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DOE OSTI2025

Unraveling Electronic Effects that Influence the Bimolecular Chemistry of Fluorinated Criegee Intermediates

Ozonolysis is important for the removal of unsaturated volatile organic compounds emitted into the Earth's atmosphere. The alkene + ozone reaction (alkene ozonolysis) forms a carbonyl oxide – a Criegee intermediate (CI). CIs are interesting from an atmospheric chemistry perspective. They are implicated in enhancing the oxidizing capacity of the troposphere and in secondary organic aerosol formation. CIs may participate in bimolecular reactions with trace atmospheric vapors like water and methanol. Here, the chemistry of the two isomers of CFHOO and of CF 3 CHOO with water, water dimer, and methanol is explored. The present study confirms that the syn-conformer is the minimum energy structure for both CIs and that the reactions of anti-CFHOO display slightly lower activation energies cf. syn-CFHOO, thus promoting faster reaction. For both syn- and anti-CFHOO, the energy barrier in the pathway to adding water, water dimer, or methanol is lower—and the overall reaction exoergicity greater—than for the corresponding reactions involving the nonfluorinated analogue, CH 2 OO. Here, the corresponding bimolecular reaction rates are thus predicted to be faster for CFHOO than CH 2 OO. Similar reactivity trends are found when comparing the same reactions of syn-CF 3 CHOO, cf. syn-CH 3 CHOO, but not when comparing the energetics of the reactions involving anti-CF 3 CHOO cf. anti-CH 3 CHOO.

Guidry, Lily M. [University of Louisiana at Lafaye↗

DOE OSTI2022

Local conformations and heterogeneities in structures and dynamics of isotactic polypropylene adsorbed onto carbon fiber

Carbon fiber (CF) reinforced polymers (CFRPs) have experienced widespread use in various industries. One of the most important parameters that controls the macroscopic property of CFRPs is the interface between a polymer matrix and CF. There is growing evidence to suggest the formation of a bound polymer layer (BPL), i.e., polymer chains that physically adsorb on a filler surface. However, this interface is always in contact with the thicker part of a polymer matrix, rendering its understanding a difficult task. Therein, we use CF-reinforced isotactic polypropylene (iPP) as a rational CFRP. To characterize the BPL on the CF surface, we extracted it from the CFRP using solvent-rinsing with p-xylene. The physical and thermal properties of the BPL were characterized by differential scanning calorimetry and thermogravimetric analysis, while its microscopic structures and dynamics were probed by small-angle neutron scattering and quasi-elastic neutron scattering (QENS) techniques. Subsequently, we employed atomistic molecular dynamics (MD) simulations to complement the QENS results above the bulk melting temperature and reveal details that were experimentally inaccessible. In this work, we observed that the degree of crystallinity of the BPL was quite lower than the bulk, while the melting temperature of the BPL remained the same as the bulks. Within the given length and time scales probed by QENS and MD, we also observed that most of the bound chains were mobile, with the formation of a high-density region (less than 1 nm in thickness) near the CF surface. The segmental dynamics of the bound chains probed by both QENS and MD were also much faster than those of the free chains, possibly due to the presence of a free surface region at the topmost surface of the BPL. Furthermore, the MD results demonstrated that the backbone chains and side groups lie nearly flat on the CF surface, which is the driving force for the flattening process of the iPP BPL to overcome the conformational entropy loss in the total free energy.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Pressure-Induced Spectroscopic Changes in a Californium 1D Material Are Twice as Large as Found in the Holmium Analog

Here, in this study, the synthesis, characterization, and pressure response of a 1D californium mellitate (mellitate = 1,2,3,4,5,6-benzenehexacarboxylate) coordination polymer, Cf 2 (mell)(H 2 O) 10 ·4H 2 O (Cf-1), are reported. The Cf–O lengths within the crystal structure are compared to its gadolinium (Gd-1) and holmium (Ho-1) analogs as well. These data show that the average Cf–O bond distance is slightly longer than the average Gd–O bond, consistent with trends in effective ionic radii. UV–vis-NIR absorption spectra as a function of pressure were collected using diamond-anvil techniques for both Cf-1 and Ho-1. These experiments show that the Cf(III) f → f transitions have a stronger dependence on pressure than that of the holmium analog. In the former case, the shift is nearly linear with applied pressure and averages 6.6 cm –1 /GPa, whereas in the latter, it is <3 cm –1 /GPa.

