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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

An Observation-Based, Reduced-Form Model for Oxidation in the Remote Marine Troposphere

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short term, spatial variations in OH (Proxy OH ) in the remote marine troposphere using unprecedented and comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. Proxy OH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. Proxy OH comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. ProxyOH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r 2 = 0.90, interquartile range = 0.80 – 0.94 across 2 km altitude by 20° latitudinal regions). We deconstruct spatial variations in Proxy OH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region Proxy OH variations—water vapor (H 2 O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer a novel avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H 2 O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of Proxy OH as a process-based approach for evaluating inter-model differences in remote marine tropospheric OH.

Colleen B. Baublitz↗

Nonmethane hydrocarbon chemistry in the remote marine boundary layer

A photochemical model of the remote marine boundary layer (MBL) is presented, with focus placed on the role of reactive nonmethane hydrocarbons (NMHC). A wide range of NMHC air-sea fluxes with various relative distributions of NMHC regions are considered. In particular, the flux magnitude at which NMHC emissions become significant, and then dominant, players in MBL chemistry is identified. Emphasis is placed on diurnal variability, diurnal ozone variations and sensitivity to NMHC emission fluxes, to CO, O3, H2O, and UV light, and to kinetics and isometric composition. Model runs indicate that, in the range consistent with current observations, the NMHCs may either dominate MBL chemistry, or simply be contributors at the 10-percent level. These model runs also show that existing observations of NMHCs in ocean water find them to scarce for fluxes from bulk-flux air-sea gas exchange models to be consistent with the fluxes needed in the proposed model to maintain the lowest observed MBL NMHC.

Donahue, Neil M.↗

Remote Marine Aerosol: A Characterization of Physical, Chemical and Optical Properties and their Relation to Radiative Transfer in the Troposphere

Our research effort is focused on improving our understanding of aerosol properties needed for optical models for remote marine regions. This includes in-situ and vertical column optical closure and involves a redundancy of approaches to measure and model optical properties that must be self consistent. The model is based upon measured in-situ aerosol properties and will be tested and constrained by the vertically measured spectral differential optical depth of the marine boundary layer, MBL. Both measured and modeled column optical properties for the boundary layer, when added to the free-troposphere and stratospheric optical depth, will be used to establish spectral optical depth over the entire atmospheric column for comparison to and validation of satellite derived radiances (AVHRR).

Clarke, Antony D.↗

The photochemistry of a remote marine stratiform cloud

The coupled gas- and aqueous-phase photochemistry of a stratiform cloud in a remote region of the marine atmosphere is investigated with a time-dependent box model. Both scavenging of ambient acidic aerosols and gases as well as aqueous-phase chemical reactions within droplets are found to be important sources of acidity to cloud water and can lead to pH levels in cloud water in the remote marine atmosphere well below 5.6. The major sources of acidity via aqueous-phase chemical reactions are the generation of sulfuric acid from dissolved SO2 and the generation of formic acid from dissolved formaldehyde. In both cases, aqueous-phase free radicals can play a significant role either directly by oxidizing dissolved SO2 and HCHO or indirectly by producing the aqueous-phase oxidant H2O2. The rate of SO2 conversion to sulfuric acid is sensitive to a variety of parameters including the accommodation or sticking coefficient for SO2, H2O2, HO2, and OH, the liquid water content, and the ambient levels of SO2, HNO3, and other acidic or basic gases. Because high levels of SO2 tend to deplete cloud water of H2O3, the possibility exists that the pH of precipitation in polluted regions will respond nonlinearly to reduced SO2 emissions.

Chameides, W. L.↗

Remote Marine Aerosol Properties over the Western North Atlantic Ocean during NAAMES

The overarching goal of this postdoctoral project is: quantitatively assess and constrain the aerosol budgets in the remote North Atlantic marine boundary layer, under a wide range of aerosol emission sources, meteorological states to improve process-level understanding of marine aerosol-cloud interactions critical to adequately link observations and climate modelling.

