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NASA NTRS2013

NASA Tech Briefs, September 2013

Topics include: ISS Ammonia Leak Detection Through X-Ray Fluorescence; A System for Measuring the Sway of the Vehicle Assembly Building; Fast, High-Precision Readout Circuit for Detector Arrays; Victim Simulator for Victim Detection Radar; Hydrometeor Size Distribution Measurements by Imaging the Attenuation of a Laser Spot; Quasi-Linear Circuit; High-Speed, High-Resolution Time-to-Digital Conversion; Li-Ion Battery and Supercapacitor Hybrid Design for Long Extravehicular Activities; Ultrasonic Low-Friction Containment Plate for Thermal and Ultrasonic Stir Weld Processes; High-Powered, Ultrasonically Assisted Thermal Stir Welding; Next-Generation MKIII Lightweight HUT/Hatch Assembly; Centrifugal Sieve for Gravity-Level-Independent Size; Segregation of Granular Materials; Ion Exchange Technology Development in Support of the Urine Processor Assembly; Nickel-Graphite Composite Compliant Interface and/or Hot Shoe Material; UltraSail CubeSat Solar Sail Flight Experiment; Mechanism for Deploying a Long, Thin-Film Antenna From a Rover; Counterflow Regolith Heat Exchanger; Acquisition and Retaining Granular Samples via a Rotating Coring Bit; Very-Low-Cost, Rugged Vacuum System; Medicine Delivery Device With Integrated Sterilization and Detection; FRET-Aptamer Assays for Bone Marker Assessment, C-Telopeptide, Creatinine, and Vitamin D; Multimode Directional Coupler for Utilization of Harmonic Frequencies from TWTAs; Dual-Polarization, Multi-Frequency Antenna Array for use with Hurricane Imaging Radiometer; Complementary Barrier Infrared Detector (CBIRD) Contact Methods; Autonomous Control of Space Nuclear Reactors; High-Power, High-Speed Electro-Optic Pockels Cell Modulator; Covariance Analysis Tool (G-CAT) for Computing Ascent, Descent, and Landing Errors; Enigma Version 12; Micrometeoroid and Orbital Debris (MMOD) Shield Ballistic Limit Analysis Program; Spitzer Telemetry Processing System; Planetary Protection Bioburden Analysis Program; Wing Leading Edge RCC Rapid Response Damage Prediction Tool (IMPACT2); ISSM: Ice Sheet System Model; Automated Loads Analysis System (ATLAS); Integrated Main Propulsion System Performance Reconstruction Process/Models. Phoenix Telemetry Processor; Contact Graph Routing Enhancements Developed in ION for DTN; GFEChutes Lo-Fi; Advanced Strategic and Tactical Relay Request Management for the Mars Relay Operations Service; Software for Generating Troposphere Corrections for InSAR Using GPS and Weather Model Data; Ionospheric Specifications for SAR Interferometry (ISSI); Implementation of a Wavefront-Sensing Algorithm; Sally Ride EarthKAM - Automated Image Geo-Referencing Using Google Earth Web Plug-In; Trade Space Specification Tool (TSST) for Rapid Mission Architecture (Version 1.2); Acoustic Emission Analysis Applet (AEAA) Software; Memory-Efficient Onboard Rock Segmentation; Advanced Multimission Operations System (ATMO); Robot Sequencing and Visualization Program (RSVP); Automating Hyperspectral Data for Rapid Response in Volcanic Emergencies; Raster-Based Approach to Solar Pressure Modeling; Space Images for NASA JPL Android Version; Kinect Engineering with Learning (KEWL); Spacecraft 3D Augmented Reality Mobile App; MPST Software: grl_pef_check; Real-Time Multimission Event Notification System for Mars Relay; SIM_EXPLORE: Software for Directed Exploration of Complex Systems; Mobile Timekeeping Application Built on Reverse-Engineered JPL Infrastructure; Advanced Query and Data Mining Capabilities for MaROS; Jettison Engineering Trajectory Tool; MPST Software: grl_suppdoc; PredGuid+A: Orion Entry Guidance Modified for Aerocapture; Planning Coverage Campaigns for Mission Design and Analysis: CLASP for DESDynl; and Space Place Prime.

