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At least 397 records · Page 22

Maximizing the Volume of Collocated Data from Two Coordinated Suborbital Platforms

Suborbital (e.g., airborne) campaigns that carry advanced remote sensing and in situ payloads provide detailed observations of atmospheric processes, but can be challenging to use when it is necessary to geographically collocate data from multiple platforms that make repeated observations of a given geographic location at different altitudes. This study reports on a data collocation algorithm that maximizes the volume of collocated data from two coordinated suborbital platforms and demonstrates its value using data from the NASA Aerosol Cloud Meteorology Interactions Over the western Atlantic Experiment (ACTIVATE) suborbital mission. A robust data collocation algorithm is critical for the success of the ACTIVATE mission goal to develop new and improved remote sensing algorithms, and quantify their performance. We demonstrate the value of these collocated data to quantify the performance of a recently developed vertically resolved lidar + polarimeter–derived aerosol particle number concentration (Na ) product, resulting in a range-normalized mean absolute deviation (NMAD) of 9% compared to in situ measurements. We also show that this collocation algorithm increases the volume of collocated ACTIVATE data by 21% compared to using only nearest-neighbor finding algorithms alone. Additional to the benefits demonstrated within this study, the data files and routines produced by this algorithm have solved both the critical collocation and the collocation application steps for researchers who require collocated data for their own studies. This freely available and open-source collocation algorithm can be applied to future suborbital campaigns that, like ACTIVATE, use multiple platforms to conduct coordinated observations, e.g., a remote sensing aircraft together with in situ data collected from suborbital platforms.

Atmosphere↗

ARM Lead Mentor Selection Process

The Atmospheric Radiation Measurement (ARM) Program was created in 1989 with funding from the U.S. Department of Energy (DOE) to develop several highly instrumented ground stations to study cloud-formation processes and their influence on radiative transfer. This scientific infrastructure provides for fixed sites, mobile facilities, an aerial facility, and a data archive available for use by scientists worldwide through the ARM Climate Research Facility—a scientific user facility. The ARM Climate Research Facility currently operates more than 300 instrument systems that provide ground-based observations of the atmospheric column. To keep ARM at the forefront of climate observations, the ARM infrastructure depends heavily on instrument scientists and engineers, known as Mentors. Mentors must have an excellent understanding of instrumentation theory and operation for their instrument areas and have comprehensive knowledge of critical scale-dependent atmospheric processes. They must also possess the technical and analytical skills to develop new data retrievals that provide innovative approaches for creating research-quality data sets. The ARM Facility seeks the best overall qualified candidate, or team when appropriate, that can fulfill Mentor requirements in a timely manner. The roles and responsibilities of the ARM Instrument Operations Manager are provided in Appendix A. The key role and responsibilities and detailed responsibilities of ARM Lead Mentors are provided in Appendix B and Appendix C, respectively.

47 OTHER INSTRUMENTATION↗

Molecular and physical characteristics of aerosol at a remote free troposphere site: implications for atmospheric aging

Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth's radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225 m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range-transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two of the samples were influenced by North American wildfire emissions transported in the free troposphere and one by North American outflow mainly transported within the marine boundary layer.Ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry was used to determine the detailed molecular composition of the samples. Thousands of molecular formulas were assigned to each of the individual samples. On average ~60 % of the molecular formulas contained only carbon, hydrogen, and oxygen atoms (CHO), ~30 %contained nitrogen (CHNO), and ~10 % contained sulfur (CHOS). The molecular formula compositions of the two wildfire-influenced aerosol samples transported mainly in the free troposphere had relatively low averageO/C ratios (0.48±0.13 and 0.45±0.11) despite the 7–10 days of transport time according to FLEXPART. In contrast, the molecular composition of the North American outflow transported mainly in the boundary layer had a higher average O/C ratio (0.57±0.17) with 3 days of transport time. To better understand the difference between free tropospheric transport and boundary layer transport, the meteorological conditions along the FLEXPART simulated transport pathways were extracted from the Global Forecast System analysis for the model grids. We used the extracted meteorological conditions and the observed molecular chemistry to predict the relative-humidity-dependent glass transition temperatures (T g ) of the aerosol components. Comparisons of the T g to the ambient temperature indicated that a majority of the organic aerosol components transported in the free troposphere were more viscous and therefore less susceptible to oxidation than the organic aerosol components transported inthe boundary layer. Although the number of observations is limited, the results suggest that biomass burning organic aerosol injected into the free troposphere is more persistent than organic aerosol in the boundary layer having broader implications for aerosol aging.