Aerosol NAAMES↗

Determining the Primary Sources of Uncertainty in Retrieval of Marine Remote Sensing Reflectance From Satellite Ocean Color Sensors

Uncertainties in the retrieval of the remote sensing reflectance, R_rs, from Ocean Color (OC) satellite sensors have a strong impact on the performance of algorithms for the estimation of chlorophyll-a, mineral concentrations, and inherent optical properties (IOPs). The uncertainties are highest in the blue bands. The total radiance measured at the top of the atmosphere captures the instantaneous state of the atmosphere-ocean system: the in-water conditions, sky and Sun glint reflected from the wind-roughened ocean surface, as well as light scattered from molecules and aerosols in the atmosphere. Each of these components has associated uncertainties, and when combined with the additional uncertainties from the instrument noise and the atmospheric correction process, they contribute to the total uncertainty budget for the retrieved R_rs. We analyzed the contribution of each component uncertainties to the total R_rs uncertainties in SNPP-VIIRS level 2 products, taking advantage of the spectral differences between the components. We examined multiple scenes in the open ocean and coastal waters at spatial resolutions ranging from 2250 to 5250 m by comparing the retrieved R_rs to in situ measurements made at several AERONET-OC sites and at the MOBY site. It was shown that uncertainties associated with the molecular (Rayleigh) scattering play the most significant role, while the contributions of other components are usually smaller. Uncertainties in Rayleigh scattering are primarily attributed to the variability of Rayleigh optical thickness (ROT) with a standard deviation of approximately 1.5% of ROT, which can largely explain the frequency of negative R_rs retrievals as observed using the current standard atmospheric correction process employed by NASA. Variability of the sky light reflected from the ocean surface in some conditions also contributed to uncertainties in the blue; water variability proportional to R_rs had a very pronounced peak in the green at coastal sites.

remote sensing reflectance↗

On the sensitivity of numerical weather prediction to remotely sensed marine surface wind data - A simulation study

The reported investigation has the objective to assess the potential impact on numerical weather prediction (NWP) of remotely sensed surface wind data. Other investigations conducted with similar objectives have not been satisfactory in connection with a use of procedures providing an unrealistic distribution of initial errors. In the current study, care has been taken to duplicate the actual distribution of information in the conventional observing system, thus shifting the emphasis from accuracy of the data to the data coverage. It is pointed out that this is an important consideration in assessing satellite observing systems since experience with sounder data has shown that improvements in forecasts due to satellite-derived information is due less to a general error reduction than to the ability to fill data-sparse regions. The reported study concentrates on the evaluation of the observing system simulation experimental design and on the assessment of the potential of remotely sensed marine surface wind data.

Cane, M. A.↗

Exchange of sulfur between the free troposphere, marine boundary layer, and the sea surface

A steady state analysis has been made of the sources and sinks of sulfur in the remote marine atmosphere and of the steady state exhanges of SO2 and sulfate between the sea, boundary layer, and free troposphere. Two situations were examined: an area of high biological productivity (Gulf of Guinea) and an area of low productivity (tropical Atlantic). The results of the analysis suggest that about one-third of the background concentrations of SO2 and excess sulfate observed in the remote marine atmosphere mixes in from the free troposphere, with the balance, about 100 micrograms S/sq m per day, attributed to the local oxidation of reduced sulfur-bearing precursors in the boundary layer.

Kritz, M. A.↗

TPSAS-NF1676L-33032-DND

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES; http://naames.larc.nasa.gov) is a five-year NASA 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. The objectives of this study are to determine the major transport pathways for North American pollution outflow to the North Atlantic, and to quantify the terrestrial and marine sources of aerosols during NAAMES using ground, ship, aircraft, and remote sensing observations in conjunction with a state-of-the-art global 3-D chemical transport model (GEOS-Chem). This poster presents an initial evaluation of GEOS-Chemfor the periods of NAAMES campaigns #1 (Nov. 2015) and #2 (May 2016).

