot explain the pattern. Heating of brown carbon or tarballs in the beam causing evaporation and shrinking of the particles is the most plausible explanation, though mis-sizing due to non-sphericity cannot be ruled out. A small fraction (10 %–30 %) of the particles were undersized by 25 % to 35 %. Those were apparently the particles containing refractory black carbon. Laboratory calibrations confirm that black carbon is drastically undersized by the UHSAS, because particles heat to their vaporization point and shrink. A simple empirical correction equation was implemented that dramatically improves agreement with DMA distributions between 100 and 500 nm. It raised the median particle diameter by 18 nm, from 163 to 181 nm, during the August 2017 deployment and by smaller amounts during deployments with less intense pollution. Calculated scattering from UHSAS size distributions increased by about 130 %, dramatically improving agreement with scattering measured by nephelometers. The correction is only valid in polluted instances; clean marine boundary layer and free troposphere aerosols behaved more like the calibration spheres. We were unable to directly test the correction between 500 and 1000 nm, though aerodynamic particle sizer (APS) data appear to show that the correction is poor at the largest diameters, which is no surprise as the composition of those particles is likely to be quite different than that of the accumulation mode. This adds to the evidence that UHSAS data must be treated cautiously whenever the aerosol may absorb infrared light. Similar corrections may be required whenever brown carbon aerosol is present.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Identifying a regional aerosol baseline in the eastern North Atlantic using collocated measurements and a mathematical algorithm to mask high-submicron-number-concentration aerosol events

Abstract. High-time-resolution measurements of in situ aerosol and cloud properties provide the ability to study regional atmospheric processes that occur on timescales of minutes to hours. However, one limitation to this approach is that continuous measurements often include periods when the data collected are not representative of the regional aerosol. Even at remote locations, submicron aerosols are pervasive in the ambient atmosphere with many sources. Therefore, periods dominated by local aerosol should be identified before conducting subsequent analyses to understand aerosol regional processes and aerosol–cloud interactions. Here, we present a novel method to validate the identification of regional baseline aerosol data by applying a mathematical algorithm to the data collected at the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility in the eastern North Atlantic (ENA). The ENA central facility (C1) includes an aerosol observing system (AOS) for the measurement of aerosol physical, optical, and chemical properties at time resolutions from seconds to minutes. A second temporary supplementary facility (S1), located ∼0.75 km from C1, was deployed for ∼1 year during the Aerosol and Cloud Experiments (ACE-ENA) campaign in 2017. First, we investigate the local aerosol at both locations. We associate periods of high submicron number concentration (Ntot) in the fine-mode condensation particle counter (CPC) and size distributions from the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) as a function of wind direction using a meteorology sensor with local sources. Elevated concentrations of Aitken-mode (< 100 nm diameter) particles were observed in correspondence with the wind directions associated with airport operations. At ENA, the Graciosa Airport and its associated activities were found to be the main sources of high-concentration aerosol events at ENA, causing peaks in 1 min Ntot that exceeded 8000 and 10 000 cm−3 at C1, in summer and winter, respectively, and 5000 cm−3 at S1 in summer. Periods with high Ntot not associated with these wind directions were also observed. As a result, the diverse local sources at ENA yielded a poor relationship between Ntot measurements collected at C1 and S1 (R2=0.03 with a slope =0.05±0.001). As a first approach to mask these events, the time periods when the wind direction was associated with the airport operations (west to northwest and southeast to south at C1 and east to south at S1) were applied. The meteorological masks removed 38.9 % of the data at C1 and 43.4 % at S1, and they did not significantly improve the relationship between the two sites (R2=0.18 with a slope =0.06±0.001). Due to the complexity of high-Ntot events observed at ENA, we develop and validate a mathematical ENA Aerosol Mask (ENA-AM) to identify high-Ntot events using 1 min resolution data from the AOS CPC at C1 and S1. After its parameterization and application, ENA-AM generated a high correlation between Ntot in the summer at C1 and S1 (R2=0.87 with a slope =0.84±0.001). We identified the regional baseline at ENA to be 428±228 cm−3 in the summer and 346±223 cm−3 in the winter. Lastly, we compared masked measurements from the AOS with the ARM Aerial Facility (AAF) during flights over C1 in the summer to understand submicron aerosol vertical mixing over C1. The high correlation (R2=0.71 with a slope of 1.04±0.01) observed between C1 and the AAF Ntot collected within an area of 10 km surrounding ENA and at altitudes < 500 m indicated that the submicron aerosol at ENA was well mixed within the first 500 m of the marine boundary layer during the month of July during ACE-ENA. Our novel method for determining a regional aerosol baseline at ENA can be applied to other time periods and at other locations with validation by a secondary site or additional collocated measurements.

54 ENVIRONMENTAL SCIENCES↗