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At least 109 records · Page 6

Extreme Wet and Dry Conditions Affected Differently by Greenhouse Gases and Aerosols

Global warming due to greenhouse gases and atmospheric aerosols alter precipitation rates, but the influence on extreme precipitation by aerosols relative to greenhouse gases is still not well known. Here we use the simulations from the Precipitation Driver and Response Model Intercomparison Project that enable us to compare changes in mean and extreme precipitation due to greenhouse gases with those due to black carbon and sulfate aerosols, using indicators for dry extremes as well as for moderate and very extreme precipitation. Generally, we find that the more extreme a precipitation event is, the more pronounced is its response relative to global mean surface temperature change, both for aerosol and greenhouse gas changes. Black carbon (BC) stands out with distinct behavior and large differences between individual models. Dry days become more frequent with BC-induced warming compared to greenhouse gases, but so does the intensity and frequency of extreme precipitation. An increase in sulfate aerosols cools the surface and thereby the atmosphere, and thus induces a reduction in precipitation with a stronger effect on extreme than on mean precipitation. A better understanding and representation of these processes in models will provide knowledge for developing strategies for both climate change and air pollution mitigation.

Sillmann, Jana↗

Simultaneous Retrievals of Biomass Burning Aerosols and Trace Gases From the Ultraviolet to Near-Infrared Over Northern Thailand During the 2019 Pre-Monsoon Season

With the advent of spaceborne spectroradiometers in a geostationary constellation, measuring high spectral resolution ultraviolet–visible (UV-VIS) and selected near-/shortwave-infrared (NIR/SWIR) radiances can enable the probing of the life cycle of key atmospheric trace gases and aerosols at higher temporal resolutions over the globe. The UV-VIS measurements are important for retrieving several key trace gases (e.g., O 3 , SO 2 , NO 2 , and HCHO) and particularly for deriving aerosol characteristics (e.g., aerosol absorption and vertical profile). This study examines the merit of simultaneous retrievals of trace gases and aerosols using a ground-based spectroradiometer covering the UV-NIR to monitor their physicochemical processes and to obtain reliable aerosol information for various applications. During the 2019 pre-monsoon season over northern Thailand, we deployed a ground-based SMART–s (Spectral Measurements for Atmospheric Radiative Transfer–spectroradiometer) instrument, which is an extended-range Pandora with reliable radiometric calibration in the 330–820 nm range, to retrieve remotely sensed chemical and aerosol properties for the first time near biomass burning sources. The high spectral resolution (∼ 1.0 nm full width half maximum with ∼ 3.7 × oversampling) of sun and sky measurements from SMART–s provides several key trace gases (e.g., O 3 , NO 2 , and H 2 O) and aerosol properties covering the UV where significant light absorption occurs by the carbonaceous particles. During the measurement period, highly correlated total column amounts of NO 2 and aerosol optical thickness (т aer ) retrieved from SMART–s (correlation coefficient, R=0.74) indicated their common emissions from biomass burning events. The SMART–s retrievals of the spectral single scattering albedo (ω 0 ) of smoke aerosols showed an abrupt decrease in the UV, which is an important parameter dictating photochemical processes in the atmosphere. The values of ω 0 and column precipitable water vapor (H 2 O) gradually increase with the mixing of biomass burning smoke particles and higher water vapor concentrations when approaching the monsoon season. The retrieved ω 0 and weighted mean radius of fine-mode aerosols from SMART–s showed positive correlations with the H 2 O (R=0.81 for ω 0 at 330 nm and 0.56 for the volume-weighted mean radius), whereas the real part of the refractive index of fine-mode aerosol (n f ) showed negative correlations (R = -0.61 at 330 nm), which suggest that aerosol aging processes including hygroscopic growth (e.g., humidification and cloud processing) can be a major factor affecting the temporal trends of aerosol optical properties. Retrieved n f and ω 0 were closer to those of the water droplet (i.e., n f of about 1.33 and ω 0 of about 1.0) under lower amounts of NO 2 during the measurement period; considering that the NO 2 amounts in the smoke may indicate the aging of the plume after emission due to its short lifetime, the tendency is also consistent with active hygroscopic processes of the aerosols over this area. Retrieved UV aerosol properties from SMART–s generally support the assumed smoke aerosol models (i.e., the spectral shape of aerosol absorption) used in NASA's current satellite algorithms, and their spectral ω 0 retrievals from ground and satellites showed good agreements (R = 0.73–0.79). However, temporal and spectral variabilities in the aerosol absorption properties in the UV emphasize the importance of a realistic optical model of aerosols for further improvements in satellite retrievals.