Source record↗

NASA NTRS1999

Dynamical and Chemical Behavior of the Lower Stratosphere and Interactions with the Troposphere

Equivalent-barotropic calculations, in tandem with Lagrangian analyses, reveal how changes of total ozone follow from vertical and horizontal transport by planetary waves. Those calculations also throw light on how diabatic motions comprising the Brewer-Dobson circulation develop from quasi-horizontal advection by planetary waves. Potential temperature along a material surface indicates organized subsidence inside the polar-night vortex, resembling tracer observations from UARS. Lagrangian histories illustrate that this sinking motion follows in large part from parcels being driven out of thermodynamic equilibrium by planetary waves, especially at high latitudes. Irreversible heat transfer then produces a net drift of air across isentropic surfaces as parcels orbit about the displaced vortex. By driving mean-meridional overturning in the stratosphere, this downward drift is ultimately responsible for transferring ozone from the tropics to the extratropical lower stratosphere. It also introduces horizontal structure into the distribution of total ozone, which surfaces clearly in ozone trends. High-resolution global cloud imagery constructed from 6 satellites simultaneously observing the Earth was used to investigate the spectrum of equatorial waves generated by tropical convection and propagating vertically into the stratosphere. The results indicate that temperature variability is dominated by planetary-scale equatorial waves like the Kelvin mode, which agrees with satellite observations of the tropical stratosphere. However, the Kelvin mode accounts for only about 30 - 50% of the eastward momentum flux radiating into the stratosphere, the remainder coming from gravity waves. An algorithm was developed to determine 3-dimensional atmospheric motion from satellite tracer measurements. Based on Lagrangian constraints, the algorithm circumvents limitations of the traditional scheme for inferring motion from temperature measurements and determines the circulation in the tropics as reliably as elsewhere. A study of deep convection revealed that the highest towers (those penetrating into stratospheric air and controlling tropopause height and composition through convective mixing) occur in close association with the diurnal cycle of convection. Clouds colder than 220 K develop almost entirely in association with the diurnal cycle of convection over tropical landmasses and substantially in association with it even over maritime regions.

Salby, Murry L.↗

NASA NTRS2016

Planning, Implementation, and Scientific Goals of the Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) Field Missions

The Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission based at Ellington Field, Texas, during August and September 2013 employed the most comprehensive airborne payload to date to investigate atmospheric composition over North America. The NASA ER-2, DC-8, and SPEC Inc. Learjet flew 57 science flights from the surface to 20 km. The ER-2 employed seven remote sensing instruments as a satellite surrogate and eight in situ instruments. The DC-8 employed 23 in situ and five remote sensing instruments for radiation, chemistry, and microphysics. The Learjet used 11 instruments to explore cloud microphysics. SEAC4RS launched numerous balloons, augmented Aerosol RObotic NETwork, and collaborated with many existing ground measurement sites. Flights investigating convection included close coordination of all three aircraft. Coordinated DC-8 and ER-2 flights investigated the optical properties of aerosols, the influence of aerosols on clouds, and the performance of new instruments for satellite measurements of clouds and aerosols. ER-2 sorties sampled stratospheric injections of water vapor and other chemicals by local and distant convection. DC-8 flights studied seasonally evolving chemistry in the Southeastern U.S., atmospheric chemistry with lower emissions of NOx and SO2 than in previous decades, isoprene chemistry under high and low NOx conditions at different locations, organic aerosols, air pollution near Houston and in petroleum fields, smoke from wildfires in western forests and from agricultural fires in the Mississippi Valley, and the ways in which the chemistry in the boundary layer and the upper troposphere were influenced by vertical transport in convective clouds.

Toon, Owen B.↗

NASA NTRSDate not supplied

The Stratospheric Aerosol and Gas Experiment (SAGE) IV

Atmospheric composition continues to be a key Earth science focus for international space agencies and research organizations. The target constituent varies depending upon the topic area of interest such as monitoring the ozone layer and the efficacy of the Montreal Protocol, assessing the influence of volcanic eruptions and large wildfires on the atmosphere, improving our knowledge of transport processes, or evaluating the impacts of greenhouse gases on climate. Additionally, there is a growing need for measurement continuity of many trace gases both from an inability to properly assess long-term trends without it as well as the reliance of reanalyses and chemistry climate models on observational input. To this end, proper continuity requires continuous and overlapping multi-instrument data records of which spaceborne measurements are a critical component. However, most current satellite systems are well beyond their expected lifetimes, and so we look toward the future to develop the Stratospheric Aerosol and Gas Experiment (SAGE) IV as a future mission concept. Enabled by the NASA Earth Science Technology Office’s (ESTO) Instrument Incubator Program, the SAGE IV Pathfinder project developed and validated a prototype demonstration that paves the way for a future SAGE IV spaceflight mission. Utilizing solar occultation imaging, SAGE IV will be capable of measuring key species in the stratosphere and upper troposphere with the same quality as previous SAGE instruments but with greatly improved pointing knowledge and extensibility to new science targets. The precision and stability of a well-designed occultation instrument can act as a calibration reference standard for other spaceborne instruments, ensuring proper continuity of the desired science targets. Furthermore, current technological advancements allow SAGE IV to fit within a CubeSat framework and make use of commercial hardware, significantly reducing the size and cost when compared with traditional missions and enabling sustainability of future measurements.

