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241 records · Page 14

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DOE OSTI2021

Aerosol responses to precipitation along North American air trajectories arriving at Bermuda

North American pollution outflow is ubiquitous over the western North Atlantic Ocean, especially in winter, making this location a suitable natural laboratory for investigating the impact of precipitation on aerosol particles along air mass trajectories. We take advantage of observational data collected at Bermuda to seasonally assess the sensitivity of aerosol mass concentrations and volume size distributions to accumulated precipitation along trajectories (APT). The mass concentration of particulate matter with aerodynamic diameter less than 2.5 µm normalized by the enhancement of carbon monoxide above background (PM 2.5 /ΔCO) at Bermuda was used to estimate the degree of aerosol loss during transport to Bermuda. Results for December–February (DJF) show that most trajectories come from North America and have the highest APTs, resulting in a significant reduction (by 53 %) in PM 2.5 /ΔCO under high-APT conditions (> 13.5 mm) relative to low-APT conditions (< 0.9 mm). Moreover, PM 2.5 /ΔCO was most sensitive to increases in APT up to 5 mm (–0.044 µg m –3 ppbv –1 mm –1 ) and less sensitive to increases in APT over 5 mm. While anthropogenic PM 2.5 constituents (e.g., black carbon, sulfate, organic carbon) decrease with high APT, sea salt, in contrast, was comparable between high- and low-APT conditions owing to enhanced local wind and sea salt emissions in high-APT conditions. The greater sensitivity of the fine-mode volume concentrations (versus coarse mode) to wet scavenging is evident from AErosol RObotic NETwork (AERONET) volume size distribution data. A combination of GEOS-Chem model simulations of the 210 Pb submicron aerosol tracer and its gaseous precursor 222 Rn reveals that (i) surface aerosol particles at Bermuda are most impacted by wet scavenging in winter and spring (due to large-scale precipitation) with a maximum in March, whereas convective scavenging plays a substantial role in summer; and (ii) North American 222 Rn tracer emissions contribute most to surface 210 Pb concentrations at Bermuda in winter (~75 %–80 %), indicating that air masses arriving at Bermuda experience large-scale precipitation scavenging while traveling from North America. A case study flight from the ACTIVATE field campaign on 22 February 2020 reveals a significant reduction in aerosol number and volume concentrations during air mass transport off the US East Coast associated with increased cloud fraction and precipitation. These results highlight the sensitivity of remote marine boundary layer aerosol characteristics to precipitation along trajectories, especially when the air mass source is continental outflow from polluted regions like the US East Coast.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Update of Erosion Conditions and Assessment of Mitigation Options for the L-Bar Site

The L-Bar former uranium milling site was remediated and closed per regulations and is now under the long-term stewardship of the U.S. Department of Energy, Office of Legacy Management (DOE/LM). Since assuming stewardship in 2004, DOE/LM has observed erosion and sedimentation processes at the L-Bar Site that will challenge meeting the design closure criteria in the long term, and therefore erosion control structures were installed in several areas. Portions of these structures were subsequently damaged by summer convective storm events and they are being redesigned. At the request of DOE/LM, Desert Research Institute (DRI) reviewed the proposed redesign plans of the erosion control structures. The purpose of this review is to support DOE/LM decisions regarding mitigation of ongoing erosion processes, including assessing possible repair of the existing erosion control structures, as well as plan for effective long-term site management. This design review is performed in reference to the Uranium Mill Tailings Radiation Control Act (UMTRCA) standards contained in 40 CFR 192.02 that require containment of residual radioactive material be effective for up to 1,000 years (if achievable, but certainly for 200 years), limit radon release, protect groundwater, and minimize future maintenance. The erosion control structures under review are not subject to the UMTRCA standard directly, but they contribute to the performance of the overall containment system by virtue of their relationship with the large diversion channels bounding the disposal cell. The 11 design drawings included in “Erosion Control Alternatives Analysis, L-Bar, New Mexico, Disposal Site, LTS-111-0043-08-002,” dated January 11, 2019, and listed in Appendix A, and supporting calculations in Weston (2019) are the focus of the review. Additionally, DOE/LM provided supporting data such as a 2018 photogrammetry-based digital elevation model of the site, precipitation records collected from an on-site weather station, and sedimentation records collected at an on-site basin. This assessment includes review of the proposed design to mitigate current site conditions but also addresses site changes between the initial erosion assessment report (Miller et al., 2012) and current conditions. The analysis is at a predesign engineering level and does not include development of hydraulic or sediment transport models. Site precipitation data are included in Miller et al. (2012). The natural conditions of the site, the design of site diversion systems, observed erosion at the site, and predesign engineering analysis are used to develop a holistic view of the challenges to L-Bar Site stability and possible responsive actions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

How much information on precipitation is contained in satellite infrared imagery?