54 ENVIRONMENTAL SCIENCES↗

An evaluation of the variable-resolution CESM for modeling California's climate

In this paper, the recently developed variable-resolution option within the Community Earth System Model (VR-CESM) is assessed for long-term regional climate modeling of California at 0.25° (~ 28 km) and 0.125° (~ 14 km) horizontal resolutions. The mean climatology of near-surface temperature and precipitation is analyzed and contrasted with reanalysis, gridded observational data sets, and a traditional regional climate model (RCM)—the Weather Research and Forecasting (WRF) model. Statistical metrics for model evaluation and tests for differential significance have been extensively applied. VR-CESM tended to produce a warmer summer (by about 1–3°C) and overestimated overall winter precipitation (about 25%–35%) compared to reference data sets when sea surface temperatures were prescribed. Increasing resolution from 0.25° to 0.125° did not produce a statistically significant improvement in the model results. By comparison, the analogous WRF climatology (constrained laterally and at the sea surface by ERA-Interim reanalysis) was ~1–3°C colder than the reference data sets, underestimated precipitation by ~20%–30% at 27 km resolution, and overestimated precipitation by ~ 65–85% at 9 km. Overall, VR-CESM produced comparable statistical biases to WRF in key climatological quantities. Moreover, this assessment highlights the value of variable-resolution global climate models (VRGCMs) in capturing fine-scale atmospheric processes, projecting future regional climate, and addressing the computational expense of uniform-resolution global climate models.

54 ENVIRONMENTAL SCIENCES↗

Improving vertical detail in simulated temperature and humidity data using machine learning

Atmospheric models used for weather forecasting and climate predictions discretise the atmosphere onto a vertical grid. There are however atmospheric phenomena that occur on scales smaller than the thickness of those model layers. The formation of low-level clouds due to temperature inversions is an example. This leads to atmospheric models underestimating, or even missing, these clouds and their radiative effects. Using radiosonde observations as training data, a machine learning model is used to improve the vertical detail of modelled profiles of temperature and specific humidity. In addition, a physics-informed machine learning model is developed and compared to the traditional approach; showing improvements in the cloud fraction profiles calculated from its predictions. The vertically enhanced profiles also improve the representation of layers of convective inhibition and anomalous refractivity gradients. This work facilitates targeted improvements to the representation of certain atmospheric processes without the burden of increased memory and computational cost from increasing vertical resolution throughout the whole model.

54 ENVIRONMENTAL SCIENCES↗

A review of coarse mineral dust in the Earth system

Mineral dust particles suspended in the atmosphere span more than three orders of magnitude in diameter, from <0.1 µm to more than 100 µm. This wide size range makes dust a unique aerosol species with the ability to interact with many aspects of the Earth system, including radiation, clouds, hydrology, atmospheric chemistry, and biogeochemistry. This review focuses on coarse and super-coarse dust aerosols, which we respectively define as dust particles with a diameter of 2.5–10 µm and 10–62.5 µm. We review several lines of observational evidence indicating that coarse and super-coarse dust particles are transported farther than previously expected and that the abundance of these particles is substantially underestimated in current global models. We synthesize previous studies that used observations, theories, and model simulations to highlight the impacts of coarse and super-coarse dust aerosols on the Earth system, including their effects on dust-radiation interactions, dust-cloud interactions, atmospheric chemistry, and biogeochemistry. Specifically, coarse and super-coarse dust aerosols produce a net positive direct radiative effect (warming) at the top of the atmosphere and can modify temperature and water vapor profiles, influencing the distribution of clouds and precipitation. In addition, coarse and super-coarse dust aerosols contribute a substantial fraction of ice-nucleating particles, especially at temperatures above –23 °C. They also contribute a substantial fraction to the available reactive surfaces for atmospheric processing and the dust deposition flux that impacts land and ocean biogeochemistry by supplying important nutrients such as iron and phosphorus. Furthermore, we examine several limitations in the representation of coarse and super-coarse dust aerosols in current model simulations and remote-sensing retrievals. Because these limitations substantially contribute to the uncertainties in simulating the abundance and impacts of coarse and super-coarse dust aerosols, we offer some recommendations to facilitate future studies. Overall, we conclude that an accurate representation of coarse and super-coarse properties is critical in understanding the impacts of dust aerosols on the Earth system.