Robert Damadeo↗

NASA NTRSDate not supplied

The Stratospheric Aerosol and Gas Experiment IV

Atmospheric composition continues to be a key Earth science focus for international space agencies and research organizations. The target constituent varies depending upon the topic area of interest such as monitoring the ozone layer and the efficacy of the Montreal Protocol, assessing the influence of volcanic eruptions and large wildfires on the atmosphere, improving our knowledge of transport processes, or evaluating the impacts of greenhouse gases on climate. Additionally, there is a growing need for measurement continuity of many trace gases both from an inability to properly assess long-term trends without it as well as the reliance of reanalyses and chemistry climate models on observational input. To this end, proper continuity requires continuous and overlapping multi-instrument data records of which spaceborne measurements are a critical component. However, most current satellite systems are well beyond their expected lifetimes, and so we look toward the future to develop the Stratospheric Aerosol and Gas Experiment (SAGE) IV as a future mission concept. Enabled by the NASA Earth Science Technology Office’s (ESTO) Instrument Incubator Program, the SAGE IV Pathfinder project has developed and validated a prototype demonstration that paves the way for a future SAGE IV spaceflight mission. Utilizing solar occultation imaging, SAGE IV will be capable of measuring key species in the stratosphere and upper troposphere with the same quality as previous SAGE instruments but with greatly improved pointing knowledge and extensibility to new science targets. Furthermore, current technological advancements allow SAGE IV to fit within a CubeSat framework and make use of commercial hardware, significantly reducing the size and cost when compared with traditional missions and enabling sustainability of future measurements.

Robert Damadeo↗

NASA NTRSDate not supplied

An Observationally-Based Determination of the Arctic Sea Ice-Cloud Feedback Since 2000: Isolating the Arctic Cloud Response to Sea Ice Loss

Arctic sea ice responds to and drives Arctic climate change. The interactions between Arctic sea ice and clouds represent a mechanism through which sea ice can drive climate change. We composite active remote sensing satellite cloud properties for ice-free, marginal ice zone (MIZ), and ice-covered surfaces during MIZ crossing events to investigate the influence of the transition from an ice-covered to an ice-free surface on low-level clouds. We demonstrate that the event-based methodology controls for large-scale meteorological factors and isolates the sea ice effect on clouds. We find larger cloud fraction and total water content below ~1.5 km over ice-free relative to ice-covered surfaces during non-summer months, indicating a low-level cloud sensitivity to Arctic sea ice decline. During summer, results show larger cloud fraction and water content over ice-free surfaces, however the differences are statistically indistinguishable. Evidence is provided that atmospheric thermodynamic profile differences cause the cloud property differences, namely that ice-free footprints are warmer, moister, have more positive surface turbulent fluxes and are less stable than their ice-covered counterparts. Ice-free and ice-covered surface cloud property differences scale with surface temperature differences such that cloud property differences are only found in the presence of a surface temperature difference. We conclude that surface temperature differences modulate the cloud response to sea ice loss through influences on surface turbulent fluxes and lower tropospheric stability. The results imply a positive non-summer sea ice-cloud feedback and that up to a 0.02 cloud fraction and 0.05 g m 3 total water content increase in fall are due to the observed sea ice decline.

Patrick C Taylor↗

NASA NTRSDate not supplied

Estimating the Arctic Cloud-Sea Ice Feedback With Observations during the EOS Period

Patrick C. Taylor↗

NASA NTRS2012

The Distribution of Snow Black Carbon observed in the Arctic and Compared to the GISS-PUCCINI Model