Satellite infrared (IR) brightness temperature providing information on the characteristics of cloud tops is one of the primary input data used for estimating precipitation from satellites. Thus, the natural questions to ask are: Does IR imagery contain more information about precipitation in some regions more than others? What are the factors that lead to such differences? Should we expect the amount of information provided by IR imagery to change with respect to temporal or spatial aggregation? Comprehensive analysis of the accuracy of satellite-based precipitation estimates obtained from any given algorithm may provide qualitative answers to the above questions. However, such an approach only offers conclusions within the limited context of the algorithm used to obtain precipitation estimates; that is, patterns caused by the inherent information content of IR imagery are inextricable from those induced by assumptions embedded in the precipitation estimation algorithm. Here, we address the abovementioned questions from a different perspective using an information-theoretic measure, free of structural assumptions and general to a wide range of relationships, to characterize the average and seasonal dependence between IR imagery provided by satellite sensors in the spectral range (10.7–11.5 μm) and precipitation rates in the contiguous United States (CONUS) across distinct temporal and spatial scales. We analyze a total of more than 1.3 billion pairs of IR and precipitation observations over CONUS, and we observe interesting patterns. First, we show that there is a strong inverse relationship (ρ = - 0.73) between the information content of IR data and the number of no-rain observations; however, its robustness varies regionally and seasonally with less significant correlation during the warm season. Second, we demonstrate that the intuitive relationship of increasing dependence between IR and precipitation as a result of temporal or spatial aggregation exhibits a diminishing returns behavior. For instance, temporal aggregation from 1 to 3 h increases the dependence approximately 7 times as much as temporal aggregation from 12 to 24 h. Furthermore, we quantitatively examine and re-confirm several statements previously reported in the literature such as the strong association between IR and precipitation in convective storms and the low association in orographic rainfall. Finally, we conclude by illustrating the potential of the analysis in diagnosis of operational algorithms for estimating precipitation from IR brightness temperature. The findings of this study pinpoint spatial domains and time scales at which IR is not an adequate proxy for estimating precipitation. Thus, they can potentially guide the development of operational algorithms that utilize satellite Infrared imagery for estimating, downscaling and data fusion of precipitation. Finally, the analysis presented here opens up the possibility of developing new methodologies for diagnosis of satellite-based precipitation estimation algorithms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Vertical profiles of trace gas and aerosol properties over the eastern North Atlantic: variations with season and synoptic condition

Abstract. Because of their extensive coverage, marine low clouds greatly impact the global climate. Presently, the response of marine low clouds to the changes in atmospheric aerosols remains a major source of uncertainty in climate simulations. One key contribution to this large uncertainty derives from the poor understanding of the properties and processes of marine aerosols under natural conditions and the perturbation by anthropogenic emissions. The eastern North Atlantic (ENA) is a region of persistent but diverse subtropical marine boundary layer (MBL) clouds, where cloud albedo and precipitation are highly susceptible to perturbations in aerosol properties. Here we examine the key processes that drive the cloud condensation nuclei (CCN) population in the MBL using comprehensive characterizations of aerosol and trace gas vertical profiles during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) field campaign. During ACE-ENA, a total of 39 research flights were conducted in the Azores: 20 during summer 2017 and 19 during winter 2018. During summer, long-range-transported aerosol layers were periodically observed in the lower free troposphere (FT), leading to elevated FT CCN concentrations (NCCN). Both biomass burning and pollution from North America contribute to submicron aerosol mass in these layers, with pollution likely the dominant contributor. In contrast, long-range transported continental emissions have a much weaker influence on the aerosol properties in the ENA during the winter season. While the entrainment of FT air is a major source of particle number in the MBL for both seasons, on average it does not serve as a direct source of CCN in the MBL because the average FT NCCN is the same or even lower than that in the MBL. The particle number flux due to FT entrainment is dominated by pre-CCN (particles that are too small to form cloud droplets under typical conditions, i.e., particles with sizes below the Hoppel minimum) due to the elevated Npre-CCN in the lower FT. Once these pre-CCN are entrained into the MBL, they can grow and reach CCN size range through condensational growth, representing an indirect and major source of MBL CCN in the ENA. The impact of synoptic conditions on the aerosol properties is examined. Under pre-front and post-front conditions, shallow convective activity often leads to a deep and decoupled boundary layer. Coalescence scavenging and evaporation of drizzle below clouds lead to reduced NCCN and larger accumulation-mode particle sizes in the upper cloud-containing decoupled layer, indicating that surface measurements overestimate the NCCN relevant to the formation of MBL clouds under decoupled conditions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Effects of Atwood and Reynolds numbers on the evolution of buoyancy-driven homogeneous variable-density turbulence

