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  • 1
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Infrared spectra of clusters of protonated nitric acid and water exhibit a marked change with cluster size, indicating that an intracluster reaction occurs with sufficient solvation. In small clusters, H2O binds to a nitronium ion core, but at a critical cluster size the NO+2 reacts. A lower bound of 174 kcal/mol is found for the proton affinity of HNO3.
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  • 2
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Infrared spectra of mass-selected clusters NO+(H2O)n for n=1 to 5 were recorded from 2700 to 3800 cm−1 by vibrational predissociation spectroscopy. Vibrational frequencies and intensities were also calculated for n=1 and 2 at the second-order Møller–Plesset (MP2) level, to aid in the interpretation of the spectra, and at the singles and doubles coupled cluster (CCSD) level energies of n=1 isomers were computed at the MP2 geometries. The smaller clusters (n=1 to 3) were complexes of H2O ligands bound to a nitrosonium ion NO+ core. They possessed perturbed H2O stretch bands and dissociated by loss of H2O. The H2O antisymmetric stretch was absent in n=1 and gradually increased in intensity with n. In the n=4 clusters, we found evidence for the beginning of a second solvation shell as well as the onset of an intracluster reaction that formed HONO. These clusters exhibited additional weak, broad bands between 3200 and 3400 cm−1 and two new minor photodissociation channels, loss of HONO and loss of two H2O molecules. The reaction appeared to go to completion within the n=5 clusters. The primary dissociation channel was loss of HONO, and seven vibrational bands were observed. From an analysis of the spectrum, we concluded that the n=5 cluster rearranged to form H3O+(H2O)3(HONO), i.e., an adduct of the reaction products.
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  • 3
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
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  • 4
    Publication Date: 2019-07-20
    Description: Greenhouse gas (GHG) concentrations have increased over the past decades and are linked to global temperature increases and climate change. These changes in climate have been suggested to have varying effects, and uncertain consequences, on agriculture, water supply, weather, sea-level rise, the economy, and energy. To counteract the trend of increasing atmospheric concentrations of GHGs, the state of California has passed the California Global Warming Act of 2006 (AB-32). This requires that by the year 2020, GHG (e.g., carbon dioxide (CO2) and methane (CH4)) emissions will be reduced to 1990 levels. To quantify GHG fluxes, emission inventories are routinely compiled for the State of California (e.g., CH4 emissions from the California Greenhouse Gas Emissions Measurement (CALGEM) Project). The major sources of CO2 and CH4 in the state of California are: transportation, electricity production, oil and gas extraction, cement plants, agriculture, landfills/waste, livestock, and wetlands. However, uncertainties remain in these emission inventories because many factors contributing to these processes are poorly quantified. To alleviate these uncertainties, a synergistic approach of applying air-borne measurements and chemical transport modeling (CTM) efforts to provide a method of quantifying local and regional GHG emissions will be performed during this study. Additionally, in order to further understand the temporal and spatial distributions of GHG fluxes in California and the impact these species have on regional climate, CTM simulations of daily variations and seasonality of total column CO2 and CH4 will be analyzed. To assess the magnitude and spatial variation of GHG emissions and to identify local hot spots, airborne measurements of CH4 and CO2 were made by the Alpha Jet Atmospheric eXperiment (AJAX) over the San Francisco Bay Area (SFBA) and San Joaquin Valley (SJV) in January and February 2013 during the Discover-AQ-CA study. High mixing ratios of GHGs were observed in-flight with a high degree of spatial variability. To provide an additional method to quantify GHG emissions, and analyze AJAX measurement data, the GEOS-Chem CTM is used to simulate SFBA/SJV GHG measurements. A nested-grid version of GEOS-Chem will be applied and utilizes varying emission inventories and model parameterizations to simulate GHG fluxes/emissions. The model considers CO2 fluxes from fossil fuel use, biomass/biofuel burning, terrestrial and oceanic biosphere exchanges, shipping and aviation, and production from the oxidation of carbon monoxide, CH4, and non-methane volatile organic carbons. The major sources of CH4 simulated in GEOS-Chem are domesticated animals, rice fields, natural gas leakage, natural gas venting/flaring (oil production), coal mining, wetlands, and biomass burning. Preliminary results from the comparison between available observations (e.g., AJAX and CALGEM CH4 emission maps) and GEOS-Chem results will be presented, along with a discussion of CO2 and CH4 source apportionment and the use of the GEOS-Chem-adjoint to perform inverse GHG modeling.
