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Bates, Timothy S.

Publications and source records attributed to Bates, Timothy S..

9 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2019

The North Atlantic Aerosol and Marine Ecosystem Study (NAAMES): Science Motive and Mission Overview

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is an interdisciplinary investigation to improve understanding of Earth's ocean ecosystem-aerosol-cloud system. Specific overarching science objectives for NAAMES are to (1) characterize plankton ecosystem properties during primary phases of the annual cycle and their dependence on environmental forcings, (2)determine how these phases interact to recreate each year the conditions for an annual plankton bloom, and (3) resolve how remote marine aerosols and boundary layer clouds are influenced by plankton ecosystems. Four NAAMES field campaigns were conducted in the western subarctic Atlantic between November 2015 and April 2018, with each campaign targeting specific seasonal events in the annual plankton cycle. A broad diversity of measurements were collected during each campaign, including ship, aircraft, autonomous float and drifter, and satellite observations. Here, we present an overview of NAAMES science motives, experimental design, and measurements. We then briefly describe conditions and accomplishments during each of the four field campaigns and provide information on how to access NAAMES data. The intent of this manuscript is to familiarize the broad scientific community with NAAMES and to provide a common reference overview of the project for upcoming publications.

Behrenfeld, Michael J.↗
NASA NTRS2000

Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2 and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

Analyses of aerosol optical depth (AOD) and colurnmn water vapor (CWV) measurements acquired with NASA Ames Research Center's 6-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V Professor Vodyanitskiy during the 2nd Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA-14/AVHRR satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering mearured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from radiosonde measurements during 8 soundings on 7 days and also with values calculated from measurements taken on 10 July with the AATS-14 and the University of Washington Passive Humidigraph aboard the Pelican.

Livingston, John M.↗
NASA NTRS2000

Shipboard Sunphotometer Measurements of Aerosol Optical Depth Spectra and Columnar Water Vapor During ACE-2, and Comparison with Selected Land, Ship, Aircraft, and Satellite Measurements

Analyses of aerosol optical depth (AOD) and columnar water vapor (CWV) measurements acquired with NASA Ames Research Center's six-channel Airborne Tracking Sunphotometer (AATS-6) operated aboard the R/V (research vehicle) Professor Vodyanitskiy during the second Aerosol Characterization Experiment (ACE-2) are discussed. Data are compared with various in situ and remote measurements for selected cases. The focus is on 10 July, when the Pelican airplane flew within 70 km of the ship near the time of a NOAA (National Oceanographic and Atmospheric Administration)-14/AVHRR (Advanced Very High Resolution Radiometer) satellite overpass and AOD measurements with the 14-channel Ames Airborne Tracking Sunphotometer (AATS-14) above the marine boundary layer (MBL) permitted calculation of AOD within the MBL from the AATS-6 measurements. A detailed column closure test is performed for MBL AOD on 10 July by comparing the AATS-6 MBL AODs with corresponding values calculated by combining shipboard particle size distribution measurements with models of hygroscopic growth and radiosonde humidity profiles (plus assumptions on the vertical profile of the dry particle size distribution and composition). Large differences (30-80% in the mid-visible) between measured and reconstructed AODs are obtained, in large part because of the high sensitivity of the closure methodology to hygroscopic growth models, which vary considerably and have not been validated over the necessary range of particle size/composition distributions. The wavelength dependence of AATS-6 AODs is compared with the corresponding dependence of aerosol extinction calculated from shipboard measurements of aerosol size distribution and of total scattering measured by a shipboard integrating nephelometer for several days. Results are highly variable, illustrating further the great difficulty of deriving column values from point measurements. AATS-6 CWV values are shown to agree well with corresponding values derived from radiosonde measurements during eight soundings on seven days and also with values calculated from measurements taken on 10 July with the AATS-14 and the University of Washington Passive Humidigraph aboard the Pelican.