The evolution of buoyancy-driven homogeneous variable-density turbulence (HVDT) at Atwood numbers up to 0.75 and large Reynolds numbers is studied by using high-resolution direct numerical simulations. To help understand the highly non-equilibrium nature of buoyancy-driven HVDT, the flow evolution is divided into four different regimes based on the behaviour of turbulent kinetic energy derivatives. The results show that each regime has a unique type of dependence on both Atwood and Reynolds numbers. It is found that the local statistics of the flow based on the flow composition are more sensitive to Atwood and Reynolds numbers compared to those based on the entire flow. It is also observed that, at higher Atwood numbers, different flow features reach their asymptotic Reynolds-number behaviour at different times. The energy spectrum defined based on the Favre fluctuations momentum has less large-scale contamination from viscous effects for variable-density flows with constant properties, compared to other forms used previously. The evolution of the energy spectrum highlights distinct dynamical features of the four flow regimes. Thus, the slope of the energy spectrum at intermediate to large scales evolves from -7/3 to -1 , as a function of the production-to-dissipation ratio. The classical Kolmogorov spectrum emerges at intermediate to high scales at the highest Reynolds numbers examined, after the turbulence starts to decay. Finally, the similarities and differences between buoyancy-driven HVDT and the more conventional stationary turbulence are discussed and new strategies and tools for analysis are proposed.

42 ENGINEERING↗

DOE OSTI2024

Exploring the Neutron Substructure with Advanced Polarized Helium-3 Targets (Or: How I Learned to Stop Worrying and Love Spectroscopy)

As we seek to understand the smallest, physical aspects of our universe, we cannot simply rely on our senses to probe the world around us as we did in the past. The smallest physical elements of our universe behave in strange, probabilistic ways and are completely invisible to the naked eye/ear/etc. So, we design clever experiments (such as scattering experiments) to probe these minute realms. Then, just as with the larger, observable world, we devise models and equations to describe what we think is happening. Due to the nature of the physical universe at the quantum scale and with the aid of symmetries such as Lorentz invariance, we can write down equations that describe the scattering, but the expressions contain functions, which we call ?form factors? and ?structure functions?, that we cannot compute from first principles. We can, however, formulate models that make predictions for these functions. By comparing our predictions with the observed data, we can gain insight into the validity of our models and thus a better physical understanding of what is happening at these minuscule scales. Studying the constituents inside of the nucleus of an atom adds another layer of difficulty if we can?t remove those components from the nucleus. This is the case with the neutron. When not bound in the nucleus with protons and other neutrons, the neutron will decay into a proton after about 15 minutes. So, we?re forced to study the neutron while it is still bound in the nucleus of an atom such as helium-3 (3He). For the last 1,000 years (rounding up), our group has developed high quality, polarized 3He targets made of an aluminosilicate glass. These targets are made in order to perform experiments at Jefferson Lab (JLab), experiments which let us determine the form factors and structure functions of the neutron by scattering polarized electrons from polarized neutrons (or rather polarized 3He). The specific experiments reported on in this thesis push the bounds of our understanding of the internal structure of the neutron. Good science is often about pushing experimental techniques to a new level. Toward that goal we study our polarized 3He targets both to advance the technology and to choose the best ones for our experiments. We do this using a process called nuclear magnetic resonance (NMR) to gauge the maximum polarization of a target and how fast the polarization decays with time. While these tests primarily provide us information that make analysis of our experimental scattering data possible, they also let us determine whether or not a target-cell is useful or even, dare I say, of spectacular quality. Our latest targets utilize a novel convection design allowing 3He to be polarized and quickly moved in front of the electron-beam, making it possible to use larger targets with higher electron-beam currents than ever before. This means more electrons scatter and we get more data. And by studying our targets in detail prior to using them in our experiments, we have found techniques to take effects which could have been detrimental to target quality and turn them to our advantage! It?s a real case of making lemonade out of lemons. We also use laser spectroscopy to study the absorption lines of alkali-metals in the target (potassium and rubidium, specifically). We add these alkali-metals to our target to facilitate polarizing the 3He. We can use the measurement of these pressure broadened absorption lines to determine the 3He density inside of the target with great precision. Historically, we understood the width of these lines would be dependent on the temperature of the target. Specifically, if I raise the temperature, the width should get bigger. I found that was not the case, which was very confusing at first, though very exciting now that I realize the data are self-consistent and suggestive of unexpected behavior. This thesis details the development of high quality, glass, polarized 3He targets for the 2020 An 1 /dn 2 and 2023 Gn E experiments, which utilized the first 3He convection targets and broke records in target quality. This thesis also covers the initial development of metal windows for the next-generation of 3He target-cells. Finally, this thesis documents the temperature dependence of the width of potassium (K) and rubidium (Rb) absorption lines as measured with laser spectroscopy.

Jantzi, Christopher↗