    Keywords: Earth Resources and Remote Sensing
    Type: ARC-E-DAA-TN11653 , AGU Fall Meeting; Dec 09, 2013 - Dec 13, 2013; San Francisco, CA; United States
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  • 5
    Publication Date: 2019-07-19
    Description: Ozone (O3) is a toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address the limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME (Global Ozone Monitoring Experiment), GOME-2, and OMI (Ozone Monitoring Instrument). This algorithm is suggested to use a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB-Clim) O3 climatology). This study evaluates the TB-Clim dataset and model simulated O3 profiles, which could potentially serve as a priori O3 profile information in TEMPO retrievals, from near-real-time data assimilation model products (NASA GMAO's (Global Modeling and Assimilation Office) operational GEOS-5 (Goddard Earth Observing System, Version 5) FP (Forecast Products) model and reanalysis data from MERRA2 (Modern-Era Retrospective analysis for Research and Applications, Version 2)) and a full chemical transport model (CTM), GEOS-Chem. In this study, vertical profile products are evaluated with surface (0-2 kilometers) and tropospheric (0-10 kilometers) TOLNet (Tropospheric Ozone Lidar Network) observations and the theoretical impact of individual a priori profile sources on the accuracy of TEMPO O3 retrievals in the troposphere and at the surface are presented. Results indicate that while the TB-Clim climatological dataset can replicate seasonally-averaged tropospheric O3 profiles, model-simulated profiles from a full CTM resulted in more accurate tropospheric and surface-level O3 retrievals from TEMPO when compared to hourly and daily-averaged TOLNet observations. Furthermore, it is shown that when large surface O3 mixing ratios are observed, TEMPO retrieval values at the surface are most accurate when applying CTM a priori profile information compared to all other data products.
    Keywords: Environment Pollution
    Type: ARC-E-DAA-TN46979 , AGU Fall Meeting 2017; Dec 11, 2017 - Dec 15, 2017; New Orleans, LA; United States
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  • 6
    Publication Date: 2019-07-19
    Description: High ozone (O3) concentrations at low altitudes (1.5e4 km) were detected from airborne Alpha Jet Atmospheric eXperiment (AJAX) measurements on 30 May 2012 off the coast of California (CA). We investigate the causes of those elevated O3 concentrations using airborne measurements and various models. GEOS-Chem simulation shows that the contribution from local sources is likely small. A back trajectory model was used to determine the air mass origins and how much they contributed to the O3 over CA. Low-level potential vorticity (PV) from Modern Era Retrospective analysis for Research and Applications 2 (MERRA-2) reanalysis data appears to be a result of the diabatic heating and mixing of airs in the lower altitudes, rather than be a result of direct transport from stratospheric intrusion. The Q diagnostic, which is a measure of the mixing of the air masses, indicates that there is sufficient mixing along the trajectory to indicate that O3 from the different origins is mixed and transported to the western U.S.The back-trajectory model simulation demonstrates the air masses of interest came mostly from the mid troposphere (MT, 76), but the contribution of the lower troposphere (LT, 19) is also significant compared to those from the upper troposphere/lower stratosphere (UTLS, 5). Air coming from the LT appears to be mostly originating over Asia. The possible surface impact of the high O3 transported aloft on the surface O3 concentration through vertical and horizontal transport within a few days is substantiated by the influence maps determined from the Weather Research and Forecasting Stochastic Time Inverted Lagrangian Transport (WRF-STILT) model and the observed increases in surface ozone mixing ratios. Contrasting this complex case with a stratospheric-dominant event emphasizes the contribution of each source to the high O3 concentration in the lower altitudes over CA. Integrated analyses using models, reanalysis, and diagnostic tools, allows high ozone values detected by in-situ measurements to be attributed to multiple source processes.
    Keywords: Earth Resources and Remote Sensing
    Type: ARC-E-DAA-TN42777 , Atmospheric Environment (ISSN 1352-2310); 155; 53-57
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  • 7
    Publication Date: 2019-07-19
    Description: Marine-sourced organic aerosols (MOA) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem model. The implemented emission scheme improved the large under-prediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from -79% when using the default settings to -12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of -36%) with hourly surface concentrations of MOA observed during the summertime at an inland site near Paris, France. Our study shows that MOA have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having 〉 10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly-emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.