54 ENVIRONMENTAL SCIENCES↗

Sea spray aerosol production flux retrieval based on Doppler lidar measurements

Supermicron sea spray aerosols (SSA) play a crucial role in stratocumulus cloud microphysics and drizzle formation. However, our understanding of SSA's spatiotemporal distribution, production mechanisms, and fluxes in the marine boundary layer remains limited. This study introduces a novel approach to determine supermicron SSA production flux and number concentration at various heights above the ocean surface. Our method leverages Doppler lidar data, specifically attenuated backscatter and vertical velocity, collected at a 105 m range gate during the Eastern Pacific Clouds and Aerosols for Precipitation Experiment (EPCAPE) at Scripps Pier, La Jolla, California. To focus on nascent SSA, we analyzed data from periods with wind directions between 225° and 315° and wind speeds exceeding 4 m s −1 . Cloud and precipitation events were excluded using relative humidity, backscatter thresholds, and 2D Video Disdrometer observations. Results show that calculated supermicron SSA number concentrations at 105 m ranged from 0.26 to 2.93 cm −3 for surface wind speeds between 4 and 6 ms −1 . When exceeding the method's Limit of Detection, estimated production fluxes ranged from 0.20 to 1.53 cm −2 s −1 . This methodology has potential for application in various oceanic locations, likely enhancing our understanding of SSA's role in atmospheric processes and climate interactions.

54 ENVIRONMENTAL SCIENCES↗

The root-zone soil moisture spectrum in a mediterranean ecosystem

Storage of water within soil pores of the root zone introduce memory effects in the dynamics of soil moisture that are considerably longer than the integral timescale of many atmospheric processes. Thus, hydro-climatic states can be “sustained” through land-surface heat and water vapor fluxes primarily because they can “feed off” on this long-term soil moisture memory. Root-zone soil moisture memory is only but one feature characterizing the spectrum of soil moisture dynamics, which is analyzed here using a combination of long-term measurements and models. In particular, the spectrum of root-zone soil moisture content in a Mediterranean ecosystem is examined using 14-years of half-hourly measurements. A distinguishing hydro-climatic feature in such ecosystems is that sources (mainly rainfall) and sinks (mainly evapotranspiration) of soil moisture are roughly out of phase with each other. For over 4 decades of time scales and 7 decades of energy, the canonical shape of the measured soil moisture spectrum is shown to be approximately Lorentzian determined by the soil moisture variance and its memory but with two exceptions: the occurrences of a peak at diurnal-to-daily time scales and a weaker peak at near annual time scales. Model calculations and spectral analysis demonstrate that diurnal and seasonal variations in hydroclimate forcing responsible for variability in evapotranspiration had minor impact on the normalized shape of the soil moisture spectrum. However, their impact was captured by adjustments in the temporal variance. These findings indicate that precipitation and not evapotranspiration variability dominates the multi-scaling properties of soil moisture variability consistent with prior climate model simulations. Furthermore, the soil moisture memory inferred by the annual peak of soil moisture (340 d) is consistent with climate model simulations, while the memory evaluated from the loss function of a linearized mass balance approach leads to a smaller value (50 d), highlighting the effect of weak non-stationarity on soil moisture variability.