biomass burning↗

Noble Gases in Samples Returned From Asteroids Ryugu and Bennu

Introduction: The asteroid sample return missions, JAXA’s Hayabusa2 [1] and NASA’s OSIRIS-REx [2], fromC-rich asteroids Ryugu and Bennu offer unique opportunities to sample pristine early solar system material, unaffected by terrestrial weathering and contamination, and with a known geological context. The comparison with most primi-tive members of carbonaceous –and inner solar system ordinary and enstatite– chondrite classes allows us to (i) assess the variation (or the lack of thereof) of the distribution of the most volatile elements throughout the entire early solar system, (ii) determine the effects of parent body thermal and aqueous alteration, and (iii) learn about the dynamic evolution and history of the various parent bodies, as sampled by both return missions and meteorite delivery. Here we will present noble gas data obtained from newly received particles from Ryugu and Bennu. Samples & Analysis: We received nine particles allocated by JAXA, with masses of 0.5-1.7 mg mass: four col-lected during Hayabusa2’s first touchdown (chamber A) and five from a small artificial crater (chamber C). We received three particles from Bennu of 0.07, 0.89 and 0.94 mg mass (OREX-800032-102/3/4). All particles were processed, allocated, weighed, and transferred into our UHV sample chamber within pure N2, to prevent any contact with air. We examined all He-Xe isotopes with our custom-built mass spectrometer “Albatros” ([3,4]). Gases were extracted individually from each particle by melting induced by a 1064 μm Nd:YAG IR laser in 2–4 heating steps. Large amounts of water and other reactive volatiles were released, consistent with the presence of abundant volatiles from both Ryugu and Bennu. Residues of Ryugu particles remaining after lasering, subsequently exposed to air, were additionally extracted in a crucible to verify complete gas extraction. Only the particle that still showed a “crystalline” structure after lasering contained detectable Ryugu noble gases, whereas all other particles turned immediately into glassy spheres by laser heating and lacked any gas. Results & Discussion: Ryugu and Bennu matter contains noble gases similar to the most pristine, unheated aqueously altered meteorites, e.g., CM or CI chondrites [5,6]. Remarkably, all four chamber A samples that originated from Ryugu’s surface show solar wind (SW) Ne (trapped (20Ne/22Ne)tr ~12–13), whereas all five chamber C samples do not ((20Ne/22Ne)tr ~9.0–10.7 consistent with the presence of non-solar trapped Ne components such as Q and HL). This demonstrates that JAXA’s sampling strategy succeeded: Chamber C samples analyzed in this work originated from areas shielded from SW, slightly below the surface, that was sampled after the impactor excavated material. The three Bennu particles populate the same range as the Ryugu particles in Ne isotope space with one particle containing SW suggesting that it was part of the uppermost surface layer of Bennu during sampling, while Ne in the smallest sample can be explained best by mixing Ne from presolar diamonds and SiC or graphite, and that in the third one by mixing of, e.g., Q and HL. Using cosmic ray production rates given by [7] yields preliminary exposure ages for Ryugu particles in the same range as determined in [7]. There is, as expected, also no systematic difference between samples from chambers A and C because both sample sets were likely collected within the uppermost layer of Ryugu, which were not shielded from cosmic rays. The concentration of cosmogenic (cos) Ne in the Bennu particle, where Necos was resolvable, is in the same range as found for Ryugu, suggesting roughly similar exposure time to cosmic rays for 5–8 Ma for all particles examined here. The Xe isotopic compositions of all particles are consistent with those of phase Q, with small additions of Xe-HL from presolar diamonds and excess 129Xe* from short-lived 129I decay. The comparably high 129Xe*/129XeQ ratio is similar in all samples, suggesting similar initial I concentrations and closure to Xe loss –or the incorporation of a well-mixed Xe reservoir. The Bennu material was in brief contact with air in the capsule, after atmospheric entry and before storage in pure N2 in a clean room. Both, the –most diagnostic– Xe isotopes and the Ar/Xe vs. Kr/Xe systematics prove that the noble gases are not affected by terrestrial contamination, in contrast to many CI, CY, and CM chondrites found on Earth [5,6], illustrating the importance of sample return. He-Xe concentrations in all particles unaffected bySW are comparable to but at the upper end of ranges reported [5-7]. In accordance with the strong aqueous alteration experienced on the parent bodies of Ryugu and Bennu [1,2], all samples lack the Ar-rich and water-susceptible noble gas components found in less aqueously altered CMs or CRs [e.g., 5,8] and all COs.