absorption spectroscopy↗

DOE OSTI2024

Design Principles and Routes for Calcium Alkoxyaluminate Electrolytes

Multivalent-ion battery technologies are increasingly attractive options for meeting diverse energy storage needs. Calcium ion batteries (CIB) are particularly appealing candidates for their earthly abundance, high theoretical volumetric energy density, and relative safety advantages. Here, at present, only a few Ca-ion electrolyte systems are reported to reversibly plate at room temperature: for example, aluminates and borates, including Ca[TPFA] 2 , where [TPFA] - = [Al(OC(CF 3 ) 3 ) 4 ] - and Ca[B(hfip) 4 ] 2 , [B(hfip) 4 ] 2 – = [B(OCH(CF 3 ) 2 ) 4 ] - . Analyzing the structure of these salts reveals a common theme: the prevalent use of a weakly coordinating anion (WCA) consisting of a tetracoordinate aluminum/boron (Al/B) center with fluorinated alkoxides. Leveraging the concept of theory-aided design, we report an innovative, one-pot synthesis of two new calcium-ion electrolyte salts (Ca[Al(tftb) 4 ] 2 , Ca[Al(hftb) 4 ] 2 ) and two reported salts (Ca[Al(hfip) 4 ] 2 and Ca[TPFA] 2 ) where hfip = (-OCH(CF 3 ) 2 ), tftb = (-OC(CF 3 )(Me) 2 ), hftb = (-OC(CF 3 ) 2 (Me)), [TPFA] - = [Al(OC(CF 3 ) 3 ) 4 ] - . We also reveal the dependence of Coulombic efficiency on their inherent propensity for cation–anion coordination.

25 ENERGY STORAGE↗

DOE OSTI2020

Routes to Acetonitrile-Supported Trifluoromethyl and Perfluorometallacyclopentane Complexes of Cobalt

In this report, synthetic routes to [(MeCN) 3 Co(CF 3 ) 3 ], [Co(MeCN) 6 ][PF 6 ] 2 , [(MeCN) 4 Co(CF 3 ) 2 ][PF 6 ], [(MeCN) 2 (py)Co(CF 3 ) 3 ], [(MeCN)(py) 2 Co(CF 3 ) 3 ], and [(MeCN) 4 Co(C 4 F 8 )][PF 6 ] are described. The unusual [(py) 2 (CF 3 ) 2 Co(μ-CH 2 CN)] 2 has also been identified as a decomposition product of [(py) 2 (MeCN)Co(CF 3 ) 3 ]. In conclusion, the aforementioned compounds, all of which have been characterized by X-ray crystallography, are expected to serve as useful precursors to cobalt trifluoromethyl- and C 4 F 8 -containing derivatives.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Chemical bonding in actinyl( V / VI ) dipyriamethyrin complexes for the actinide series from americium to californium: a computational investigation

The separation of minor actinides in their dioxocation (i.e., actinyl) form in high-valence oxidation states requires efficient ligands for their complexation. Here, in this work, we evaluate the complexation properties of actinyls including americyl, curyl, berkelyl, and californyl in their pentavalent and hexavalent oxidation states with the dipyriamethyrin ligand (L) using density functional theory calculations. The calculated bond parameters show shorter An&#x2550O yl bonds with covalent character and longer An–N bonds with ionic character. The bonding between the actinyl cation and the ligand anion shows a flow of charges from the ligand to actinyl in all [An V/VI O 2 –L] 1–/0 complexes. However, across the series, backdonation of charges from the metal to the ligand becomes prominent and stabilizes the complexes. The thermodynamic parameters in the gas phase and solution suggest that the complex formation reaction is spontaneous for [Cf V/VI O 2 –L] 1–/0 complexes and spontaneous at elevated temperatures (>298.15 K) for all other complexes. Spin–orbit corrections have a quantitative impact while the overall trend remains the same. Energy decomposition analysis (EDA) reveals that the interaction between actinyl and the ligand is mainly due to electrostatic contributions that decrease from Am to Cf along with an increase in orbital contributions due to the backdonation of charges from the actinyl metal center to the ligand that greatly stabilizes the Cf complex. The repulsive Pauli energy contribution is observed to increase in the case of [An V O 2 –L] 1– complexes from Am to Cf while a decrease is observed among [An VI O 2 –L] 0 complexes, showing minimum repulsion in [Cf VI O 2 –L] 0 complex formation. Overall, the hexavalent actinyl complexes show greater stability (increasing from Am to Cf) than their pentavalent counterparts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Strong mutual increase in the efficiency of isotope-selective laser IR dissociation of molecules under nonequilibrium thermodynamic conditions of the compression shock under irradiation in a bimolecular mixture