Livingston, John M.↗
NASA NTRS1993

Atmospheric measurements of carbonyl sulfide, dimethyl sulfide, and carbon disulfide using the electron capture sulfur detector

Measurements of atmospheric dimethyl sulfide (DMS), carbonyl sulfide (COS), and carbon disulfide (CS2) were conducted over the Atlantic Ocean on board the NASA Electra aircraft during the Chemical Instrumentation Test and Evaluation (CITE 3) project using the electron capture sulfur detector (ECD-S). The system employed cryogenic preconcentration of air samples, gas chromatographic separation, catalytic fluorination, and electron capture detection. Samples collected for DMS analysis were scrubbed of oxidants with NaOH impregnated glass fiber filters to preconcentration. The detection limits (DL) of the system for COS, DMS, and CS2 were 5, 5, and 2 ppt, respectively. COS concentrations ranged from 404 to 603 ppt with a mean of 489 ppt for measurements over the North Atlantic Ocean (31 deg N to 41 deg N), and from 395 to 437 ppt with a mean of 419 ppt for measurements over the Tropical Atlantic Ocean (11 deg S to 2 deg N). DMS concentrations in the lower marine boundary layer, below 600-m altitude, ranged from below DL to 150 ppt from flights over the North Atlantic, and from 9 to 104 ppt over the Tropical Atlantic. CS2 concentrations ranged from below DL to 29 ppt over the North Atlantic. Almost all CS2 measurements over the Tropical Atlantic were below DL.

Johnson, James E.↗
NASA NTRS1993

Measurements of atmospheric carbonyl sulfide during the NASA Chemical Instrumentation Test and Evaluation Project: Implications for the global COS budget

Atmospheric carbonyl sulfide COS concentrations were measured by three analytical systems during the Chemical Instrumentation Test and Evaluation (CITE 3) project. The three systems all used cryogenic sample preconcentration and gas chromatographic (GC) separation but differed in the method of detection. The FPD system used a flame photometric detector, the MS system used a mass selective detector, and the ECD-S system used a fluorinating catalyst followed by an electron capture detector. With the FPD system, we found a mean COS concentration of 510 ppt over the North Atlantic and 442 ppt over the Tropical Atlantic. With the ECD-S system, we found a mean COS concentration of 489 ppt over the North Atlantic and 419 ppt over the Tropical Atlantic. All three systems registered a latitudinal gradient in atmospheric COS of between 1.6 and 2.0 ppt per degree of latitude, with increasing COS concentrations northward which was similar to the gradient measured by Bingemer et al. (1990). It is difficult to reconcile the measured latitudinal concentration gradient with present theories of the global COS budget since the largest sink of COS is thought to be a flux to land plants, most of which are in the northern hemisphere.

Johnson, James E.↗
NASA NTRS1992

Variations in the methanesulfonate to sulfate molar ratio in submicrometer marine aerosol particles over the south Pacific Ocean

Seawater concentrations of dimethylsulfide (DMS) and atmospheric concentrations of DMS, sulfur dioxide, methanesulfonate (MSA), and non-sea-salt (nss) sulfate were measured over the eastern Pacific Ocean between 105 deg and 110 deg W from 20 deg N to 60 deg S during February and March 1989. Although the samples collected in the Southern Hemisphere appear to be of marine origin, no significant correlation was found between the latitudinal distributions of DMS, SO2, MSA, and nss SO4(2-). However, an inverse correlation was found between atmospheric temperature and the MSA to nss SO4(2-) molar ratio in submicrometer aerosol particles with a decrease in temperature corresponding to an increase in the molar ratio. Although this trend is consistent with laboratory results indicating the favored production of MSA at lower temperatures, it is contrary to Southern Hemisphere baseline station data. This suggests either a decrease in the supply of DMS relative to nonmarine sources of nss SO4(2-) at the baseline stations in winter or additional mechanisms that affect the relative production of MSA and nss SO4(2-).

Bates, Timothy S.↗
NASA NTRS1991

Sulfur isotope measurements of submicrometer sulfate aerosol particles over the Pacific Ocean

Stable isotopes were used to analyze the submicron-size sulfate aerosol particles in the atmosphere over the Pacific Ocean, together with the air-mass back trajectories, in order to test the hypothesis of Charlson et al. (1987) who suggested that, over the remote ocean areas, the primary source of atmospheric nonseasalt (NSS) sulfate is marine emissions of dimethylsulfide (DMS). The observed results of isotopic fractionation between the seawater sulfate and NSS sulfate fractions was found to be consistent with the isotopic fractionation predicted for the transformation of the seawater sulfate to the atmospheric NSS sulfate via a DMS path way, supporting the hypothesis of Charlson et al.

Calhoun, Julie A.↗