In this study, we evaluate the ability of the latest NASA GISS composition-climate model, GISS-E2- PUCCINI, to simulate the spatial distribution of snow BC (sBC) in the Arctic relative to present-day observations. Radiative forcing due to BC deposition onto Arctic snow and sea ice is also estimated. Two sets of model simulations are analyzed, where meteorology is linearly relaxed towards National Centers for Environmental Prediction (NCEP) and towards NASA Modern Era Reanalysis for Research and Applications (MERRA) reanalyses. Results indicate that the modeled concentrations of sBC are comparable with presentday observations in and around the Arctic Ocean, except for apparent underestimation at a few sites in the Russian Arctic. That said, the model has some biases in its simulated spatial distribution of BC deposition to the Arctic. The simulations from the two model runs are roughly equal, indicating that discrepancies between model and observations come from other sources. Underestimation of biomass burning emissions in Northern Eurasia may be the main cause of the low biases in the Russian Arctic. Comparisons of modeled aerosol BC (aBC) with long-term surface observations at Barrow, Alert, Zeppelin and Nord stations show significant underestimation in winter and spring concentrations in the Arctic (most significant in Alaska), although the simulated seasonality of aBC has been greatly improved relative to earlier model versions. This is consistent with simulated biases in vertical profiles of aBC, with underestimation in the lower and middle troposphere but overestimation in the upper troposphere and lower stratosphere, suggesting that the wet removal processes in the current model may be too weak or that vertical transport is too rapid, although the simulated BC lifetime seems reasonable. The combination of observations and modeling provides a comprehensive distribution of sBC over the Arctic. On the basis of this distribution, we estimate the decrease in snow and sea ice albedo and the resulting radiative forcing. We suggest that the albedo reduction due to BC deposition presents significant space-time variations, with highest mean reductions of 1.25% in the Russian Arctic, which are much larger than those in other Arctic regions (0.39% to 0.64 %). The averaged value over the Arctic north of 66degN is 0.4-0.6% during spring, leading to regional surface radiative forcings of 0.7, 1.1 and 1.0Wm(exp−2) in spring 2007, 2008 and 2009, respectively.

Dou, T.↗

NASA NTRS2004

Scientific Objectives, Measurement Needs, and Challenges Motivating the PARAGON Aerosol Initiative

Aerosols are involved in a complex set of processes that operate across many spatial and temporal scales. Understanding these processes, and ensuring their accurate representation in models of transport, radiation transfer, and climate, requires knowledge of aerosol physical, chemical, and optical properties and the distributions of these properties in space and time. To derive aerosol climate forcing, aerosol optical and microphysical properties and their spatial and temporal distributions, and aerosol interactions with clouds, need to be understood. Such data are also required in conjunction with size-resolved chemical composition in order to evaluate chemical transport models and to distinguish natural and anthropogenic forcing. Other basic parameters needed for modeling the radiative influences of aerosols are surface reflectivity and three-dimensional cloud fields. This large suite of parameters mandates an integrated observing and modeling system of commensurate scope. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) concept, designed to meet this requirement, is motivated by the need to understand climate system sensitivity to changes in atmospheric constituents, to reduce climate model uncertainties, and to analyze diverse collections of data pertaining to aerosols. This paper highlights several challenges resulting from the complexity of the problem. Approaches for dealing with them are offered in the set of companion papers.

optical depth↗

NASA NTRS2014

Reply to Comment by Cole-dai Et Al. on "Climatic Impact of the Long-lasting Laki Eruption: Inapplicability of Mass-independent Sulfur Isotope Composition Measurements"

Here we respond to the comments by Cole-Dai et al. [2014] on our article Schmidt et al. [2012]. Specifically, in response to section 2 of their reply, we argued in Schmidt et al. [2012] that based on previously published estimates of the volatile release height during the 1783-1784 C.E. Laki eruption, the lack of a sulfur massindependent fractionation (MIF) anomaly is expected. In other words, no previous study on Laki ever argued that this eruption emitted SO2 into altitudes >13-15 km. In section 2.3, Cole-Dai et al. [2014] argue that the nonzero Δ33S value of their Laki sample 1 may be explained by a short-lived explosive phase at Laki during which volatiles reached the stratosphere. In Schmidt et al. [2012] in section 2, we argued in agreement with Cole-Dai et al. [2014] (section 3.1) that for a MIF anomaly to be preserved, the Laki volatiles would have had to be emitted in >20 km altitude. Our main point is that eruption column heights >20 km are unlikely based on the historical accounts and plume-rise modeling for the Laki eruption [Stothers et al., 1986; Woods, 1993; Thordarson and Self, 2003]. In Schmidt et al. [2012], we argued that to deduce a short-lived climatic impact of the Laki eruption based on the lack of a MIF anomaly and the length of the sulfate deposition in Greenland ice cores may be misleading because the climatic impact will outlast the radiative forcing of the Laki aerosol cloud. Cole-Dai et al. [2014] acknowledge the latter in their reply in section 4.2. We agreewith Cole-Dai et al. [2014] in that themagnitude and length of the climatic impact during the winter of 1783-1784 depends on the altitude of the volatile release during the eruption (sections 2.3 and 4.2). However, even if we assumed that during Laki all sulfur dioxide (SO2) would have been released in the troposphere, then the aerosol cloud would still be present in the upper troposphere during March 1784, as is evident from independent model simulations of this "tropospheric-only" scenario [Stevenson et al., 2003]. We acknowledge that there is uncertainty on the volatile release height for Laki; however, it is worth considering that those climate model simulations that used an injection altitude between 9 km and 13 km for the Laki SO2 [Highwood and Stevenson, 2003; Oman et al., 2006a, 2006b; Schmidt et al., 2012] best match the observed temperature changes during summer of 1783 [Angell and Korshover, 1985; Brázdil et al., 2010; Briffa et al., 1998; D'Arrigo and Jacoby, 1999; Jacoby et al., 1999; Kington, 1988; Manley, 1974; Parker et al., 1992; Thordarson and Self, 2003]. Based on these model simulations, a climatic impact during the winter of 1783-1784, albeit weaker than during the climactic phases of Laki, is expected (and our argument here does not exclude the role of natural variability in contributing to the cold winter of 1783-1784 as discussed in Schmidt et al. [2012]). Therefore, we continue to argue that for high-latitude eruptions such as Laki, the applicability of sulfur isotopic measurements to interpret the climatic relevance has yet to be demonstrated. Itmay transpire that the interpretation of MIF signals for the climate-relevance of an eruption is valid and unambiguous only for short-lived explosive eruptions in the tropics. In terms of the processes producing a MIF anomaly (section 3.3 in Cole-Dai et al. [2014]), the works by Hattori et al. [2013] and Ono et al. [2013] suggest that there are remaining issues not discussed by Cole-Dai et al. [2014], for instance, self-shielding of SO2 due to high column densities typical for eruptions of Pinatubo-scale and greater, and the preservation of the MIF signature in general.

