Search NASA⌕ Search

SEARCH · Search NASA

Results for “hydroxyl radicals”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 343 records · Page 19

Design Solutions for the Treatment of DMSD in the ISS Water Recovery System

Dimethylsilanediol (DMSD) has been identified as a problematic organic on ISS. This contaminant was initially identified in the Water Processor Assembly (WPA) product water in 2010 by the Total Organic Carbon Analyzer (TOCA). DMSD is not a crew health hazard at the levels observed in the product water, but it may degrade the performance of the Oxygen Generation System (OGS) which uses the WPA product water for electrolysis and does impact the effective operation of the WPA catalytic reactor. To mitigate these impacts, early replacement of the Multifiltration Beds in the WPA is required. An investigation has determined that the decomposition of atmospheric polydimethylsiloxanes (PDMSs) is the primary source of DMSD in the condensate. PDMSs are prevalent on ISS from a variety of sources, including crew hygiene products, adhesives, caulks, lubricants, and various nonmetallics. These PDMSs also contribute to degradation of the CHX hydrophilic coating, rendering it hydrophobic and therefore affecting its ability to transmit water to the condensate bus. In addition, literature research has determined that PDMSs are likely oxidized to DMSD in the atmosphere when exposed to hydroxyl radicals in the ISS atmosphere. To address these mechanisms, filters have been developed for removal of PDMSs from the ISS atmosphere. However, ongoing analysis indicates a significant reduction in atmospheric PDMSs is required to achieve a measurable reduction of DMSD in the condensate. As a result, additional measures are being pursued to mitigate this issue. First, credible sources are being investigated to quantity to the extent possible the significant sources of PDMSs and identify sources that can be reasonably removed from ISS. Second, a Reverse Osmosis technology is being investigated as an alternate means for removing DMSD from the condensate. This paper summarizes the current status of the overall effort to mitigate DMSD in the US condensate.

Perry, Jay↗

Lightning NOx Estimates from Space-Based Lightning Imagers

The intense heating of air by a lightning channel, and subsequent rapid cooling, leads to the production of lightning nitrogen oxides (NOx = NO + NO2) as discussed in Chameides [1979]. In turn, the lightning nitrogen oxides (or "LNOx" for brevity) indirectly influences the Earth's climate because the LNOx molecules are important in controlling the concentration of ozone (O3) and hydroxyl radicals (OH) in the atmosphere. Climate is most sensitive to O3 in the upper troposphere, and LNOx is the most important source of NOx in the upper troposphere at tropical and subtropical latitudes; hence, lightning is a useful parameter to monitor for climate assessments. The National Climate Assessment (NCA) program was created in response to the Congressionally-mandated Global Change Research Act (GCRA) of 1990. Thirteen US government organizations participate in the NCA program which examines the effects of global change on the natural environment, human health and welfare, energy production and use, land and water resources, human social systems, transportation, agriculture, and biological diversity. The NCA focuses on natural and human-induced trends in global change, and projects major trends 25 to 100 years out. In support of the NCA, the NASA Marshall Space Flight Center (MSFC) continues to assess lightning-climate inter-relationships. This activity applies a variety of NASA assets to monitor in detail the changes in both the characteristics of ground- and space- based lightning observations as they pertain to changes in climate. In particular, changes in lightning characteristics over the conterminous US (CONUS) continue to be examined by this author using data from the Tropical Rainfall Measuring Mission Lightning Imaging Sensor. In this study, preliminary estimates of LNOx trends derived from TRMM/LIS lightning optical energy observations in the 17 yr period 1998-2014 are provided. This represents an important first step in testing the ability to make remote retrievals of LNOx from a satellite-based lightning sensor. As is shown, the methodology can also be directly applied to more recently launched lightning mappers, such as the Geostationary Lightning Mapper, and the International Space Station LIS.