    Keywords: Earth Resources and Remote Sensing
    Type: ARC-E-DAA-TN20802 , NCTS# 21764-15 The International GEOS-Chem Meeting; May 04, 2015 - May 07, 2015; Cambridge, MA; United States
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  • 8
    Publication Date: 2019-07-19
    Description: High ozone concentrations at low altitudes near the surface were detected from airborne Alpha Jet Atmospheric eXperiment (AJAX) measurements on May 30, 2012. We investigate the causes of the elevated ozone concentrations using the airborne measurements and various models. GEOS-chem and WRF-STILT model simulations show that the contribution from local sources is small. From MERRA reanalysis, it is found that high potential vorticity (PV) is observed at low altitudes. This high PV appears to be only partially coming through the stratospheric intrusions because the air inside the high PV region is moist, which shows that mixing appears to be enhanced in the low altitudes. Considering that diabatic heating can also produce high PV in the lower troposphere, high ozone is partially coming through stratospheric intrusion, but this cannot explain the whole ozone concentration in the target areas of the western U.S. A back-trajectory model is utilized to see where the air masses originated. The air masses of the target areas came from the lower stratosphere (LS), upper (UT), mid- (MT), and lower troposphere (LT). The relative number of trajectories coming from LS and UT is low (7.7 and 7.6, respectively) compared to that from LT (64.1), but the relative ozone concentration coming from LS and UT is high (38.4 and 20.95, respectively) compared to that from LT (17.7). The air mass coming from LT appears to be mostly coming from Asia. Q diagnostics show that there is sufficient mixing along the trajectory to indicate that ozone from the different origins is mixed and transported to the western U.S. This study shows that high ozone concentrations can be detected by airborne measurements, which can be analyzed by integrated platforms such as models, reanalysis, and satellite data.
    Keywords: Environment Pollution
    Type: ARC-E-DAA-TN29592 , AGU Fall Meeting 2015; Dec 14, 2015 - Dec 18, 2015; San Francisco, CA; United States
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  • 9
    Publication Date: 2019-07-19
    Description: Ozone (O3) is an important greenhouse gas, toxic pollutant, and plays a major role in atmospheric chemistry. Tropospheric O3 which resides in the planetary boundary layer (PBL) is highly reactive and has a lifetime on the order of days, however, O3 in the free troposphere and stratosphere has a lifetime on the order of weeks or months. Modeling O3 mixing ratios at and above the surface is difficult due to the multiple formation/destruction processes and transport pathways that cause large spatio-temporal variability in O3 mixing ratios. This talk will summarize in detail the global/regional models that are commonly used to simulate/predict O3 mixing ratios in the United States. The major models which will be focused on are the: 1) Community Multi-scale Air Quality Model (CMAQ), 2) Comprehensive Air Quality Model with Extensions (CAMx), 3) Goddard Earth Observing System with Chemistry (GEOS-Chem), 4) Real Time Air Quality Modeling System (RAQMS), 5) Weather Research and Forecasting/Chemistry (WRF-Chem) model, National Center for Atmospheric Research (NCAR)'s Model for OZone And Related chemical Tracers (MOZART), and 7) Geophysical Fluid Dynamics Laboratory (GFDL) AM3 model. I will discuss the major modeling components which impact O3 mixing ratio calculations in each model and the similarities/differences between these models. This presentation is vital to the 2nd Annual Tropospheric Ozone Lidar Network (TOLNet) Conference as it will provide an overview of tools, which can be used in conjunction with TOLNet data, to evaluate the complex chemistry and transport pathways controlling tropospheric O3 mixing ratios.
    Keywords: Geophysics
    Type: ARC-E-DAA-TN22608 , TOLNet (Tropospheric Ozone LIDAR Network) Workshop.; Jun 16, 2015 - Jun 18, 2015; Boulder, CO; United States
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  • 10
    Publication Date: 2019-07-19
    Description: The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is a five-year Earth-Venture Suborbital-2 Mission to characterize the plankton ecosystems and their influences on remote marine aerosols, boundary layer clouds, and their implications for climate in the North Atlantic. While marine-sourced aerosols have been shown to make important contributions to surface aerosol loading, cloud condensation nuclei and ice nuclei concentrations over remote marine and coastal regions, it is still a challenge to differentiate the marine biogenic aerosol signal from the strong influence of continental pollution outflow. We examine here the spatiotemporal variability and quantify the sources of tropospheric aerosols over the North Atlantic during the first two phases (November 2015 and May-June 2016) of NAAMES using a state-of-the-art chemical transport model (GEOS-Chem). The model is driven by the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) from the NASA Global Modeling and Assimilation Office (GMAO). It includes sulfate-nitrate-ammonium aerosol thermodynamics coupled to ozone-NOx-hydrocarbon-aerosol chemistry, mineral dust, sea salt, elemental and organic carbon aerosols, and especially a recently implemented parameterization for the marine primary organic aerosol emission. The simulated aerosols over the North Atlantic are evaluated with available satellite (e.g., MODIS) observations of aerosol optical depths (AOD), and aircraft and ship aerosol measurements. We diagnose transport pathways for continental pollution outflow over the North Atlantic using carbon monoxide, an excellent tracer for anthropogenic pollution transport. We also conduct model perturbation experiments to quantify the relative contributions of terrestrial and oceanic sources to the aerosol loading, AOD, and their variability over the North Atlantic.
    Keywords: Earth Resources and Remote Sensing
    Type: ARC-E-DAA-TN38154 , 2016 AGU Fall Meeting; Dec 12, 2016 - Dec 16, 2016; San Francisco, CA; United States
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