general circulation model↗

NASA NTRS2012

Concentration Effects and Ion Properties Controlling the Fractionation of Halides during Aerosol Formation

During the aerosolization process at the sea surface, halides are incorporated into aerosol droplets, where they may play an important role in tropospheric ozone chemistry. Although this process may significantly contribute to the formation of reactive gas phase molecular halogens, little is known about the environmental factors that control how halides selectively accumulate at the air−water interface. In this study, the production of sea spray aerosol is simulated using electrospray ionization (ESI) of 100 nM equimolar solutions of NaCl, NaBr, NaI, NaNO2, NaNO3, NaClO4, and NaIO4. The microdroplets generated are analyzed by mass spectrometry to study the comparative enrichment of anions (f (Isub x-)) and their correlation with ion properties. Although no correlation exists between f (sub x-) and the limiting equivalent ionic conductivity, the correlation coefficient of the linear fit with the size of the anions R(sub x-), dehydration free-energy ΔGdehyd, and polarizability alpha, follows the order: (R(sub x-)(exp −2)) > (R(sub x-)(exp −1)) >(R(sub x-) > delta G(sub dehyd) > alpha. The same pure physical process is observed in H2O and D2O. The factor f (sub x-) does not change with pH (6.8−8.6), counterion (Li+, Na+, K+, and Cs+) substitution effects, or solvent polarity changes in methanol − and ethanol−water mixtures (0 <= xH2O <= 1). Sodium polysorbate 20 surfactant is used to modify the structure of the interface. Despite the observed enrichment of I− on the air−water interface of equimolar solutions, our results of seawater mimic samples agree with a model in which the interfacial composition is increasingly enriched in I− < Br− < Cl− over the oceanic boundary layer due to concentration effects in sea spray aerosol formation.

iodine↗

NASA NTRSDate not supplied

NASA TROPOMI Aerosol Products: Algorithmic Upgrades and Preliminary Evaluation

This poster presentation describes an expanded NASA TROPOMI (Tropospheric Monitoring Instrument)aerosol algorithm (N-TROPOMAER) that takes advantage of TROPOMI observations in the ultraviolet and visible spectral regions. The availability of the Oxygen B-band observations, and the unprecedentedly high spatial resolution (3.5 km X 5.5 km) for a hyper-spectral sensor are significant improvements for aerosol properties retrieval. The heritage N-TROPOMAER aerosol algorithm uses near-ultraviolet radiances at 354 nm and 388 nm from Sentinel 5 Precursor-TROPOMI for simultaneously retrieving aerosol optical depth (AOD), single-scattering albedo (SSA), aerosol absorption optical depth (AAOD), and above-cloud aerosol optical depth(ACAOD) at 388 nm, along with the qualitative UV aerosol index (UVAI). We have expanded the inversion capability beyond the UV, to retrieve AOD at 466 nm and 680 nm. Surface reflectance effects at466 nm are accounted for using a recently developed geometry-dependent surface Lambertian-equivalent reflectivity (GLER) product, which is derived from the top-of-atmosphere radiance computed with Rayleigh scattering and surface bidirectional reflectance distribution function (BRDF) for the exact viewing geometry at the sensor’s spatial resolution. Aerosol layer height (ALH) and 680 nm AOD are simultaneously derived from observations at 680 nm and at the Oxygen-B band (688 nm). Another important upgrade is the use of time averaged total column carbon monoxide from the NASA GEOS-CF(Global Earth Observing System Composition Forecast) as a tracer of carbonaceous aerosols.