Koshak, William J.↗

Deriving Global OH Abundance and Atmospheric Lifetimes for Long-Lived Gases: A Search for CH3CCl3 Alternatives

An accurate estimate of global hydroxyl radical (OH) abundance is important for projections of air quality, climate, and stratospheric ozone recovery. As the atmospheric mixing ratios of methyl chloroform (CH3CCl3) (MCF), the commonly used OH reference gas, approaches zero, it is important to find alternative approaches to infer atmospheric OH abundance and variability. The lack of global bottom-up emission inventories is the primary obstacle in choosing a MCF alternative. We illustrate that global emissions of long-lived trace gases can be inferred from their observed mixing ratio differences between the Northern Hemisphere (NH) and Southern Hemisphere (SH), given realistic estimates of their NH-SH exchange time, the emission partitioning between the two hemispheres, and the NH versus SH OH abundance ratio. Using the observed long-term trend and emissions derived from the measured hemispheric gradient, the combination of HFC-32 (CH2F2), HFC-134a (CH2FCF3, HFC-152a (CH3CHF2), and HCFC-22 (CHClF2), instead of a single gas, will be useful as a MCF alternative to infer global and hemispheric OH abundance and trace gas lifetimes. The primary assumption on which this multispecies approach relies is that the OH lifetimes can be estimated by scaling the thermal reaction rates of a reference gas at 272 K on global and hemispheric scales. Thus, the derived hemispheric and global OH estimates are forced to reconcile the observed trends and gradient for all four compounds simultaneously. However, currently, observations of these gases from the surface networks do not provide more accurate OH abundance estimate than that from MCF.

Lifetime↗

Three Decades of Global Methane Sources and Sinks

Methane is an important greenhouse gas, responsible for about 20 of the warming induced by long-lived greenhouse gases since pre-industrial times. By reacting with hydroxyl radicals, methane reduces the oxidizing capacity of the atmosphere and generates ozone in the troposphere. Although most sources and sinks of methane have been identified, their relative contributions to atmospheric methane levels are highly uncertain. As such, the factors responsible for the observed stabilization of atmospheric methane levels in the early 2000s, and the renewed rise after 2006, remain unclear. Here, we construct decadal budgets for methane sources and sinks between 1980 and 2010, using a combination of atmospheric measurements and results from chemical transport models, ecosystem models, climate chemistry models and inventories of anthropogenic emissions. The resultant budgets suggest that data-driven approaches and ecosystem models overestimate total natural emissions. We build three contrasting emission scenarios which differ in fossil fuel and microbial emissions to explain the decadal variability in atmospheric methane levels detected, here and in previous studies, since 1985. Although uncertainties in emission trends do not allow definitive conclusions to be drawn, we show that the observed stabilization of methane levels between 1999 and 2006 can potentially be explained by decreasing-to-stable fossil fuel emissions, combined with stable-to-increasing microbial emissions. We show that a rise in natural wetland emissions and fossil fuel emissions probably accounts for the renewed increase in global methane levels after 2006, although the relative contribution of these two sources remains uncertain.

periodic variations↗

Radiolysis of Macromolecular Organic Material in Mars-Relevant Mineral Matrices

The fate of organic material on Mars after deposition is crucial to interpreting the source of these molecules. Previous work has addressed how various organic compounds at millimeter depths in sediments respond to ultraviolet radiation. In contrast, this study addressed how high‐energy particle radiation (200‐MeV protons, simulating the effect of galactic cosmic rays and solar wind at depths of <4–5 cm) influences organic macromolecules in sediments. Specifically, we report the generation of organic‐acid radiolysis products after exposure to radiation doses equivalent to geological time scales (1–7 Myr). We found that formate and oxalate were produced from a variety of organic starting materials and mineral matrices. Unlike ultraviolet‐driven reactions that can invoke Fenton chemistry to produce organic acids, our work suggests that irradiation of semiconductor surfaces, such as TiO2 or possible clay minerals found on Mars, forms oxygen and hydroxyl radical species, which can break down macromolecules into organic acids. We also investigated the metastability of benzoate in multiple mineral matrices. Benzoate was added to samples prior to irradiation and persisted up to 500 kGys of exposure. Our findings suggest that organic acids are likely a major component of organic material buried at depth on Mars.