Henner Busemann↗

Quantum Emitters Induced by High Pressure and UV Laser Irradiation in Multilayer GaSe

In this work, we report on defect generation in multilayer GaSe through hydrostatic pressure quenching and UV laser irradiation. The Raman line width from the UV 266 nm irradiated sample is much wider than that in pressure-quenched GaSe, corresponding to a wider defect energy distribution range in the former sample than the latter. After quenching from 11.2 GPa, three photoluminescence (PL) peaks from defect states are observed at 657, 681, and 695 nm at a low temperature of 93 K. Defect-related peaks at 649, 694, 750, and 774 nm also appear in low-temperature PL spectra after UV laser irradiation, with a nonmonotonous intensity dependence on irradiation duration. There are common features in defects produced by these two methods: the PL peaks with the lowest energy are sharp, and their PL intensities increase linearly with the excitation laser power and saturate above a certain excitation laser power. These two features are similar to those in defects for single-photon emission (SPE) in other 2D materials at even lower temperatures. Fluorescence lifetime imaging shows distinguished short (2.3 ns) and long (75.6 nm) lifetimes of the 695 nm PL line in pressure-quenched GaSe. The density functional theory predicts defect energy levels related to Se vacancy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Preferential adsorption of noble gases in zeolitic tuff with variable saturation: A modeling study of counter-intuitive diffusive-adsorptive behavior

Noble gas transport through geologic media has important applications in the prediction and characterization of measured gas signatures related to underground nuclear explosions (UNEs). Retarding processes such as adsorption can cause significant species fractionation of radionuclide gases, which has implications for measured and predicted signatures used to distinguish radioxenon originating from civilian nuclear facilities or from UNEs. Accounting for the effects of variable water saturation in geologic media on tracer transport is one of the most challenging aspects of modeling gas transport because there is no unifying relationship for the associated tortuosity changes between different rock types, and reactive transport processes such as adsorption that are affected by the presence of water likewise behave differently between gas species. In this study, we perform numerical diffusive-adsorptive transport simulations to estimate gas transport parameters associated with bench-scale laboratory diffusion cell experiments measuring breakthrough in zeolitic and non-zeolitic rocks for a gaseous mixture of xenon, krypton, and SF 6 at varying degrees of water saturation (S w ). Counter-intuitive transport behavior was observed in the zeolitic rock experiments whereby breakthrough concentrations were significantly higher when the core was partially saturated (S w = 17 %) than under dry (S w = 0 %) conditions. Breakthrough of xenon was especially retarded in the dry core – likely due to comparatively high affinity of xenon for zeolitic adsorption sites – and estimated effective diffusion coefficients for all gases were approximately an order of magnitude lower than what is predicted by porosity-tortuosity models. We propose the counter-intuitive behavior observed is because water infiltration of zeolite nanopores reduces both the adsorptive capacity of the rock and the tortuosity of connected flow paths. We developed a two-site competitive kinetic Langmuir adsorption reaction for the porous media transport simulator in order to constrain transport parameters within zeolitic tuff, where differential adsorption to zeolite and non-zeolite pores was observed. We determined that liquid saturation-dependent diffusive-adsorptive transport is affected by subtle and at times competing processes that are specific to different gases, which have a significant overall influence on effective transport parameters.