TROPOMI↗

NASA NTRS1994

Summertime distribution and relations of reactive odd nitrogen species and NO(y) in the troposphere over Canada

We report here large-scale features of the distribution of NO(x), HNO3, PAN, particle NO3, and NO(y) in the troposphere from 0.15 to 6 km altitude over central Canada. These measurements were conducted in July - August 1990 from the NASA Wallops Electra aircraft as part of the joint United States-Canadian Arctic Boundary Layer Expedition (ABLE) 3B-Northern Wetlands Study. Our findings show that this region is generally NO(x) limited, with NO(x) mixing ratios typically 20-30 parts per trillion by volume (pptv). We found little direct evidence for anthropogenic enhancement of mixing ratios of reactive odd nitrogen species and NO(y) above those in 'background' air. Instead, it appears that enhancements in the mixing ratios of these species were primarily due to emissions from several day old or CO-rich-NO(x)-poor smoldering local biomass-burning fires. NO(x) mixing ratios in biomass-burning impacted air masses were usually less than 50 pptv, but those of HNO3 and PAN were typically 100-300 pptv representing a twofold-threefold enhancement over 'background' air. During our study period, inputs of what appeared to be aged tropical air were a major factor influencing the distribution of reactive odd nitrogen in the midtroposphere over northeastern North America. These air masses were quite depleted in NO(y) (generally less than 150 pptv), and a frequent summertime occurrence of such air masses over this region would imply a significant influence on the reactive odd nitrogen budget. Our findings show that the chemical composition of aged air masses over subarctic Canada and those documented in the Arctic during ABLE 3A have strikingly similar chemistries, suggesting large-scale connection between the air masses influencing these regions.

Talbot, R. W.↗

DOE OSTI2021

Insertion products in the reaction of carbonyl oxide Criegee intermediates with acids: Chloro(hydroperoxy)methane formation from reaction of CH 2 OO with HCl and DCl

The reactions of carbonyl oxides (“Criegee intermediates”) with organic and inorganic acids have been postulated to proceed predominantly by an insertion mechanism, and the hydroperoxy-substituted ester products from reactions with organic acids have been spectroscopically observed. Here this work characterizes the products from one of the simplest reactions of carbonyl oxides with inorganic acids, that of formaldehyde oxide, CH 2 OO, with hydrogen chloride, which occurs via a 1,2-insertion in the H–Cl bond. Reactions of both HCl and DCl isotopologues yield product signal at the mass of the insertion product chloro(hydroperoxy)methane and a dissociative ionisation peak at the mass of the protonated (or deuteronated) Criegee intermediate. The isotopic composition of the insertion product has been measured for reaction mixtures where both HCl isotopologues are present, and the H/D ratio of the product is consistently higher (by a factor of 1.6 ± 0.3) than that of the reactants. This isotope selectivity in the products has smaller uncertainty than the ratio of measured rate coefficients and suggests a normal (k H > k D ) kinetic isotope effect in the reaction. Theoretical kinetics calculations predict a small normal kinetic isotope effect for the overall reaction (k H / k D = 1.35 at 20 Torr N 2 and k H / k D = 1.2 for 1 atm N 2 ) but predict a substantial inverse kinetic isotope effect (k D > k H ) for the stabilisation fraction, in disagreement with the experimental observation.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS2022

Faster Tropical Upper Stratospheric Upwelling Drives Changes in Ozone Chemistry

Tropospheric trends in long-lived source gases N2O and the chlorofluorocarbons (CFCs) cause trends in O3 through changes in their reactive product gases. Transport affects the product gases because it controls the distribution of the long-lived source gases. We find that large changes in tropical upwelling 10-5 hPa since 2012 have strengthened the northern branch of the upper stratospheric (UpS) transport circulation, dramatically altering the abundances of N2O and its odd nitrogen product gases, NOx and HNO3. Increased upwelling is connected to stronger and more frequent Quasi-Biennial Oscillation easterly winds at 10 hPa and above. We use simulations with and without time varying MERRA2 meteorology to quantify the impact of dynamical changes on O3 loss via the NOx and ClOx cycles. We find that dynamical impacts on these cycles explain the mid-stratospheric tropical O3 increase and Arctic UpS O3 decrease since 2005.

