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NASA NTRS1999

The Goddard Three Dimensional Chemistry and Transport Model-A Waystation on the Road to Predicting the Future of Stratospheric Ozone

The Goddard 3D Chemistry and Transport Model (CTM) is an off-line model which includes a full description of stratospheric photochemistry and calculates constituent transport using winds and temperatures from the Goddard Earth Observing System Data Assimilation System. The model can be used to understand and quantify the photochemical and transport processes which produce observed constituent evolution and variability. Data from any platform - ground based, aircraft, balloon, satellite - can play a role. Since any measurement systems has its own set of advantages and disadvantages (e.g., good temporal sampling but poor spatial sampling; good spatial and temporal sampling but poor vertical resolution; high vertical resolution and spatial sampling but poor temporal sampling), using data from disparate sources and a CTM can provide a more complete picture of atmospheric processes.

Douglass, Anne↗

DOE OSTI2023

Revisiting the equatorial Pacific sea surface temperature response to global warming

The relative roles of the oceanic and atmospheric processes in the pattern formation of the equatorial Pacific sea surface temperature (SST) response to global warming is investigated using a set of climate model experiments embedded with a novel partial coupling technique. Here, the modeling results show that the SST response experiences a transition from a La Niña-like warming pattern at the initial stage to an El Niño-like warming pattern at the quasi-equilibrium stage. By decomposing anomalous equatorial Pacific SST into atmosphere-forced passive component and ocean dynamics-induced active component, it is found that the SST warming pattern at both stages is entirely induced by its active component. Specifically, the meridional and vertical ocean circulation changes play a dominant role in forming the La Niña-like SST warming pattern at the initial stage, and the zonal and meridional ocean circulation changes are responsible for the formation of the El Niño-like SST warming pattern at the quasi-equilibrium stage. In contrast, the passive SST at both stages is characterized by a zonally uniform warming along the equator, which can be explained by a balance between the cooling effect associated with mean upwelling and the warming effect due to surface passive heat flux change. In addition, this study finds that it is the slowdown of the Pacific subtropical cells during the transition period that controls the evolution of the equatorial SST warming pattern by changing the meridional and vertical ocean heat transports.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth's biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June-October), aerosol particles reaching 3-5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2021

An overview of the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) project: aerosol–cloud–radiation interactions in the southeast Atlantic basin

Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.

Jens Redemann↗

NASA NTRS1999

Assessed Using Satellite Data and Ground Based Sun/Sky Radiometers

The short aerosol lifetime and the variety of sources and atmospheric processes that affect the aerosol concentration and properties, generate a very heterogeneous aerosol field. Satellite data are needed to assess the daily global distribution of aerosol loading, properties and radiative forcing of climate. The Moderate Resolution Imaging Spectroradiometer (MODIS) instrument launched in July 1999 measures the aerosol properties and backscattered radiation in 7 spectral channels across the solar channel with spatial resolution of 500 m. Novel inversion techniques are used to derive the aerosol forcing at the top of the atmosphere in these 7 spectral bands with even higher accuracy than the derivation of the aerosol loading or microphysical properties. But satellites cannot sense the aerosol attenuation of radiation reaching the Earth surface. A network of 100 sun/sky radiometers, members of the AErosol RObotic NEtwork (AERONET) is used to assess, simultaneously, the radiative forcing of aerosol at the surface level. The relevance of MODIS and AERONET to assess the global aerosol forcing, and the inversion techniques will be presented and discussed.