54 ENVIRONMENTAL SCIENCES↗

Spatial variability of aerosol iron mineralogy and oxidation states over the Arctic Ocean

The mineralogy and oxidation state of aerosol iron (Fe) play important roles in controlling aerosol Fe solubility and consequent bioavailability in seawater. In this study, the spatial variability of Fe mineralogy and oxidation states in aerosols collected during the US GEOTRACES Western Arctic cruise (GN01) were determined using synchrotronbased X-ray absorption near edge structure (XANES) spectroscopy. Both Fe(II) minerals (biotite, ilmenite) and Fe (III) minerals (ferrihydrite, hematite, Fe(III) phosphate) were found in these samples. However, aerosol Fe mineralogy and solubility observed during this cruise varied spatially and can be grouped into three clusters based on the air masses that affected aerosols collected in different regions: (1) biotite-enriched particles (87 % biotite, 13 % hematite) with the air masses passing over Alaska, showing relatively low Fe solubility (4.0 +/- 1.7 %); (2) ferrihydrite-enriched particles (82 % ferrihydrite, 18 % ilmenite) collected in the remote Arctic air, showing relatively high Fe solubility (9.6 +/- 3.3 %); (3) the fresh dust derived from North America and Siberia, primarily dominated by hematite (41 % hematite, 25 % Fe(III) phosphate, 20 % biotite, 13 % ferrihydrite), showing relatively low Fe solubility (5.1 +/- 3.5). A significant positive correlation was found between Fe oxidation state and Fe fractional solubility, suggesting that long-range transport could modify iron (hydr) oxide such as ferrihydrite through atmospheric processing, influencing aerosol Fe solubility and consequently Fe bioavailability in the remote Arctic Ocean.

54 ENVIRONMENTAL SCIENCES↗

X-ray Spectroscopic Quantification of Phosphorus Transformation in Saharan Dust during Trans-Atlantic Dust Transport

Saharan dust is an important phosphorus (P) supply to remote and oligotrophic parts of the oceans and American lowland tropical rainforests. Phosphorus speciation in aeolian dust ultimately controls the release and bioavailability of P after dust deposition, but the speciation in Saharan dust and its change during the trans-Atlantic transport remains unclear. Here, using P K-edge X-ray absorption near edge structure (XANES) spectroscopy, we showed that with increasing dust traveling distance from the Sahara Desert to Cape Verde and to Puerto Rico, about 570 and 4000 km, respectively, the proportion of Ca-bound P (Ca-P), including both apatite and non-apatite forms, decreased from 68–73% to 50–71% and to 21–37%. The changes were accompanied by increased iron/aluminum-bound P proportion from 14–25% to 23–46% and to 44–73%, correspondingly. Laboratory simulation experiments suggest that the changes in P speciation can be ascribed to increasing degrees of particle sorting and atmospheric acidification during dust transport. The presence of relatively soluble non-apatite Ca-P in the Cape Verde dust but not in the Puerto Rico dust is consistent with the higher P water solubility of the former than the latter. Our findings provide insights into the controls of atmospheric processes on P speciation, solubility, and stability in Saharan dust.