Fox, A. C.↗

Constraining Remote Oxidation Capacity with ATom Observations

The global oxidation capacity, defined as the tropospheric mean concentration of the hydroxyl radical (OH), controls the lifetime of reactive trace gases in the atmosphere such as methane and carbon monoxide (CO). Models tend to underestimate the methane lifetime and CO concentrations throughout the troposphere, which is consistent with excessive OH. Approximately half the oxidation of methane and non-methane volatile organic compounds (VOCs) is thought to occur over the oceans where oxidant chemistry has received little validation due to a lack of observational constraints. We use observations from the first two deployments of the NASA ATom aircraft campaign during July–August 2016 and January–February 2017 to evaluate the oxidation capacity over the remote oceans and its representation in the GEOS-Chem chemical transport model. The model successfully simulates the magnitude and vertical profile of remote OH within the measurement uncertainties. Comparisons against the drivers of OH production (water vapor, ozone, and NOy concentrations, ozone photolysis frequencies) also show minimal bias with the exception of wintertime NOy, for which a model overestimate may indicate insufficient wet scavenging and/or missing loss on seasalt aerosol but large uncertainties remain that require further studies of NOy partitioning and removal in the troposphere. During the ATom-1 deployment, OH reactivity (OHR) below 3 km is significantly enhanced, and this is not captured by the sum of its measured components (cOHRobs) or by the model (cOHRmod). This enhancement could suggest missing reactive VOCs but cannot be explained by new estimates of ocean VOC sources and additional modeled reactivity in this region would be difficult to reconcile with the full suite of ATom measurement constraints. The model generally reproduces the magnitude and seasonality of cOHRobs but underestimates the contribution of oxygenated VOC, mainly acetaldehyde, which is severely underestimated throughout the troposphere despite its calculated lifetime of less than a day. Missing model acetaldehyde in previous studies was attributed to measurement uncertainties that have been largely resolved. Observations of peroxyacetic acid (PAA) provide new support for remote levels of acetaldehyde. The underestimate in modeled acetaldehyde and PAA is present throughout the year in both hemispheres and peaks during Northern Hemisphere summer. The addition of ocean VOC sources in the model increases annual surface cOHRmod by 10 % and improves model-measurement agreement for acetaldehyde particularly in winter but cannot resolve the model summertime bias. Doing so would require a 100 Tg yr−1 source of a long-lived unknown precursor throughout the year with significant additional emissions in the Northern Hemisphere summer. Improving the model bias for remote acetaldehyde and PAA is unlikely to fully resolve previously reported model global biases in OH and methane lifetime, suggesting that future work should examine the sources and sinks of OH over land.

Travis, Katherine R.↗

The Global Methane Budget 2000–2017

Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. Atmospheric emissions and concentrations of CH4 continue to increase, making CH4 the second most important human-influenced greenhouse gas in terms of climate forcing, after carbon dioxide (CO2). The relative importance of CH4 compared to CO2 depends on its shorter atmospheric lifetime, stronger warming potential, and variations in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in reducing uncertainties in the atmospheric growth rate arise from the variety of geographically overlapping CH4 sources and from the destruction of CH4 by short-lived hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. Following Saunois et al. (2016), we present here the second version of the living review paper dedicated to the decadal methane budget, integrating results of top-down studies (atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up estimates (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). For the 2008–2017 decade, global methane emissions are estimated by atmospheric inversions (a top-down approach) to be 576 Tg CH4/yr (range 550–594, corresponding to the minimum and maximum estimates of the model ensemble). Of this total, 359 Tg CH4/yr or ∼ 60 % is attributed to anthropogenic sources, that is emissions caused by direct human activity (i.e. anthropogenic emissions; range 336–376 Tg CH4/yr or 50 %–65 %). The mean annual total emission for the new decade (2008–2017) is 29 Tg CH4/yr larger than our estimate for the previous decade (2000–2009), and 24 Tg CH4/yr larger than the one reported in the previous budget for 2003–2012 (Saunois et al., 2016). Since 2012, global CH4 emissions have been tracking the warmest scenarios assessed by the Intergovernmental Panel on Climate Change. Bottom-up methods suggest almost 30 % larger global emissions (737 Tg CH4/yr, range 594–881) than top-down inversion methods. Indeed, bottom-up estimates for natural sources such as natural wetlands, other inland water systems, and geological sources are higher than top-down estimates. The atmospheric constraints on the top-down budget suggest that at least some of these bottom-up emissions are overestimated. The latitudinal distribution of atmospheric observation-based emissions indicates a predominance of tropical emissions (∼ 65 % of the global budget, < 30° N) compared to mid-latitudes (∼ 30 %, 30–60° N) and high northern latitudes (∼ 4 %, 60–90° N). The most important source of uncertainty in the methane budget is attributable to natural emissions, especially those from wetlands and other inland waters. Some of our global source estimates are smaller than those in previously published budgets (Saunois et al., 2016; Kirschke et al., 2013). In particular wetland emissions are about 35 Tg CH4/yr lower due to improved partition wetlands and other inland waters. Emissions from geological sources and wild animals are also found to be smaller by 7 Tg CH4/yr by 8 Tg CH4/yr, respectively. However, the overall discrepancy between bottom-up and top-down estimates has been reduced by only 5 % compared to Saunois et al. (2016), due to a higher estimate of emissions from inland waters, highlighting the need for more detailed research on emissions factors. Priorities for improving the methane budget include (i) a global, high-resolution map of water-saturated soils and inundated areas emitting methane based on a robust classification of different types of emitting habitats; (ii) further development of process-based models for inland-water emissions; (iii) intensification of methane observations at local scales (e.g., FLUXNET-CH4 measurements) and urban-scale monitoring to constrain bottom-up land surface models, and at regional scales (surface networks and satellites) to constrain atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) development of a 3D variational inversion system using isotopic and/or co-emitted species such as ethane to improve source partitioning.