Kaufman, Yoram J.↗

DOE OSTI2026

Experimental protocol for phase 1 of the APARC QUOCA (QUasibiennial oscillation and Ozone Chemistry interactions in the Atmosphere) working group

The quasi-biennial oscillation (QBO) is the main mode of variability in the tropical stratosphere, influencing the predictability of other regions in the atmosphere through its teleconnections to the stratospheric polar vortices and coupling to surface tropical and extratropical variability. However, climate and forecasting models consistently underestimate QBO amplitudes in the lower stratosphere, likely contributing to their failure to simulate these teleconnections. One underexplored contributor to model biases is missing representation of ozone-radiative feedbacks, which enhance temperature variability in the lower stratosphere, particularly at periods at and greater than the QBO (>28 months). While previous studies suggest that ozone-radiative feedbacks can impact QBO periods, amplitudes and the associated secondary circulation in the lower stratosphere, the reported impacts differ widely among models and are hard to interpret due to differences in methodology. To this end, here we propose a coordinated experimental protocol – held joint between the Atmospheric Processes and their Role in Climate (APARC) Quasi-Biennial Oscillation Initiative (QBOi) and Chemistry Climate Modeling Initiative (CCMI) activities – which is aimed at assessing the coupling between stratospheric ozone, temperature and the circulation. We use the proposed experiments to define the ozone feedback on the QBO in both present-day and idealized (abrupt quadrupling of carbon dioxide) climates. While primary focus is on the QBO, the proposed protocol also enables analysis of other aspects of ozone-radiative-dynamical coupling in the atmosphere, including impacts on the Brewer-Dobson Circulation and tropospheric eddy-driven jet responses to future climate change. Here we document the scientific rationale and design of the QUOCA Phase 1 experiments, summarize the data request, and give a brief overview of participating models. Preliminary results using the NASA Goddard Institute for Space Studies E2-2 climate model are used to illustrate sensitivities to certain methodological choices.

Environmental sciences↗

DOE OSTI2020

The atmospheric importance of methylamine additions to Criegee intermediates

We report that Criegee intermediates are important targets for study in atmospheric chemistry because of their capacity to oxidize airborne species. Among these species, ammonia has received critical attention for its presence in polluted agricultural or industrial areas and its role in forming particulate matter and condensation nuclei. Although methylamine has been given less attention than ammonia, both theoretical and experimental studies have demonstrated that the additional methyl substitution on the ammonia derivatives increases the rate constants for some systems. This suggests that the methylamine addition to Criegee intermediates could be more significant to atmospheric processes. In this work, geometries are optimized at the DF-CCSD(T)/ANO1 level for the methylamine addition reactions to the simplest Criegee intermediate and the anti- and syn-methylated Criegee intermediates. Energies for each stationary point were computed at the CCSD(T)/CBS level with corrections from the CCSDT(Q) method. Rate constants are obtained for each reaction using canonical transition state theory. Although methylamine addition proved to be a more favorable reaction relative to ammonia addition, the significantly lower concentration of atmospheric methylamine limits the prevalence of these reactions, even in the most optimal conditions. It is unlikely that the methylamine addition to Criegee intermediates will contribute significantly to the consumption of Criegee intermediates in the atmosphere.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Direct kinetic measurements and theoretical predictions of an isoprene-derived Criegee intermediate

Isoprene has the highest emission into Earth’s atmosphere of any nonmethane hydrocarbon. Atmospheric processing of alkenes, including isoprene, via ozonolysis leads to the formation of zwitterionic reactive intermediates, known as Criegee intermediates (CIs). Direct studies have revealed that reactions involving simple CIs can significantly impact the tropospheric oxidizing capacity, enhance particulate formation, and degrade local air quality. Methyl vinyl ketone oxide (MVK-oxide) is a four-carbon, asymmetric, resonance-stabilized CI, produced with 21 to 23% yield from isoprene ozonolysis, yet its reactivity has not been directly studied. We present direct kinetic measurements of MVK-oxide reactions with key atmospheric species using absorption spectroscopy. Direct UV-Vis absorption spectra from two independent flow cell experiments overlap with the molecular beam UV-Vis-depletion spectra reported recently [M. F. Vansco, B. Marchetti, M. I. Lester, J. Chem. Phys. 149, 44309 (2018)] but suggest different conformer distributions under jet-cooled and thermal conditions. Comparison of the experimental lifetime herein with theory indicates only the syn -conformers are observed; anti -conformers are calculated to be removed much more rapidly via unimolecular decay. We observe experimentally and predict theoretically fast reaction of syn -MVK-oxide with SO 2 and formic acid, similar to smaller alkyl-substituted CIs, and by contrast, slow removal in the presence of water. We determine products through complementary multiplexed photoionization mass spectrometry, observing SO 3 and identifying organic hydroperoxide formation from reaction with SO 2 and formic acid, respectively. The tropospheric implications of these reactions are evaluated using a global chemistry and transport model.