58 GEOSCIENCES↗

Deterministic Localization of Strain-Induced Single-Photon Emitters in Multilayer GaSe

The nanoscale strain has emerged as a powerful tool for controlling single-photon emitters (SPEs) in atomically thin transition metal dichalcogenides (TMDCs). However, quantum emitters in monolayer TMDCs are typically unstable in ambient conditions. Multilayer TMDCs could be a solution, but they suffer from low quantum efficiency, resulting in low brightness of the SPEs. Here, we report the deterministic spatial localization of strain-induced SPEs in multilayer GaSe by nanopillar arrays. The strain-controlled quantum confinement effect introduces well-isolated sub-bandgap photoluminescence and corresponding suppression of the broad band edge photoluminescence. Clear photon-antibunching behavior is observed from the quantum dot-like GaSe sub-bandgap exciton emission at 3.5 K. The strain-dependent confinement potential and the brightness are found to be strongly correlated, suggesting a promising route for tuning and controlling SPEs. The comprehensive investigations of strain-engineered GaSe SPEs provide a solid foundation for the development of 2D devices for quantum photonic technologies.

2D materials↗

Impact Delivery of Reduced Greenhouse Gases on Early MARS

While there is abundant evidence for flowing liquid water on the ancient Martian surface, a widely accepted greenhouse mechanism for explaining this in the presence of a faint young sun has yet to emerge. Gases such as NH3, CO2 alone, SO2, clouds, and CH4, have sustainability issues or limited greenhouse power. Recently, Ramirez et al. proposed that CO2-H2 atmospheres, through collision induced absorptions (CIA), could solve the problem if large amounts are present (1.3-4 bars of CO2, 50-20% H2). However, they had to estimate the strength of the H2- CO2 interaction from the measured strength of the H2- N2 interaction. Recent ab initio calculations show that the strength of CO2-H2 CIA is greater than Ramirez et al. assumed. Wordsworth et al. also calculated the absorption coefficients for CO2-CH4 CIA and show that on early Mars a 0.5 bar CO2 atmosphere with percent levels of H2 or CH4 can raise mean annual temperatures by tens of degrees Kelvin. Freezing temperatures can be reached in atmospheres containing 1-2 bars of CO2 and 2-10% H2 and CH4. The new work demonstrates that less CO2 and reduced gases are needed than Ramirez et al. originally proposed, which improves prospects for their hypothesis. If thick weakly reducing atmospheres are the solution to the faint young sun paradox, then plausible mechanisms must be found to generate and sustain the required concentrations of H2 and CH4. Possible sources of reducing gases include volcanic outgassing, serpentinization, and impact delivery; sinks include photolysis, oxidation, and hydrogen escape. The viability of the reduced greenhouse hypothesis depends, therefore, on the strength of these sources and sinks.

Martian surface↗

Coexisting Quantum Gases in Earth’s Orbit

Summary: Ultracold atomic gases provide a unique tool for exploring the quantum nature of matter and for probing the foundations of modern physics. Researchers with NASA’s Cold Atom Lab (CAL) have now simultaneously produced gases of two atomic species (rubidium and potassium) in a uniquely quantum (wave-like) phase of matter called a Bose-Einstein condensate (BEC) for the first time in space. CAL scientists are using the unique micro gravity environment onboard the International Space Station to study interactions, molecule formation, and the emergence of structure and complexity in these coexisting dual-species gases at unprecedented low temperatures, for long times in free fall, and specifically in the absence of the perturbing force of gravity.

quantum gases↗

Effect of the Electrostatic Field due to the Surface Monolayer Metal Atoms on the Dissociation of Homonuclear Diatomic Gases in Gas-Metal Surface Reactions

The present paper examines the role of an electrostatic field generated by the outermost monolayer of metal ions prior to gas adsorption in aiding the dissociation of homonuclear diatomic gas molecules. The interaction of five homonuclear diatomic gases, Cl 2 , F 2 , H 2 , N 2 and O 2 , with several pure metals are examined using Coulomb’s law to calculate the attractive and repulsive forces between the electrons or ions in the gas molecule and the free surface metallic electrons or ions assuming a Bohr model. These calculations demonstrate that the total energy of the electrostatic fields from the metals can exceed the molecular binding energies of Cl 2 , F 2 , and O 2 at some distance from the metallic surface thereby suggesting that these gases interact primarily with the metallic surface in their atomic states after molecular bond dissociation prior to reaction. In contrast, H 2 and N 2 gases do not dissociate prior to reaching the metal surface due to the fact that the effective charge of the gas ions is less than the total electron charge at the outermost electronic shell. The present results correlate linearly with the electrochemical series standard reduction potential as well as with the Pauling electronegativity for several metals.