Hongyu Liu↗

A51F-0123: Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

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.

aerosols↗

Theoretical and global scale model studies of the atmospheric sulfur/aerosol system

The primary focus during the third-phase of our on-going multi-year research effort has been on 3 activities. These are: (1) a global-scale model study of the anthropogenic component of the tropospheric sulfur cycle; (2) process-scale model studies of the factors influencing the distribution of aerosols in the remote marine atmosphere; and (3) an investigation of the mechanism of the OH-initiated oxidation of DMS in the remote marine boundary layer. In this paper, we describe in more detail our research activities in each of these areas. A major portion of our activities during the fourth and final phase of this project will involve the preparation and submission of manuscripts describing the results from our model studies of marine boundary-layer aerosols and DMS-oxidation mechanisms.

Kasibhatla, Prasad↗

Validation of Formaldehyde Products From Three Satellite Retrievals (OMI SAO, OMPS-NPP SAO, and OMI BIRA) in the Marine Atmosphere With Four Seasons of Atom Aircraft Observations

Formaldehyde (HCHO) in the atmosphere is an intermediate product from the oxidation of methane and non-methane volatile organic compounds. In remote marine regions, HCHO variability is closely related to atmospheric oxidation capacity and modeled HCHO in these regions is usually added as a global satellite HCHO background. Thus, it is important to understand and validate the levels of satellite HCHO over the remote oceans. Here we intercompare three satellite retrievals of total HCHO columns (OMI-SAO (v004), OMPS-NPP SAO, and OMI BIRA) and validate them against in situ observations from the NASA Atmospheric Tomography Mission (ATom) mission. All retrievals are correlated with ATom integrated columns over remote oceans, with OMI SAO (v004) showing the best agreement. This is also reflected in the mean bias (MB) for OMI SAO (-0.73±0.87) x 10 15 molec cm -2 , OMPS SAO (-0.76±0.88) x 10 15 molec cm -2 , and OMI BIRA (-1.40±1.11) x 10 15 molec cm -2 . We recommend the OMI-SAO (v004) retrieval for remote ocean atmosphere studies. Three satellite HCHO retrievals and in situ ATom columns all generally captured the spatial and seasonal distributions of HCHO in the remote ocean atmosphere. Retrieval bias varies by latitude and season, but a persistent low bias is found in all products at high latitudes and the general low bias is most severe for the OMI BIRA product. Examination of retrieval components reveals slant column corrections have a larger impact on the retrievals over remote marine regions while AMFs play a smaller role. This study informs that the potential latitude-dependent biases in the retrievals require further investigation for improvement and should be considered when using marine HCHO satellite data, and vertical profiles from in situ instruments are crucial for validating satellite retrievals.

Atom↗

Dimethylsulfide oxidation over the tropical South Atlantic: OH and other oxidants

The general course of events in the formation of a marine cloud begins with the emission of species which can eventually serve as nuclei around which water can condense to form a cloud droplet. In remote marine regions, cloud condensation nuclei (CCN) are primarily composed of sulfate, in either its acid or ammonium salt form. Most sulfate in these regions is the product of atmospheric oxidation of dimethyl sulfide (DMS), a reduced sulfur gas that is released by phytoplankton at the ocean surface. Therefore, in order to effectively quantify the links in the cloud-formation cycle, one must begin with a well-defined description of the atmospheric chemistry of DMS. The intent of this project has been to initiate development of a comprehensive model of the chemistry and dynamics responsible for the formation of clouds in the remote marine boundary layer. The primary tool in this work has been the Global/Regional Atmospheric Chemistry Event Simulator (GRACES), a global atmospheric chemistry model, which is under development within the Atmospheric Chemistry and Dynamics Branch of NASA-Ames Research Center. In this effort, GRACES was used to explore the first chemical link between DMS and sulfate by modeling the diurnal variation of DMS.