Middle atmosphere chemistry and composition↗

NASA NTRSDate not supplied

Analog Environments for Venus Aerosol Instrument and Mission Concept Testing

The most common hypothesis discussed for life on Venus is a habitat in the dense, persistent clouds, which are primarily sulfuric acid with a secondary water component. Although Earth lacks a complete Venus analog environment, several partial analogs exist which can inform our understanding of the requirements for cloud habitability as well as serving as potential testbeds for future Venus instruments or missions. Earth’s tropospheric clouds have larger particles, more water, and shorter lifetimes than Venus’s; however, they have a partial overlap in pressure and temperature, and are our only example of an airborne habitat.They can inform how particle residence time and microbial generation time constrain habitable atmospheric regions. On the biological side, this includes available nutrients and energy, environmental stressors such as radiation, osmotic potential and acidity, and time spent in protective but inactive forms (endospores, cysts, akinetes); on the physical side, gravity, air density and viscosity, thermal lofting, gravity waves, scavenging due to precipitation, and other airflow dynamics, as well as effective particle radius and electrical charge. They can also enable sampling strategy tests for airborne life detection, ranging from10 2 to10 8 viable cells/mL (10 -3 to 10 -9 cells/particle). Conversely, Earth's stratospheric sulfate layer lacks an active microbial presence, and is at a colder and less dense altitude but has partially analogous values in terms of H2SO4 and water concentration, particle size, and number density. These aerosols are accessible to aircraft and high-altitude balloons. Even more accessible potential analogs include sea spray, which overlaps with the smaller (haze) particle sizes and densities at Venus and contains trace organic constituents; marine fog, which at higher densities can match Venus’s larger (Mode 2) particle properties and contains a range of trace compounds including ammonia, phosphates, sulfates, and nitrates; and spray from acidic hydrothermal systems, which can cover a wide variety of sizes, densities, and chemical compositions. These analogs could improve the development of Venus cloud sampling instruments or sondes, including field tests of material compatibility, particle capture efficiency, and analysis sensitivity.

Analog↗

DOE OSTI2023

Modeling the Impact of the Organic Aerosol Phase State on Multiphase OH Reactive Uptake Kinetics and the Resultant Heterogeneous Oxidation Timescale of Organic Aerosol in the Amazon Rainforest

Accurate predictions of chemical lifetime, i.e., oxidation timescale and change in the mass of organic aerosols (OAs) in atmospheric models, are critical to quantify the impacts of OA on aerosol–cloud interactions, radiative forcing, and air quality. The heterogeneous oxidation of OA by hydroxyl (OH) radicals is a key process governing OA mass changes during their oxidation. Recently, laboratory observations of the OH uptake coefficient (γ OH ) and heterogeneous reaction rate (k het,OH ) for different OA systems with varying phase states have been combined to develop a new parameterization of γ OH and k het,OH as a function of the OA phase state, i.e., viscosity (η OA ). Here, in this work, we use a recently published viscosity prediction framework to analyze the new γ OH and k het,OH parameterization with a box model. Subsequently, we implement this box model to predict γ OH and k het,OH over the Amazon rainforest in the dry-to-wet transition season with both significant biomass burning and biogenic influences. Relevant parameters within our box model are specified based on detailed regional model simulations over the Amazon using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). η OA is predicted as a function of species volatility, OA composition (including water uptake) along with ambient relative humidity (RH), and temperature. Based on ambient conditions simulated by WRF-Chem over the entire atmospheric column, we use the box model to predict the upper bounds of the heterogeneous oxidation timescale of OA. Based on previous laboratory measurements, we assume that this heterogeneous OH oxidation causes fragmentation (carbon loss) of OA, followed by the evaporation of the fragmented molecules that results in the exponential decay of OA. We predict that the oxidation timescale of OA is ~1 month near the Earth’s surface in the pristine Amazonian background because of low OH concentrations. But OA is oxidized more rapidly within urban and wildfire plumes near the Earth’s surface with an order of magnitude higher OH concentrations compared to the pristine background, causing the simulated oxidation timescale of OA to be much shorter, ~3–4 days. At 3–5 km altitudes where biomass burning OA is predicted to be semisolid, the heterogeneous oxidation timescale is estimated as ~6 days to 3 weeks and decreases with increasing OH concentrations within plumes. We show that the simulated mass loss of OA is strongly size-dependent, where smaller particles oxidize more rapidly compared to larger particles due to their greater per-particle surface area-to-volume ratio. Increasing urbanization and deforestation in the Amazon in the future might increase OH concentrations in the background Amazon, causing faster oxidation of OA. At higher altitudes above liquid clouds, especially in the upper troposphere where temperatures approach ~250 K, future measurements are needed to reduce the uncertainties related to the mass loss of OA at colder temperatures and low relative humidity conditions due to its heterogeneous OH oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2004