Gas-metal reactions↗

The ZBOT-NC Experiment - Effects of Non-Condensable Gases on Propellant Tank Pressurization and Pressure Control

Introduction Integral to all phases of NASA’s projected planetary expeditions is affordable and reliable cryogenic fluid storage for use in propellant or life support systems. It is greatly advantageous to develop innovative vent-less pressure control designs based on cooling/mixing of the bulk tank fluid to allow storage of the cryogenic fluid with zero or reduced boil-off. The presence of noncondensable gases, can interfere with the condensation at the interface impacting tank pressure control during subcooled jet mixing especially in microgravity. The Zero-Boil-Off Tank (ZBOT) Experiments are a series of small-scale experiments aboard the International Space Station (ISS) that use a transparent volatile simulant fluid in a transparent sealed tank to delineate various fundamental fluid flow, heat and mass transport, and phase change phenomena associated with storage tank pressurization and pressure control in microgravity. The ZBOT-1 experiment was performed on the ISS 2017-2018 timeframe and collected data to validate a state-of-the-art CFD model for tank pressurization and pressure control for a pure system. The ZBOT-NC Experiment is the second experiment in the series to be performed on the International Space Station (ISS) in 2025. Its goal is to investigate the effects of noncondensable gases on interfacial evaporation and condensation during self -pressurization and jet-mixing pressure control in microgravity for a two-component system. Materials & Methods In this work, we will describe the detailed features of the ZBOT-NC experimental hardware and Diagnostics that includes nonintrusive Quantum Dot Thermometry (QDT) for whole field temperature measurement. All microgravity pressurization and pressure control tests will be performed for both the pure and the two-components systems with Xenon and Neon as the two noncondensable gases spanning small and large molecular weights and sizes. The two-phase CFD model that is developed as part of the project will be also presented and discussed. Results Ground-based pressurization and jet mixing experiments and CFD simulation results are compared to each other to validate both the fidelity of the CFD model predictions and the accuracy of the QDT measurement. Model simulations for noncondensable gas effects will also be compared against large Cryogenic LH2-GHe experiments to indicate the noncondensable gas effects on tank pressure control during jet mixing in 1G. Finally, CFD results will be presented to predict the effects of the noncondensable gas during subcooled jet mixing during the ZBOT-NC in advance of the microgravity experiment in 2015.

Evaporation Condensation↗

The Zero-Boil-Off Tank Experiment: the Effects of Non-Condensable Gases on Pressurization and Pressure Control of Propellant Tanks in Microgravity

Introduction Integral to all phases of NASA’s projected planetary expeditions is affordable and reliable cryogenic fluid storage for use in propellant or life support systems. It is greatly advantageous to develop innovative vent-less pressure control designs based on cooling/mixing of the bulk tank fluid to allow storage of the cryogenic fluid with zero or reduced boil-off. The presence of noncondensable gases, can interfere with the condensation at the interface impacting tank pressure control during subcooled jet mixing especially in microgravity. The Zero-Boil-Off Tank (ZBOT) Experiments are a series of small-scale experiments aboard the International Space Station (ISS) that use a transparent volatile simulant fluid in a transparent sealed tank to delineate various fundamental fluid flow, heat and mass transport, and phase change phenomena associated with storage tank pressurization and pressure control in microgravity. The ZBOT-1 experiment was performed on the ISS 2017-2018 timeframe and collected data to validate a state-of-the-art CFD model for tank pressurization and pressure control for a pure system. The ZBOT-NC Experiment is the second experiment in the series to be performed on the International Space Station (ISS) in 2025. Its goal is to investigate the effects of noncondensable gases on interfacial evaporation and condensation during self -pressurization and jet-mixing pressure control in microgravity for a two-component system. Materials & Methods In this work, we will describe the detailed features of the ZBOT-NC experimental hardware and Diagnostics that includes nonintrusive Quantum Dot Thermometry (QDT) for whole field temperature measurement. All microgravity pressurization and pressure control tests will be performed for both the pure and the two-components systems with Xenon and Neon as the two noncondensable gases spanning small and large molecular weights and sizes. The two-phase CFD model that is developed as part of the project will be also presented and discussed. Results Ground-based pressurization and jet mixing experiments and CFD simulation results are compared to each other to validate both the fidelity of the CFD model predictions and the accuracy of the QDT measurement. Model simulations for noncondensable gas effects will also be compared against large Cryogenic LH2-GHe experiments to indicate the noncondensable gas effects on tank pressure control during jet mixing in 1G. Finally, CFD results will be presented to predict the effects of the noncondensable gas during subcooled jet mixing during the ZBOT-NC in advance of the microgravity experiment in 2015.