methane budget↗

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)↗

Improved Constraints on Global Methane Emissions and Sinks Using δ13C-CH4

We study the drivers behind the global atmospheric methane (CH4) increase observed after 2006. Candidate emission and sink scenarios are constructed based on proposed hypotheses in the literature. These scenarios are simulated in the TM5 tracer transport model for 1984–2016 to produce three-dimensional fields of CH4 and δ13C-CH4, which are compared with observations to test the competing hypotheses in the literature in one common model framework. We find that the fossil fuel (FF) CH4 emission trend from the Emissions Database for Global Atmospheric Research 4.3.2 inventory does not agree with observed δ13C-CH4. Increased FF CH4 emissions are unlikely to be the dominant driver for the post-2006 global CH4 increase despite the possibility for a small FF emission increase. We also find that a significant decrease in the abundance of hydroxyl radicals (OH) cannot explain the post-2006 global CH4 increase since it does not track the observed decrease in global mean δ13C-CH4. Different CH4 sinks have different fractionation factors for δ13C-CH4, thus we can investigate the uncertainty introduced by the reaction of CH4 with tropospheric chlorine (Cl), a CH4 sink whose abundance, spatial distribution, and temporal changes remain uncertain. Our results show that including or excluding tropospheric Cl as a 13 Tg/year CH4 sink in our model changes the magnitude of estimated fossil emissions by ∼20%. We also found that by using different wetland emissions based on a static versus a dynamic wetland area map, the partitioning between FF and microbial sources differs by 20 Tg/year, ∼12% of estimated fossil emissions.

X. Lan↗

10-kHz PLIF Thermometry for a Turbulent Jet Flame using Single Burst-mode OPO

Two-color Planar laser-induced fluorescence (TC-PLIF) thermometry techniques that employ two laser systems and two cameras face challenges when implemented in practical combustion facilities because of experimental complexity and multiple laser and camera requirements, particularly for high-speed TC-PLIF. To circumvent those problems, we developed a fast, dual-wavelength switching, burst-mode OPO technology to significantly reduce the experimental complexity of high-speed TC-PLIF thermometry and simplify its implementation in harsh combustion and flow test facilities. A fast, dual-wavelength switched seed laser enabled a high-energy, high-repetition-rate burst-mode laser to generate two 10-kHz pulse trains at wavelengths of ~354.8 nm. The injection-seeded OPO efficiently converts the burst-mode laser output to285.62 nm and 285.67 nm to excite the Q2(12) and P1(8) OH transitions. PLIF images were collected from each of the two excitation transitions with a single camera and an UV intensifier, and intensity ratios from the images were used to determine local temperatures. Ten kHz hydroxyl radical (OH) TC-PLIF for premixedCH4/Air/H2 jet flame was demonstrated.

thermometry↗

10-kHz PLIF Thermometry for Turbulent Jet Flame using Single Burst-mode OPO

Two-color Planar Laser-Induced Fluorescence (TC-PLIF) thermometry techniques that employ two laser systems and two cameras face challenges when implemented in practical combustion facilities because of experimental complexity and multiple laser and camera requirements, particularly for high-speed TC-PLIF. To circumvent those problems, we developed a fast, dual-wavelength switching, burst-mode OPO technology to significantly reduce the experimental complexity of high-speed TC-PLIF thermometry and simplify its implementation in harsh combustion and flow test facilities. A fast, dual-wavelength switched seed laser enabled a high-energy, high-repetition-rate burst-mode laser to generate two 10-kHz pulse trains at wavelengths of ~354.8 nm. The injection-seeded OPO efficiently converts the burst-mode laser output to 285.62 nm and 285.67 nm to excite the Q2(12) andP1(8) OH transitions. PLIF images were collected from each of the two excitation transitions with a single camera and an UV intensifier, and intensity ratios from the images were used to determine local temperatures. Ten kHz hydroxyl radical (OH) TC-PLIF for premixedCH4/Air/H2 jet flame was demonstrated.