We have revealed a strong (by a factor of 2 to 5) mutual increase in the yield of IR molecular dissociation (by the example of CF{sub 2}HCl and CF{sub 3}Br) and a significant (by a factor of 1.5 to 3) lowering of dissociation thresholds in the nonequilibrium thermodynamic conditions of compression shock in the irradiation of the molecules by resonance IR laser radiation in the bimolecular mixture in comparison with their individual irradiation. This opens up the possibility to perform efficient isotope-selective IR dissociation of molecules at lower excitation energy densities (Φ ⩽ 1.5 – 2.0 J cm{sup −2}) and thereby to improve the dissociation selectivity. This was demonstrated by the example of chlorine- and bromine-isotope selective dissociation of the specified molecules, which are characterised by quite small (less than 0.25 cm{sup −1}) isotope shifts in the IR vibrational absorption spectra excited by laser radiation. The enrichment coefficients K {sub enr}({sup 35}Cl / {sup 37}Cl) = 0.90 ± 0.05 in the residual CF{sub 2}HCl gas and K {sub enr}({sup 79}Br / {sup 81}Br) in the resultant Br{sub 2} product are obtained when the CF{sub 2}HCl : CF{sub 3}Br = 1 : 1 molecular mixture and CF{sub 3}Br molecules, respectively, are irradiated by the 9R(30) CO{sub 2} laser line (frequency, 1084.635 cm{sup −1}) at an energy density Φ ≈ 1.3 J cm{sup −2}. (laser isotope separation)

36 MATERIALS SCIENCE↗

DOE OSTI2024

New ASME Section III, Division 5 Creep-Fatigue Design Rules Based on EPP and SMT Approaches

The integrated elastic-perfectly plastic (EPP) and simplified model test (SMT) creep-fatigue (CF) design methodology, referred to as the EPP-SMT method, is being developed as an alternative for CF evaluation in the design of pressure boundary components for high-temperature reactors. This report reviews the conceptual basis of the EPP-SMT methodology, summarizes the SMT experimental development efforts and results, and provides the technical basis for finalizing the EPP-SMT CF design curves for Alloy 617, based on a combined experimental and numerical approach conducted in FY 2024. This report presents the effect of hold time on the CF design curves for Alloy 617 at elevated temperatures. It includes proposed EPP-SMT CF design curves and tabulated values for continuous cycling, along with the effects of maximum hold time, for the use of this EPP-SMT CF evaluation method.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Tuning Thermal and Mechanical Properties of Polydimethylsiloxane with Carbon Fibers

In order to meet the needs of constantly advancing technologies, fabricating materials with improved properties and predictable behavior has become vital. To that end, we have prepared polydimethylsiloxane (PDMS) polymer samples filled with carbon nanofibers (CFs) at 0, 0.5, 1.0, 2.0, and 4.0 CF loadings (w/w) to investigate and optimize the amount of filler needed for fabrication with improved mechanical properties. Samples were prepared using easy, cost-efficient mechanical mixing to combine the PDMS and CF filler and were then characterized by chemical (FTIR), mechanical (hardness and tension), and physical (swelling, thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and coefficient of thermal expansion) analyses to determine the material properties. We found that hardness and thermal stability increased predictably, while the ultimate strength and toughness both decreased. Repeated tension caused the CF-filled PDMS samples to lose significant toughness with increasing CF loadings. The hardness and thermal degradation temperature with 4 wt.% CF loading in PDMS increased more than 40% and 25 °C, respectively, compared with the pristine PDMS sample. Additionally, dilatometer measurements showed a 20% decrease in the coefficient of thermal expansion (CTE) with a small amount of CF filler in PDMS. In this study, we were able to show the mechanical and thermal properties of PDMS can be tuned with good confidence using CFs.