Evaporation Condensation↗

The composition of gases from a diffusion flame above longleaf pine needle fuel beds

The gas and tar composition of a diffusion flame from longleaf pine needles is currently poorly understood and more data are needed to fill in the gap between pyrolysis data and smoke plume data, thus improving physical and chemical modeling of wildland smoke formation. A pilot experiment to measure light gas and tar composition of such a flame is described for three flame regions: persistent flame (flame base), intermittent flame, and smoke plume. Flame gases from 24 experimental fires were collected in canisters and analyzed using EPA method TO-14A for CO 2 , CO, H 2 , CH 4 , and C 2 to C 7 hydrocarbon gases. Condensed gas (tar) samples were collected and analyzed using GC/MS. Other light gases were measured using FTIR spectroscopy. Results from compositional data analysis suggest significant differences in (relative) concentration of compounds detected in the three regions of the flame. Statistical tests for differences in flame zones were performed using the canister data: Concentration of hydrocarbons relative to CO and CO 2 decreased from the persistent flame zone above the pyrolyzing needles through the intermittent flame region into the flame-free plume. This was likely due to both chemical reactions (oxidation) occurring in the flame as well as the introduction of air into the flame/plume by entrainment.

Biomass↗

Real-time monitoring of trace noble gases using laser-induced breakdown spectroscopy—An investigation of the impact of bulk gas on plasma properties and sensitivity

The impact of Ar and He bulk gases on laser-induced breakdown spectroscopy (LIBS) real-time monitoring of trace Xe and Kr was assessed. LIBS is being developed as a monitoring tool for measuring noble gas transport in molten salt systems, in which traditional sensors may face challenges associated with radiation, corrosive materials, and/or mixed phases. The plasma temperature and electron densities of LIBS plasmas were measured in both static and various flowing Ar and He streams (0–5 L min −1 ). The use of an Ar bulk gas resulted in higher plasma temperature, greater electron densities by an order of magnitude, and extended plasma lifetime compared with when He bulk gas was used. Gas flow rate was found to have little impact on plasma temperature; however, its effect on electron density was significant, indicating the need to consider flow rate–specific models. Matrix effects on emission peaks were reported for both bulk gases. Due to these matrix effects, multivariate models were developed for Xe and Kr ranging from 0 to 700 ppm in both bulk gases. Although the predictive behavior was similar (root mean square error of prediction ranging from 11.1 to 20.6 ppm), the limits of detection were superior in He (Xe: 22.9 ppm, Kr: 30.4 ppm). Furthermore, these models were employed in demonstrative real-time tests (>1 h), which showed strong predictive precision (relative standard deviation <5 %) regardless of the bulk gas. Ultimately, this study provides a guide for the considerations required when developing gaseous LIBS models for real-time monitoring.