54 ENVIRONMENTAL SCIENCES↗

Water–Hydrocarbon Interactions in Anionic Pyrene Monohydrate

Interactions between water and polycyclic aromatic hydrocarbons are essential in many aspects of chemistry, from interstellar and atmospheric processes to interfacial hydrophobicity and wetting phenomena. Despite their growing importance, the intermolecular potentials of the water-hydrocarbon interactions are underdeveloped compared to water-water potentials, and there are similarly few experimental probes that are sensitive to the details of the water-hydrocarbon potential. We present a combined experimental and computational study of anionic pyrene monohydrate, one of the simplest water/hydrocarbon clusters. The action spectrum in the OH region of the mass-selected cluster ion provides a rigorous benchmark for intermolecular potentials and computational methodologies. We identify missing intermolecular interactions and shortcomings in conventional dynamics calculations by comparing experimental data to density functional theory and classical molecular dynamics calculations. Kinetic trapping is prevalent, even for one water molecule and one pyrene molecule, leading to slow equilibration in conventional molecular dynamics calculations, even on nanosecond timescales and at low temperatures (50 K). At constant energy, temperature fluctuations for the pair of molecules are substantial. Immersing the system in a bath of soft spheres and employing parallel tempering alleviates kinetic trapping and dampens temperature fluctuations, bringing the system closer to the thermodynamic limit. With such augmented sampling, a simple, flexible water model reproduces the linewidth and the asymmetric broadening of the symmetric OH stretching mode, which we assign to spectral diffusion. In the OH stretching region, dynamics calculations predict a more intense antisymmetric peak than experiments observe but do not predict the bimodal split symmetric peak that the experiments show. Furthermore, our work suggests that electronic polarization, missing in the empirical force field, is responsible for the first discrepancy and that quantum nuclear effects, captured neither in density functional theory nor in classical dynamics, may be responsible for the second.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Southwestern U.S. Biomass Burning Smoke Hygroscopicity: The Role of Plant Phenology, Chemical Composition, and Combustion Properties

Biomass burning emissions have substantially increased with continued warming and drying in the southwestern U.S., impacting air quality and atmospheric processes. To better quantify impacts of biomass burning aerosols, an extensive laboratory study of fresh smoke emissions was conducted at Los Alamos National Laboratory. Laboratory burn experiments with selected native and invasive southwestern U.S. fuels were used to elucidate the role of fuel type, chemical composition, and ignition method on the hygroscopicity of smoke. Here we focus on a custom controlled relative humidity (RH) nephelometry system using the direct measurement of aerosol light scattering with two nephelometers—one at dry conditions and one at a controlled high RH (RH ~ 85%). Aerosol hygroscopicity was highly variable with the enhancement in light scattering coefficient in the range of 1.02 < f (RH = 85%) < 2.1 and corresponding to the kappa parameter (κ neph ) ranging from ~0 to 0.18. Hygroscopicity is determined primarily by the fuel's inorganic ion content. For example, invasive halophytes with high inorganic salt content exhibit much greater water uptake than native coniferous species with low inorganic content. Combustion temperature and phase, flaming or smoldering, play a secondary role in the water uptake of smoke. High–temperature ignition methods create flaming conditions that enhance hygroscopicity while lower–temperature smoldering conditions diminish hygroscopicity. Our results construct an empirical relation between κ neph and the inorganic content of the fuel and smoke to predict water uptake.

54 ENVIRONMENTAL SCIENCES↗

Martian Eolian Dust Probed by ChemCam

Here, the ubiquitous eolian dust on Mars plays important roles in the current sedimentary and atmospheric processes of the planet. The ChemCam instrument retrieves a consistent eolian dust composition at the sub–mm scale from every first laser shot on Mars targets. Its composition presents significant differences with the Aeolis Palus soils and the Bagnold dunes as it contains lower CaO and higher SiO 2 . The dust FeO and TiO 2 contents are also higher, probably associated with nanophase oxide components. The dust spectra show the presence of volatile elements (S, Cl), and the hydrogen content is similar to Bagnold sands, but lower than Aeolis Palus soils. Consequently, the dust may be a contributor to the amorphous component of soils but differences in composition indicate that the two materials are not equivalent.

58 GEOSCIENCES↗

Global Impacts of Arctic Sea Ice Loss Mediated by the Atlantic Meridional Overturning Circulation

We explore the global impacts of Arctic sea ice decline in climate model perturbation experiments focusing on the temporal evolution of induced changes. We find that climate response to a realistic reduction in sea ice cover varies dramatically between shorter decadal and longer multidecadal to centennial timescales. During the first two decades, when atmospheric processes dominate, sea ice decline induces a “bipolar seesaw” pattern in surface temperature with warming in the Northern and cooling in the Southern Hemisphere, leading to a northward displacement of the Intertropical Convergence Zone and an expansion of Antarctic sea ice. In contrast, on multidecadal and longer timescales, the weakening of the Atlantic meridional overturning circulation, caused by upper-ocean buoyancy anomalies spreading from the Arctic, mediates direct sea ice impacts and nearly reverses the original response pattern outside the Arctic. Lastly, the Southern Hemisphere warms, a Warming Hole emerges in the North Atlantic, the Intertropical Convergence Zone shifts southward, and Antarctic sea ice contracts.