09 BIOMASS FUELS↗

DOE OSTI2023

Simulating the Transport and Rupture of Pollen in the Atmosphere

Pollen, one type of primary biological aerosol particle (PBAP), is emitted from the terrestrial biosphere and can undergo physical changes in the atmosphere via particle rupture. To examine the fate of pollen and its atmospheric processing, a pollen emission and transport scheme is coupled to the Weather Research and Forecasting Model with Chemistry (WRF-Chem). We simulate the emission of pollen and its impacts on the cloud properties and precipitation in the Southern Great Plains from 12 to 19 April 2013, a period with both high pollen emissions and convective activity. We conduct a suite of ensemble runs that simulate primary pollen and three different pollen rupture mechanisms that generate subpollen particles, including (a) high humidity-induced surface rupture, (b) high humidity-induced in-atmosphere plus surface rupture, and (c) lightning-induced rupture, where in-cloud and cloud-to-ground lightning strikes trigger pollen rupture events. When relative humidity is high (>80%), coarse primary pollen (~1 μg m –3 ) is converted into fine subpollen particles (~1.2e –4 μg m –3 ), which produces 80% more subpollen particles than lightning-induced rupture. The in-atmosphere humidity-driven rupture predominantly produces subpollen particles, which is further enhanced during a frontal thunderstorm. During strong convection, vertical updrafts lift primary pollen and subpollen particles (~0.5e –4 μg m –3 ) to the upper troposphere (~12 km) and laterally transports the ruptured pollen in the anvil top outflow. In regions of high pollen and strong convection, ruptured pollen can influence warm cloud formation by decreasing low cloud (<4 km) cloud water mixing ratios and increasing ice phase hydrometeors aloft (>10 km)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Ice nucleation ability of loess from the northwestern United States

The heterogeneous nucleation of ice processes involving loess particles that influences the formation of mixed-phase clouds are poorly understood. Here, the ice nucleating ability of wind-blown dust or loess accumulated from the past glaciated area was investigated at three temperatures: -26, -30, and -34 °C and at below and above saturation with respect to liquid water conditions. Total six loess samples from different regions across Columbia Basin province, WA, USA were collected, dry dispersed, size-selected at mobility diameter 200 nm, and investigated for their ice nucleation efficiency. To understand the effect of atmospheric processing during long-range transport on their ice nucleating ability, similar experiments were also performed on acid-treated loess samples. Additionally, the ice nucleating properties of Arizona Test Dust (ATD) were investigated as a surrogate for natural mineral dust particles to test the experimental approach. Results show that treated particles have lower ice nucleation efficiency compared to untreated particles at all temperature and saturation with respect to liquid water conditions. Comparison based on ice-active site density ( N s ) metric indicate that loess particles at saturation with respect to liquid water conditions are marginally more efficient than the mineral and soil dust values reported in the literature, but they have lower efficiencies than the predicted N s efficiency of K-feldspar particles at supercooled temperatures greater than -38 °C.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Spectro-Microscopy Studies of Atmospheric Particles