Gas flow effects↗

Benchmark calculations of radiative forcing by greenhouse gases

Changes in concentrations of greenhouse gases lead to changes in radiative fluxes throughout the atmosphere. The value of this change, the instantaneous radiative forcing, varies across climate models, due partly to differences in the distribution of clouds, humidity, and temperature across models, and partly due to errors introduced by approximate treatments of radiative transfer. This paper describes an experiment within the Radiative Forcing Model Intercomparision Project that uses benchmark calculations made with line–by–line models to identify parameterization error in the representation of absorption and emission by greenhouse gases. Clear–sky instantaneous forcing by greenhouse gases is computed using a set of 100 profiles, selected from a re–analysis of present–day conditions, that represent the global annual mean forcing from pre–industrial times to the present–day with sampling errors of less than 0.01 W m –2 . Six contributing line–by–line models agree in their estimate of this forcing to within 0.025 W m –2 while even recently–developed parameterizations have typical errors four or more times larger, suggesting both that the samples reveal true differences among line–by–line models and that parameterization error will be readily identifiable. Agreement among line–by–line models is better in the longwave than in the shortwave where differing treatments of the water vapor vapor continuum affect estimates of forcing by carbon dioxide and methane. The impacts of clouds on instantaneous radiative forcing are estimated from climate model simulations. Here, the adjustment due to stratospheric temperature change by assuming fixed dynamical heating. Adjustments are large only for ozone and for carbon dioxide, for which stratospheric cooling introduces modest non–linearity.

54 ENVIRONMENTAL SCIENCES↗

In-situ measurements of chemically and radiatively important atmospheric gases from the Advanced Global Atmospheric Gas Experiment (AGAGE) and affiliated stations.

In the ALE/GAGE/AGAGE global network program, continuous high frequency gas chromatographic measurements of four biogenic/anthropogenic gases (methane, CH4; nitrous oxide, N2O; hydrogen, H2; and carbon monoxide, CO) and several anthropogenic gases that contribute to stratospheric ozone destruction and/or to the greenhouse effect have been carried out at five globally distributed sites for several years. The program, which began in 1978, is divided into three parts associated with three changes in instrumentation: the Atmospheric Lifetime Experiment (ALE), which used Hewlett Packard HP5840 gas chromatographs; the Global Atmospheric Gases Experiment (GAGE), which used HP5880 gas chromatographs; and the present Advanced GAGE (AGAGE). AGAGE uses two types of instruments: a gas chromatograph with multiple detectors (GC-MD), and a gas chromatograph with mass spectrometric analysis (GC-MS). Beginning in January 2004, an improved cryogenic preconcentration system (Medusa) replaced the absorption-desorption module in the GC-MS systems at Mace Head and Cape Grim; this provided improved capability to measure a broader range of volatile perfluorocarbons with high global warming potentials. The Medusa GC-MS systems were subsequently used at other AGAGE stations (Trinidad Head, Barbados, American Samoa, Zeppelin, Jungfraujoch, and Goan) after the initial setup at Mace Head and Cape Grim. More information may be found at the AGAGE home page: https://agage.mit.edu/instruments.Compared to the previous version (https://data.ess-dive.lbl.gov/view/doi:10.3334/CDIAC/ATG.DB1001), the latest update (Agage_gcmd_gcms_data_2021_04_07_tar.gz) includes 6 months of new data through the end of March 2020. Two new compounds, HCFC-132b, and HCFC-133a, are also included in this version. For a complete list of released compounds and used standard scales, please see “AGAGE_scale_2021_v1.pdf” file. Additional information can also be found on the AGAGE website (https://agage.mit.edu).

