Search NASA⌕ Search

Engineering topics

T. Paul Bui

Publications and source records attributed to T. Paul Bui.

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↗

Missing OH Reactivity in the Global Marine Boundary Layer

The hydroxyl radical (OH) reacts with thousands of chemical species in the atmosphere, initiating their removal and the chemical reaction sequences that produce ozone, secondary aerosols, and gas-phase acids. OH reactivity, which is the inverse of OH lifetime,influences the OH abundance and the ability of OH to cleanse the atmosphere. The NASA Atmospheric Tomography (ATom) campaign used instruments on the NASA DC-8 aircraft to measure OH reactivity and more than 100 trace chemical species. ATom presented a unique opportunity to test the completeness of the OH reactivity calculated from the chemical species measurements by comparing it to the measured OH reactivity over two oceans across four seasons. Although, throughout much of the free troposphere, the calculated OH reactivity was below the limit-of-detection for the ATom instrument used to measure OH reactivity, the instrument was able to measure the OH reactivity in and just above the marine boundary layer. The mean measured value of OH reactivity in the marine boundary layer across all latitudes and all ATom deployments was 1.9 s-1, which is 0.5 s-1larger than the mean calculated OH reactivity. The missing OH reactivity, the difference between the measured and calculated OH reactivity, varied between 0 s-1to 3.5 s-1, with the highest values over the Northern Hemisphere Pacific Ocean. Correlations of missing OH reactivity with formaldehyde, dimethyl sulfide, butanal, and sea surface temperature suggest the presence of unmeasured or unknown volatile organic compounds or oxygenated volatile organic compounds associated with ocean emissions.

NASA Atmospheric Tomography (ATom)↗

Global Airborne Sampling Reveals a Previously Unobserved Dimethyl Sulfide Oxidation Mechanism in the Marine Atmosphere

Dimethyl sulfide (DMS), emitted from the oceans, is the most abundant biological source of sulfur to the marine atmosphere. Atmospheric DMS is oxidized to condensable products that form secondary aerosols that affect Earth’s radiative balance by scattering solar radiation and serving as cloud condensation nuclei. We report the atmospheric discovery of a previously unquantified DMS oxidation product, hydroperoxymethyl thioformate (HPMTF, HOOCH2SCHO), identified through global-scale airborne observations that demonstrate it to be a major reservoir of marine sulfur. Observationally constrained model results show that more than 30% of oceanic DMS emitted to the atmosphere forms HPMTF. Coincident particle measurements suggest a strong link between HPMTF concentration and new particle formation and growth. Analyses of these observations show that HPMTF chemistry must be included in atmospheric models to improve representation of key linkages between the biogeochemistry of the ocean, marine aerosol formation and growth, and their combined effects on climate.

DMS gas-phase oxidation product↗

Quantification of CO2 and CH4 emissions over Sacramento, California, based on divergence theorem using aircraft measurements

Emission estimates of carbon dioxide (CO2) and methane (CH4) and the meteorological factors affecting them are investigated over Sacramento, California, using an aircraft equipped with a cavity ring-down greenhouse gas sensor as part of the Alpha Jet Atmospheric eXperiment (AJAX) project. To better constrain the emission fluxes, we designed flights in a cylindrical pattern and computed the emission fluxes from two flights using a kriging method and Gauss’s divergence theorem. Differences in wind treatment and assumptions about background concentrations affect the emission estimates by a factor of 1.5 to 7. The uncertainty is also impacted by meteorological conditions and distance from the emission sources. The vertical layer averaging affects the flux estimate, but the choice of raw wind or mass-balanced wind is more important than the thickness of the vertical averaging for massbalanced wind for both urban and local scales. The importance of vertical mass transfer for flux estimates is examined, and the difference in the total emission estimate with and without vertical mass transfer is found to be small, especially at the local scale. The total flux estimates accounting for the entire circumference are larger than those based solely on measurements made in the downwind region. This indicates that a closed-shape flight profile can better contain total emissions relative to a one-sided curtain flight because most cities have more than one point source and wind direction can change with time and altitude. To reduce the uncertainty of the emission estimate, it is important that the sampling strategy account not only for known source locations but also possible unidentified sources around the city. Our results highlight that aircraft-based measurements using a closed-shape flight pattern are an efficient and useful strategy for identifying emission sources and estimating local- and city-scale greenhouse gas emission fluxes.

Ju-Mee Ryoo↗

Possible Role of Mixing on Water Vapor and Ozone Anomalies During RF05

We investigate the possible role of mixing on the observed variations in water vapor and ozone anomalies during DCOTSS 29 July 2021 flight. Preliminary results indicate that enhanced water vapor is more often associated with enhanced ozone, opposite of what one might expect during convective plume encounters. We use the turbulence eddy dissipation rate as a proxy of mixing to show that when water vapor is significantly enhanced (> 30 ppmv), water vapor anomalies are negatively correlated with mixing strength: strong turbulence and large mixing are associated with relatively dry air. The mechanism behind this relationship as well as the origins of the observed turbulence and mixing will be investigate in the figure.

Mixing↗