Winds, Water Budgets and Stable Isotopes in Tropical Cyclones using TRMM and QUICKSCAT

Water vapor is the most abundant greenhouse gas in the atmosphere. Changes in its concentration and distribution are controlled by the hydrologic cycle. Because of its capacity to absorb and emit long wave radiation, release latent heat during condensation in storms and reflect short wave radiation when clouds form it has a major impact on Global climate change. The stable isotope ratios of water are H20 H2l6O and H0 H2l6O. These ratios change whenever water undergoes a phase change. They also change in both rain and water vapor whenever an air parcel is exposed to rain. In addition the relative changes in the two ratios differ as a &nction of the relative humidity. In short, the stable isotope ratios in water vapor in the atmosphere contain an integrated history of the processes affecting the concentration and distribution of water vapor in the atmosphere. Therefore the measurement and interpretation of changes in these stable isotope ratios are a powerful tool matched by no other method in tracing the transport history of water in the atmosphere. Our initial studies under this grant focused on the changes of the stable isotope ratios of precipitation and water vapor in tropical cyclones. The changes in time and space were found to be very large and to trace the transport of water in the storms reflecting changes in basic structural features. Because the stable isotope ratios of rains from tropical cyclones are so low flooding associated with land falling tropical cyclones introduces a negative isotopic spike into the coastal surface waters. In addition the stable isotope ratios of water vapor in the vicinity of tropical cyclones is anomalously low. This suggests that carbonate shelled organisms such as ostracoda living in coastal waters have the potential to record the isotopic spike and thereby provide a long term record of tropical storm activity in sediment cores containing fossil shells. Likewise, tree rings in coastal environments offer a similar potential. We have analyzed the oxygen isotopic composition of ostrcoda shells formed in the floodwaters of Tropical Storm Allison (2001) and discovered the negative isotopic 1 16 spike. Because we had learned that storm activity has a major impact on the stable isotope ratios of water vapor in the tropics and sub-tropics we decided to analyze the isotopic compositions of water vapor in different locations in the tropics. We did this in Puerto Escondido, Mexico in July 1998, near Kwajalein Island in the Pacific in 1999 as part of a TRMM summer field program and in 2001 in Key West, Florida as part of the CAMEX 4 summer field program. Our isotopic studies along with our earlier tropical cyclone studies showed that the low isotopic ratios in water vapor induced by exposure to rains the storms persisted for 48 hours often far away from the original storm site. We also noted that positive isotopic spikes were introduced into atmospheric water vapor if winds were high and extensive sea spray was present. These findings have a significant impact on the interpretation of the stable isotope studies of tropical ice cores found in the high mountain regions of the tropics. The assumption made in interpreting the ice core record is that the source water vapor evaporated from the sea surface is in near isotopic equilibrium with the seawater and undergoes a decrease during its transport that reflects the change in temperature from the sea surface to the site of the ice core. Because an additional isotopic depletion occurs at the sea surface source area that depends on the intensity, duration and size of the tropical rain system the isotopic variations found in the ice cores must take into account changes in past storm activity in the tropics. These systems must be an important source of water vapor to the ice cores because they charge the troposphere with water vapor to a far greater vertical height than evaporation in quiescent regions. Finally, an interest in increased heat transfer in thnterior of tropical cyclones resulting from greater amounts of sea spray is a topic of considerable interest to the research community. Increases in sea spray may be related to rapid changes in the intensity of hurricanes, a feature of hurricanes that currently is very poorly forecast. Project CBLAST of the Hurricane Research Division of NOAA is an active program that uses P3 research aircraft to evaluate this problem. An instrument has been designed and built at the University of Houston that will be placed on the P3 research aircraft during the 2004 hurricane season. It continuously measures the salt content of rain in hurricanes. Changes in the salt content of the rains should reflect the abundance of sea spray at the sea surface. In this way maps of sea spray intensity in hurricanes may be forthcoming. This should help computer modelers who simulate hurricanes to better understand the potential of changes in sea spray to change the intensity of hurricanes. The cost of designing, building and installing this instrument was borne largely by funding from this NASA grant. A list of presentations at national meetings and publications that were as the result of funding from this NASA grant are found in the report.

Lawrence, James R.↗