54 ENVIRONMENTAL SCIENCES↗

The Advanced Global Atmospheric Gases Experiment (AGAGE) Data

In the ALE/GAGE/AGAGE global network program, continuous high frequency gas chromatographic measurements of four biogenic/anthropogenic gases (methane, CH4; nitrous oxide, N2O; hydrogen, H2; and carbon monoxide, CO) and several anthropogenic gases that contribute to stratospheric ozone destruction and/or to the greenhouse effect have been carried out at five globally distributed sites for several years. The program, which began in 1978, is divided into three parts associated with three changes in instrumentation: the Atmospheric Lifetime Experiment (ALE), which used Hewlett Packard HP5840 gas chromatographs; the Global Atmospheric Gases Experiment (GAGE), which used HP5880 gas chromatographs; and the present Advanced GAGE (AGAGE). AGAGE uses two types of instruments: a gas chromatograph with multiple detectors (GC-MD), and a gas chromatograph with mass spectrometric analysis (GC-MS). Beginning in January 2004, an improved cryogenic preconcentration system (Medusa) replaced the absorption-desorption module in the GC-MS systems at Mace Head and Cape Grim; this provided improved capability to measure a broader range of volatile perfluorocarbons with high global warming potentials. The Medusa GC-MS systems were subsequently used at other AGAGE stations (Trinidad Head, Barbados, American Samoa, Zeppelin, Jungfraujoch, and Goan) after the initial setup at Mace Head and Cape Grim. More information may be found at the AGAGE home page: https://agage.mit.edu/instruments.Compared to the previous version (https://data.ess-dive.lbl.gov/datasets/doi: doi:10.15485/1781803), the latest update (Agage_gcmd_gcms.data.2022_01_03.tar.gz) includes 6 months of new data through the end of September 2020. For a complete list of released compounds and used standard scales, please see “AGAGE_scale_2021_v1.pdf” file. Additional information can also be found on the AGAGE website (https://agage.mit.edu).

54 ENVIRONMENTAL SCIENCES↗

Stable isotopes of carbon dioxide (CO2), dissolved inorganic carbon (DIC), water and concentrations of greenhouse gases in a mountainous watershed (Crested Butte, Colorado)

Temperature and precipitation variability in response to climate change affects water cycling of watersheds and can potentially impact water quality, water availability, elemental and molecular fluxes, and biogeochemical processes. Here we report the measurements of light stable isotopes and greenhouse gases analysis to a large multidisciplinary project addressing watershed function. Water hydrogen (H) and oxygen (O) stable isotopes of snow and water saturated soil were measured to constrain source contributions to groundwater and streamflow. In an effort to better constrain existing nitrogen and carbon cycling models in high-altitude ecosystems, carbon dioxide (CO2), nitrous oxide (N2O), methane (CH4) greenhouse gases concentrations and stable isotope signatures of CO2, dissolved inorganic carbon (DIC), and water were measured. This dataset includes one CSV file and one Excel file containing data including stable isotopes of carbon dioxide (CO2), dissolved inorganic carbon (DIC), water and concentrations of greenhouse gases. The CSV and Excel files contain the same information/data but have included both versions for accessibility.

54 ENVIRONMENTAL SCIENCES↗

The dataset of in-situ measurements of chemically and radiatively important atmospheric gases from the AGAGE and affiliated stations (2022R1)

In the ALE/GAGE/AGAGE global network program, continuous high frequency gas chromatographic measurements of four biogenic/anthropogenic gases (methane, CH4; nitrous oxide, N2O; hydrogen, H2; and carbon monoxide, CO) and several anthropogenic gases that contribute to stratospheric ozone destruction and/or to the greenhouse effect have been carried out at five globally distributed sites for several years. The program, which began in 1978, is divided into three parts associated with three changes in instrumentation: the Atmospheric Lifetime Experiment (ALE), which used Hewlett Packard HP5840 gas chromatographs; the Global Atmospheric Gases Experiment (GAGE), which used HP5880 gas chromatographs; and the present Advanced GAGE (AGAGE). AGAGE uses two types of instruments: a gas chromatograph with multiple detectors (GC-MD), and a gas chromatograph with mass spectrometric analysis (GC-MS). Beginning in January 2004, an improved cryogenic preconcentration system (Medusa) replaced the absorption-desorption module in the GC-MS systems at Mace Head and Cape Grim; this provided improved capability to measure a broader range of volatile perfluorocarbons with high global warming potentials. The Medusa GC-MS systems were subsequently used at other AGAGE stations (Trinidad Head, Barbados, American Samoa, Zeppelin, Jungfraujoch, and Goan) after the initial setup at Mace Head and Cape Grim. More information may be found at the AGAGE home page: https://agage.mit.edu/instruments. Data from the AGAGE and affiliated stations (total of 9 sites) between August 1993 and March 2021 are provided in “Agage_gcmd_gcms_data_2022_05_26_tar.gz” (compressed tar file). The metadata file has information on each station and currently released species. The standard scales used in archived species are listed in "AGAGE_scale_2022_v1.pdf". Additional information can be found on the AGAGE website (https://agage.mit.edu).

54 ENVIRONMENTAL SCIENCES↗