thermometry↗

First Observations of Mesospheric OH Emission Profiles from OMPS/LP

The hydroxyl radical (OH) is one of the most reactive trace species and plays several important roles in the photochemical equilibrium and energy balance in the mesosphere. Global observations of OH from satellite instruments have a role to play in the study of OH and water vapor variations. This study describes an advanced algorithm to detect mesospheric OH emission profiles from the Suomi NPP satellite Ozone Mapping and Profiler Suite Limb Profiler (OMPS/LP). A triplet technique has been adapted to the OMPS/LP radiance measurements for determining OH emission signatures and OH index (OHI) from the OH A2Σ+-X2Π 0-0 band near the 308.8-nm wavelength. The derived mesospheric profiles provide an overall picture of the vertical distribution of OHI between 55 and 84 km and seasonal and latitudinal variability of the strength and height of the OHI. The observed annual cycle is correlated with the water vapor cycle and anticorrelated with the mesospheric temperature cycle. The data show that the relationships persist during the period of April 2012–December 2020. The seasonal behavior of OHI may be associated with variations in solar illumination or mesospheric water vapor abundance. The influence of solar illumination is dominant in the midlatitudes, while the OHI pattern is dominated by water vapor photolysis and other influences in the tropics.

Observations of Mesospheric OH Emission↗

Global Burden of Tropospheric Ozone: Effects of Particulate Nitrate Photolysis and Assimilation of NO2 Measurements

Tropospheric ozone is a major pollutant, a greenhouse gas, and the primary source of the hydroxyl radical. It is largely produced in situ from the oxidation of CO and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2). Global atmospheric chemistry models generally underestimate NOx and CO concentrations in the northern hemisphere away from source regions, which would lead to an underestimate in the tropospheric ozone burden. Here we evaluate the tropospheric ozone simulation in the GEOS-Chem model (version 14) using observations from satellite, aircraft, and ozonesondes. We include GEOS-Chem simulations conducted in the standard offline mode, as well as in the online mode within the NASA GEOS earth system model which forms the basis for the GEOS Composition Forecasts (GEOS-CF). In both configurations, GEOS-Chem underestimates ozone concentrations in the northern midlatitude free troposphere in spring and summer. We find that we can improve the ozone simulation by including an additional NOx source over the oceans from particulate nitrate photolysis on sea salt aerosols at rates inferred from field studies over the Atlantic Ocean. We investigate whether further improvements in the ozone simulation can be achieved by assimilating satellite measurements of NO2 from the Ozone Monitoring Instrument (OMI) and CO from the Measurement of Pollution in the Troposphere (MOPITT) instruments.

tropospheric ozone↗

Impact of Stress-Activated Positive Holes on the Redox Timing in Organisms Living at the Surface of Rocks: Unlocking Nature's Secrets

Squeezing and deforming igneous and/or high-grade metamorphic rocks activates electronic charge carriers known as positive holes, h•, that are defect electrons in the O2– sublattice. Similar to h• in semiconductors the h• in rocks affect electrical and thermal properties. They produce electrochemical reactions, localized electrical signals, and currents. In this study, we explore the effects of positive holes on the electron flow in the electron transport chain (ETC) of organisms living at the surface of rocks such as gabbro or granite. We found that positive holes, h•, disrupt the temporal coordination in vivo governed by oscillating reduction-oxidation reactions, known as the redox cycle. Positive holes affect the timing of the redox cycle by interacting with molecules in vivo, leading to the formation of superoxide anions and hydroxyl radicals. Thus, we observed that positive holes significantly impede the growth of yeast Saccharomyces cerevisiae (i.e., colony size) and delay the sprouting of broccoli and chia seeds. Additionally, positive holes were found to exert discernible impacts on plant development such as stem length and leaf size. Our findings highlight the intricate interplay between positive holes, redox timing, and biological processes, shedding light on the potentially significant role of positive holes in influencing the growth and development of organisms in tectonically stressed rock environments. Understanding these effects has implications for a broader understanding of redox biology and of how environmental factors can influence cellular development in natural settings.