58 GEOSCIENCES↗

Evaluating soil moisture feedback on convective triggering: Roles of convective and land–model parameterizations

Feedbacks between soil moisture and convective precipitation are not well represented in current Earth system models, and can affect projections of drought and heavy-precipitation extremes. To explore the atmospheric and land-surface influences on the initiation (triggering) of daytime deep convection, single-column model experiments were performed using the NCAR Community Earth System Model (CESM1.2), over the U.S. Southern Great Plains. The results indicate that the positive and negative feedback mechanisms found in earlier studies (using simplified boundary-layer models) are robust to large-scale forcing and interactions between boundary-layer turbulence, cloud dynamics, and radiation. However, systematic responses of convective triggering to soil moisture emerged only after switching from a convective available potential energy-based to a convective inhibition energy-based convective parameterization. This suggests that the choice of convective mass-flux closure largely determines the sensitivity of parameterized convective clouds to land-surface state. Errors in land-model parameterizations of evapotranspiration also affect the probability of deep convection, with vegetation (transpiration) playing an important role in linking soil moisture to surface energy partitioning and clouds. Parameterizations that permit the triggering feedback mechanism better predict the statistics of daytime shallow and deep convection, with respect to observations from the Atmospheric Radiation Measurement site in the Southern Great Plains. Here, the results illustrate how errors in the representation of evapotranspiration in land-surface models can propagate through the chain of coupled land-atmosphere processes to affect convective clouds.

54 ENVIRONMENTAL SCIENCES↗

Hydrate Formation on Marine Seep Bubbles and the Implications for Water Column Methane Dissolution

Abstract Methane released from seafloor seeps contributes to a number of benthic, water column, and atmospheric processes. At seafloor seeps within the methane hydrate stability zone, crystalline gas hydrate shells can form on methane bubbles while the bubbles are still in contact with the seafloor or as the bubbles begin ascending through the water column. These shells reduce methane dissolution rates, allowing hydrate‐coated bubbles to deliver methane to shallower depths in the water column than hydrate‐free bubbles. Here, we analyze seafloor videos from six deepwater seep sites associated with a diverse range of bubble‐release processes involving hydrate formation. Bubbles that grow rapidly are often hydrate‐free when released from the seafloor. As bubble growth slows and seafloor residence time increases, a hydrate coating can form on the bubble's gas‐water interface, fully coating most bubbles within ∼10 s of the onset of hydrate formation at the seafloor. This finding agrees with water‐column observations that most bubbles become hydrate‐coated after their initial ∼150 cm of rise, which takes about 10 s. Whether a bubble is coated or not at the seafloor affects how much methane a bubble contains and how quickly that methane dissolves during the bubble's rise through the water column. A simplified model shows that, after rising 150 cm above the seafloor, a bubble that grew a hydrate shell before releasing from the seafloor will have ∼5% more methane than a bubble of initial equal volume that did not grow a hydrate shell after it traveled to the same height.

54 ENVIRONMENTAL SCIENCES↗

Quantum reactive scattering of O({sup 3}P)+H{sub 2} at collision energies up to 4.4 eV

We report the results of quantum scattering calculations for the O({sup 3}P)+H{sub 2} reaction for a range of collision energies from 0.4 to 4.4 eV, important for astrophysical and atmospheric processes. The total and state-to-state reactive cross sections are calculated using a fully quantum time-independent coupled-channel approach on recent potential energy surfaces of {sup 3}A{sup ′} and {sup 3}A{sup ″} symmetry. A larger basis set than in the previous studies was used to ensure single-surface convergence at higher energies. Our results agree well with the published data at lower energies and indicate the breakdown of reduced dimensionality approach at collision energies higher than 1.5 eV. Differential cross sections and momentum transfer cross sections are also reported.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