Hemming, Brooke L.↗

Evaluation of bio-optical algorithms to remotely sense marine primary production from space

In situ bio-optical measurements from several oceanographic campaigns were analyzed to derive a direct relationship between water column primary production P (sub t) ocean color as expressed by the ratio of reflectances R (sub 1) at 440 nm and R (sub 3) at 550 nm and photosynthetically available radiation (PAR). The study is restricted to the Morel case I waters for which the following algorithm is proposed: log (P(sub f)) = -4.286 - 1.390 log (R(sub 1)/R(sub3)) + 0.621 log (PAR), with P(sub t) in g C m(exp -2)/d and PAR in J m(exp -2)/d. Using this algorithm the rms accuracy of primary production estimate is 0.17 on a logarithmic scale, i.e., a factor of 1.5. Using spectral reflectance measurements in the entire visible spectral range, the central wavelength, spectral bandwidth, and radiometric noise level requirements are investigated for the channels to be used by an ocean color space mission dedicated to estimating global marine primary production and the associated carbon fluxes. Nearly all the useful information is provided by two channels centered at 440 nm and 550 nm, but the accuracy of primary production estimate appears weakly sensitive to spectral bandwidth, which, consequently, may be enlarged by several tens of nanometers. The sensitivity to radiometric noise, on the contrary, is strong, and a noise equivalent reflectance of 0.005 degraded the accuracy on the primary production estimate by a factor 2 (0.14-0.25 on a logarithmic scale). The results should be applicable to evaluating the primary production of oligotrophic and mesotrophic waters, which constitute most of the open ocean.

Berthelot, Beatrice↗

Clouds and wet removal as causes of variability in the trace-gas composition of the marine troposphere

A modeling study of the effects of clouds and wet removal on the chemistry of the remote marine troposphere is described. Using a time-dependent model with parameterized vertical transport to calculate trace-gas concentrations, it is found that large variations in key species (e.g., HNO3, H2CO, and H2O2) result from simulations of sporadic rainfall, changes in cloud cover, and external inputs such as surface NO sources. Depending on the frequency and intensity of an event, the effects of these perturbations may persist for several days, thereby invalidating assumptions of photochemical equilibrium in the interpretation of measurements. Long-term integrations with fixed boundary conditions and regularly occurring cloud and rain episodes demonstrate a strong sensitivity of the mean concentration of longer-lived soluble gases to precipitation frequency but also confirm the validity of using properly chosen parameterizations of wet removal in steady state calculations.

Thompson, A. M.↗

Model Analysis of Tropospheric Aerosol Variability and Sources over the North Atlantic During NAAMES 2015-2016

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES; http://naames.larc.nasa.gov) is a five year NASA 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, with the 1st field deployment in November 2015 and the 2nd in May 2016.

Liu, Hongyu↗

Clouds, Aerosol, and Precipitation in the Marine Boundary Layer: An ARM Mobile Facility Deployment

Capsule: A 21-month deployment to Graciosa Island in the northeastern Atlantic Ocean is providing an unprecedented record of the clouds, aerosols and meteorology in a poorly-sampled remote marine environment The Clouds, Aerosol, and Precipitation in the Marine Boundary Layer (CAP-MBL) deployment at Graciosa Island in the Azores generated a 21 month (April 2009- December 2010) comprehensive dataset documenting clouds, aerosols and precipitation using the Atmospheric Radiation Measurement (ARM) Mobile Facility (AMF). The scientific aim of the deployment is to gain improved understanding of the interactions of clouds, aerosols and precipitation in the marine boundary layer. Graciosa Island straddles the boundary between the subtropics and midlatitudes in the Northeast Atlantic Ocean, and consequently experiences a great diversity of meteorological and cloudiness conditions. Low clouds are the dominant cloud type, with stratocumulus and cumulus occurring regularly. Approximately half of all clouds contained precipitation detectable as radar echoes below the cloud base. Radar and satellite observations show that clouds with tops from 1- 11 km contribute more or less equally to surface-measured precipitation at Graciosa. A wide range of aerosol conditions was sampled during the deployment consistent with the diversity of sources as indicated by back trajectory analysis. Preliminary findings suggest important two-way interactions between aerosols and clouds at Graciosa, with aerosols affecting light precipitation and cloud radiative properties while being controlled in part by precipitation scavenging. The data from at Graciosa are being compared with short-range forecasts made a variety of models. A pilot analysis with two climate and two weather forecast models shows that they reproduce the observed time-varying vertical structure of lower-tropospheric cloud fairly well, but the cloud-nucleating aerosol concentrations less well. The Graciosa site has been chosen to be a permanent fixed ARM site that became operational in October 2013.

aerosols↗