Redox Timing in Organisms↗

Tropospheric Ozone in the NASA GEOS Model: Effects of Satellite NO2 Data Assimilation and Improvements in Background NOx Chemistry

Tropospheric ozone is a major atmospheric oxidant, the primary source of the hydroxyl radical, and a greenhouse gas. In the troposphere, it is produced from the oxidation of carbon monoxide and volatile organic compounds in the presence of nitrogen oxides (NOx=NO+NO2) or has its origins in the stratosphere. The tropospheric ozone burdens in global atmospheric chemistry models disagree by a factor of 1.5, indicating an incomplete understanding of ozone sources and sinks. Here we examine the tropospheric ozone simulation in NASA Global Modeling and Assimilation Office’s (GMAO’s) GEOS model with the GEOS-Chem chemistry mechanism (version 14.2), using observations from satellites, aircraft, ozonesondes, and surface sites. This modeling framework is used to produce GMAO’s GEOS Composition Forecasts (GEOS-CF), and it has been updated extensively with new emission inventories, improved model physics, satellite data assimilation capability, and an up-to-date chemical mechanism that includes tropospheric halogen chemistry and NOx recycling from particulate nitrate. Earlier versions of the model using GEOS-Chem version 12.0 showed an underestimate in tropospheric ozone in the northern hemisphere. We evaluate the ozone simulation in the updated model, focusing on the effects of assimilating satellite NO2 data from the Ozone Monitoring Instrument (OMI), constraining stratospheric ozone to satellite data, and updates to the NOx chemistry. We will examine changes in the vertical profiles of tropospheric ozone over the US in support of the Tropospheric Emissions: Monitoring of Pollution (TEMPO), and discuss implications for the tropospheric ozone budget.

V. Shah↗

GOES-16 GLM Observations for National Climate Assessments

The heating of air by a lightning discharge, followed by rapid cooling, leads to the production of lightning nitrogen oxides (“LNO x ” for brevity, where NO x = NO + NO 2 ). The LNO x are important trace gases because they control the concentration of the greenhouse gas ozone (O 3 ) and the highly reactive hydroxyl radicals (OH). In fact, LNO x are the most important source of NO x in the upper troposphere at tropical and subtropical latitudes, and climate is most sensitive to O 3 in the upper troposphere. Since lightning indirectly influences the Earth's climate, it is a key variable to monitor in National Climate Assessment (NCA) studies. In this work, GOES-16 Geostationary Lightning Mapper (GLM) flash counts and flash optical properties (i.e., optical energy, optical area, …) that are linked to LNO x production are examined in detail for the continental United States analysis region, and are compared with ground-based National Lightning Detection Network (NLDN) observations.

Lightning↗

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↗

Enhancing Long-Term Trend Simulation of OH Through the Synergy of Model Simulations and Aura Ozone Monitoring Instrument (OMI) NO 2 and HCHO Retrievals

During the last few years, tremendous progress has been made to develop an efficient parameterization module using agile machine learning techniques. The aim of this module is to provide dynamic response of the tropospheric hydroxyl radical (OH) to its major drivers, including trace gases, aerosols, clouds, and meteorology. This module, named ECCOH (pronounced “echo”) and implemented in NASA’s GEOS-5 global model, offers an unrealized opportunity to unravel the convoluted response of OH to its underlying drivers while approaching the accuracy of full-chemistry without incurring excessive computational costs, making it suitable for climate models. However, the accurate representation of OH in ECCOH poses challenges due to the lack of representation of some of its critical inputs such as the abundance of NO 2 and HCHO concentrations. As such, we leverage the well-characterized satellite observations of NO2 and HCHO columns from Aura OMI to enhance their representation in ECCOH using an optimal interpolation method for the time period of 2005 - present. We show how the inclusion of OMI information can affect the spatiotemporal variability and long-term trends of OH, CO, and CH 4 across the globe. Additionally, we underscore the necessity of obtaining high-fidelity information regarding tropospheric ozone from the southern hemisphere from space, a region currently lacking full verification in models, posing a challenge to get a reasonable amount of chemical sink for CH 4 .

OH↗