Our project investigated composition and physical properties of individual atmospheric particles collected in field campaigns organized by the DOE Atmospheric Systems Research and Atmospheric Radiation Measurement (ASR/ARM) programs, such as the Green Ocean Amazon (GoAmazon, 2014/5), the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE, 2016/7), the Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA, 2017/8), the Aerosol–Ice Formation Closure Pilot Study (AEROICESTUDY, 2019) and in additional small-scale supporting field experiments focused on the investigation of the light-absorbing (aka brown carbon) atmospheric particles. In these studies, we investigated the contribution of natural and anthropogenic sources to populations of atmospheric particles during representative atmospheric conditions; characterized particle composition and evaluated their hygroscopic properties and propensity to act as cloud condensation nuclei (CCN) and ice nuclei (IN); correlated typical particle-type and mixing state characteristics with real-time measurements in the areas of studies. We used multi-modal spectro-microscopy techniques to examine elemental and molecular composition, mixing state, size, and higher order morphology for individual particles. Specifically, we used computer-controlled scanning electron microscopy and X-ray microanalysis for quantitative analysis of particle elemental composition, and we used transmission electron microscopy to provide additional information on the distribution of different components within individual particles (particle heterogeneity). We used synchrotron-based scanning transmission X-ray microscopy for quantitative description of the mixing state and molecular bonding of carbon in particles. The particle composition, mixing state, and morphology from analyzed periods was then combined with the real-time ARM measurements of aerosol size distribution, CCN concentration, hygroscopicity, and aerosol bulk composition. Combined together, results of our studies allowed us to assess the major particle sources (biogenic vs. anthropogenic, primary vs secondary) and gain insight into the atmospheric processing of aerosol particles resulting from condensation, coagulation, oxidative aging, and cloud processing. In collaboration with other scientists involved in field campaigns, we carried out statistical analysis of particle properties and their source-specific contributions to regional aerosol loading under representative air mass, meteorological, and cloud conditions.

scanning transmission X-ray microscopy↗

NASA NTRS1998

Choosing Meteorological Input for the Global Modeling Initiative Assessment of High Speed Aircraft

The Global Modeling Initiative (GMI) science team is developing a three dimensional chemistry and transport model (CTM) to be used in assessment of the atmospheric effects of aviation. Requirements are that this model be documented, be validated against observations, use a realistic atmospheric circulation, and contain numerical transport and photochemical modules representing atmospheric processes. The model must also retain computational efficiency to be tractable to use for multiple scenarios and sensitivity studies. To meet these requirements, a facility model concept was developed in which the different components of the CTM are evaluated separately. The first use of the GMI model will be to evaluate the impact of the exhaust of supersonic aircraft on the stratosphere. The assessment calculations will depend strongly on the wind and temperature fields used by the CTM. Three meteorological data sets for the stratosphere are available to GMI: the National Center for Atmospheric Research Community Climate Model (CCM2), the Goddard Earth Observing System Data Assimilation System (GEOS DAS), and the Goddard Institute for Space Studies general circulation model (GISS). Objective criteria were established by the GMI team to identify the data set which provides the best representation of the stratosphere. Simulations of gases with simple chemical control were chosen to test various aspects of model transport. The three meteorological data sets were evaluated and graded based on their ability to simulate these aspects of stratospheric measurements. This paper describes the criteria used in grading the meteorological fields. The meteorological data set which has the highest score and therefore was selected for GMI is CCM2. This type of objective model evaluation establishes a physical basis for interpretation of differences between models and observations. Further, the method provides a quantitative basis for defining model errors, for discriminating between different models, and for ready re-evaluation of improved models. These in turn will lead to a higher level of confidence in assessment calculations.

Douglas, A. R.↗

NASA NTRS1999

Choosing Meteorological Input for the Global Modeling Initiative Assessment of High Speed Aircraft

The Global Modeling Initiative (GMI) science team is developing a three dimensional chemistry and transport model (CTM) to be used in assessment of the atmospheric effects of aviation. Requirements are that this model be documented be validated against observations, use a realistic atmospheric circulation, and contain numerical transport and photochemical modules representing atmospheric processes. The model must also retain computational efficiency to be tractable to use for multiple scenarios and sensitivity studies. To meet these requirements, a facility model concept was developed in which the different components of the CTM are evaluated separately. The first use of the GMI model will be to evaluate the impact of the exhaust of supersonic aircraft on the stratosphere. The assessment calculations will depend strongly on the wind and temperature fields used by the CTM. Three meteorological data sets for the stratosphere are available to GMI: the National Center for Atmospheric Research Community Climate Model (CCM2), the Goddard Earth Observing System Data Assimilation System (GEOS DAS), and the Goddard Institute for Space Studies general circulation model (GISS). Objective criteria were established by the GMI team to identify the data set which provides the best representation of the stratosphere. Simulations of gases with simple chemical control were chosen to test various aspects of model transport. The three meteorological data sets were evaluated and graded based on their ability to simulate these aspects of stratospheric measurements. This paper describes the criteria used in grading the meteorological fields. The meteorological data set which has the highest score and therefore was selected for GMI is CCM2. This type of objective model evaluation establishes a physical basis for interpretation of differences between models and observations. Further, the method provides a quantitative basis for defining model errors, for discriminating between different models, and for ready re-evaluation of improved models. These in turn will lead to a higher level of confidence in assessment calculations.

Douglass, A. R.↗

NASA NTRS1991

Titan aerosol and gas experiment for the Huygens Probe

The Cassini Mission is a joint undertaking of NASA and the European Space Agency (ESA) to explore the Saturnian System with a Saturn Orbiter and a Titan Probe. The launch vehicle and the Saturn Orbiter are the responsibility of NASA while the Huygens Probe (detachable Titan Probe) is the responsibility of ESA. The spacecraft will be launched in 1996 and the Huygens Probe will arrive at Titan in 2003. The Cassini Mission-Huygens Probe provides a unique opportunity to obtain detailed information about the atmosphere and, possibly, the surface of Titan. Titan possesses a substantial nitrogen atmosphere containing methane and many other organic compounds. Aerosols play an important role in the atmospheric processes on Titan. The Huygens Probe offers an opportunity to determine how organic particles are formed and grow which will clarify their role on Earth. A powerful analytical instrument, capable of addressing the above technology and other science questions, was recently proposed for the Huygens Probe. It is comprised of an aerosol and gas sampler and processor, and a gas chromatograph-ion mobility spectrometer. The instrument will be able to measure complex organics that make up the collected aerosols to the approximate 1 ppm level. Gases will be measured to approximately 10 ppb. Because the Titan atmosphere is expected to be quite complex, a gas chromatograph-ion mobility spectrometer is used to provide unequivocal identification of the components of the analytes. Further details of the science question to be investigated and the proposed instrument are described. The expected results and their implications are also addressed.

Carle, G. C.↗

DOE OSTI2020

A Causal Inference Model Based on Random Forests to Identify the Effect of Soil Moisture on Precipitation

Soil moisture influences precipitation mainly through its impact on land–atmosphere interactions. Understanding and correctly modeling soil moisture–precipitation (SM–P) coupling is crucial for improving weather forecasting and subseasonal to seasonal climate predictions, especially when predicting the persistence and magnitude of drought. However, the sign and spatial structure of SM–P feedback are still being debated in the climate research community, mainly due to the difficulty in establishing causal relationships and the high degree of nonlinearity in land–atmosphere processes. To this end, we developed a causal inference model based on the Granger causality analysis and a nonlinear machine learning model. This model includes three steps: nonlinear anomaly decomposition, nonlinear Granger causality analysis, and evaluation of the quality of SM–P feedback, which eliminates the nonlinear response of interannual and seasonal variability and the memory effects of climatic factors and isolates the causal relationship of local SM–P feedback. We applied this model by using National Climate Assessment–Land Data Assimilation System (NCA-LDAS) datasets over the United States. Here, the results highlight the importance of nonlinear atmosphere responses in land–atmosphere interactions. In addition, the strong feedback over the southwestern United States and the Great Plains both highlight the impacts of topographic factors rather than only the sensitivity of evapotranspiration to soil moisture. Furthermore, the SM–P index defined by our framework is used to benchmark Earth system models (ESMs), which provides a new metric for efficiently identifying potential model biases in modeling local land–atmosphere interactions and may help the development of ESMs in improving simulations of water cycle variability and extremes.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2012

Improvement in Simulation of Eurasian Winter Climate Variability with a Realistic Arctic Sea Ice Condition in an Atmospheric GCM

The present study investigates how much a realistic Arctic sea ice condition can contribute to improve simulation of the winter climate variation over the Eurasia region. Model experiments are set up using different sea ice boundary conditions over the past 24 years (i.e., 1988-2011). One is an atmospheric model inter-comparison (AMIP) type of run forced with observed sea-surface temperature (SST), sea ice, and greenhouse gases (referred to as Exp RSI), and the other is the same as Exp RSI except for the sea ice forcing, which is a repeating climatological annual cycle (referred to as Exp CSI). Results show that Exp RSI produces the observed dominant pattern of Eurasian winter temperatures and their interannual variation better than Exp CSI (correlation difference up to approx. 0.3). Exp RSI captures the observed strong relationship between the sea ice concentration near the Barents and Kara seas and the temperature anomaly across Eurasia, including northeastern Asia, which is not well captured in Exp CSI. Lagged atmospheric responses to sea ice retreat are examined using observations to understand atmospheric processes for the Eurasian cooling response including the Arctic temperature increase, sea-level pressure increase, upper-level jet weakening and cold air outbreak toward the mid-latitude. The reproducibility of these lagged responses by Exp RSI is also evaluated.

sea-ice↗

NASA NTRS2018

Development of a Mars Lidar (MARLI) for Measuring Wind and Aerosol Profiles from Orbit

Our understanding of the Mars atmosphere and the coupled atmospheric processes that drive its seasonal cycles is limited by a lack of observation data, particularly measurements that capture diurnal and seasonal variations on a global scale. As outlined in the 2011 Planetary Science Decadal Survey and the recent Mars Exploration Program Analysis Group(MEPAG) Goals Document, near-polar-orbital measurements of height-resolved aerosol backscatter and wind profiles area high-priority for the scientific community and would be valuable science products as part of a next-generation orbital science package. To address these needs, we have designed and tested a breadboard version of a direct detection atmospheric wind lidar for Mars orbit. It uses a single-frequency, seeded Nd:YAG laser ring oscillator operating at 1064nm (4 kHz repetition rate), with a 30-ns pulse duration amplified to 4 mJ pulse energy. The receiver uses a Fabry-Perotetalon as part of a dual-edge optical discrimination technique to isolate the Doppler-induced frequency shift of the back scattered photons. To detect weak aerosol backscatter profiles, the instrument uses a 4x4 photon-counting HgCdTeAPD detector with a 7 MHz bandwidth and < 0.4 fW/Hz(exp 1/2) noise equivalent power. With the MARLI lidar breadboard instrument, we were able to measure Doppler shifts continuously between 1 and 30 m/s by using a rotating chopper wheel to impart a Doppler shift to incident laser pulses. We then coupled the transmitter and receiver systems to a laser ranging telescope at the Goddard Geophysical and Astronomical Observatory (GGAO) to measure backscatter and Doppler wind profiles in the atmosphere from the ground. We measured a 5.3 ± 0.8 m/s wind speed from clouds in the planetary boundary layer at a range of 4 to 6 km. This measurement was confirmed with a range-over-time measurement to the same clouds as well as compared to EMC meteorological models. Here we describe the lidar approach and the breadboard instrument, and report some early results from ongoing field experiments.

Cremons, Daniel R.↗

DOE OSTI2022

Drastically different restructuring of airborne and surface-anchored soot aggregates

Combustion soot particles are fractal aggregates of hydrophobic spherules. Mixing of soot particles with other chemicals during atmospheric processing may partially offset their hydrophobicity, promoting water uptake and structural compaction. Here, we investigated morphological changes in fractal soot particles coated by sulfuric acid and then humidified, both in airborne and surface-bound states. Airborne soot was probed by tandem differential mobility analysis. Surface-bound soot was studied in a controlled microenvironment of a closed cell, using environmental transmission electron microscopy. After humidification, the airborne particles became fully compact, but the deposited particles showed only minor morphological changes despite significant water uptake. Although minor, those changes were detected during both water condensation and evaporation, indicating that condensation-evaporation cycles play an important role in atmospheric soot compaction. Lesser restructuring of deposited aggregates was caused by surface anchoring and coating loss, making anchoring an indispensable tool for preserving morphology of aggregates against changing experimental environment.

54 ENVIRONMENTAL SCIENCES↗