degradation temperature↗

DOE OSTI2025

DTS data from SGP TBS

Distributed temperature-sensing data collected using a Silixa-XT DTS and 50/125 MM fiber. Data are calibrated using two water baths at the surface and an iMet aloft at the end of the fiber and tether. The data are then assigned an altitude for the TBS flight. Data collected prior to Febuary 11, 2020 were collected at the SGP Central Facility (CF). Data from 2/11/20 were collected with a Sensornet Oryx DTS at the E9 site, not at the CF. Data from May 2021 were collected with a Sensornet Oryx at the CF, and with a Silixa XT at the CF. Data from July 2021 were collected at the SGP CF, EF9, and EF36 with a Silixa XT. Data from October 2021 were collected at the SGP EF36 with a Silixa XT. Data from February 2022 were collected at the CF with a Silixa XT.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1975

Organopolysiloxane-bonded graphite fluoride as a solid lubricant

A study was conducted on the lubricating properties of organopolysiloxane-bonded graphite fluoride (CF sub 1.1) sub n films. The effects of temperature, atmosphere, composition of organopolysiloxane, and burnishing additional (CF sub 1.1) sub n powder onto the film surface were studied. For comparison, similar experiments were conducted on organopolysiloxane-bonded MoS2 films. The results are equivalent for both films, except that in a moist air environment the wear lives of the films formulated with (CF sub 1.1) sub n are up to 10 times longer than the wear lives of the MoS2-formulated films. Comparison to other (CF sub 1.1) sub n films showed organopolysiloxane films to give better lubrication results than hand-burnished (CF sub 1.1) sub n films but not as good as polyimide-bonded (CF sub 1.1) sub n films.

Fusaro, R. L.↗

NASA NTRS2014

Inferred Variable FeO Content in Medium-sized Lunar Pyroclastic Deposits from LRO Diviner Data

Lunar pyroclastic deposits (LPDs) are low albedo features that mantle underlying terrain (Gaddis et al. 1985). They are high priority targets for science and exploration as they are believed to originate from and therefore reflect the composition of the deep lunar interior (NRC, 2011). They are also the best potential resource of oxygen out of any Apollo samples (Allen et al. 1996). Historically, LPDs have been divided into regional versus local categories (Gaddis et al. 2003). The large (>1000 km2 area) regional deposits are deeply sourced (>400 km deep) and result from fire fountaining. Small (<1000 km2) local deposits are thought to result from Vulcanian eruptions in which magma is slowly emplaced beneath the surface until enough volatiles exsolve and the high pressure causes an explosion. Bennett et al. (2013) identified a local deposit (674 km2 area) that may have resulted from both Vulcanian activity and fire fountaining. This deposit potentially represents a new intermediate class of LPDs that straddles the interface between the two formation mechanisms. The deposit also exhibits the highest inferred FeO wt.% of any known lunar glass. In this work we investigate the inferred FeO abundances of other medium-sized deposits to characterize this potential new class of deposits and understand the magnitude of variations in inferred FeO among pyroclastic deposits. We use the method of Greenhagen et al. (2010) to calculate the wavelength of the Christiansen Feature (CF) from Lunar Reconnaissance Orbiter Diviner Lunar Radiometer instrument thermal-infrared observations for four medium-sized deposits. From the CF values, we estimate each deposit's FeO abundance using the method of Allen et al. (2012). The four LPDs that we examined (Oppenheimer South, Beer, Cleomedes, and J. Herschel) all have average CF values from 8.22-8.28 microns, corresponding to FeO abundances of approx. 10-15 wt.%. All of these values are within the range and uncertainties of FeO abundances measured in Apollo samples. As previously identified, the Oppenheimer South deposit exhibits an area of enhanced CF values (8.49 microns) that, if the methods of Allen et al. (2012) can be extrapolated, correspond to a highest observed approx. 30 wt.% FeO. Moon Mineralogy Mapper near-infrared spectra indicate that this area is glass-rich as opposed to olivine-rich. While we are still investigating the nature of the high CF wavelength in Oppenheimer South, spatially-resolved observations there and (to a smaller degree) in our other study sites, shows that FeO wt.% can vary within LPDs. Thus, obtaining only the average FeO abundance over a large area may not be adequate to understand global variation. The magnitude of Oppenheimer South's CF variability, if due to actual surface variations rather than calibration artifacts or spectral mixing, could indicate that it is a unique deposit and not part of a new mid-sized class of deposits. The higher value could be a result of its location within the South Pole Aitken Basin and exsolution of more deeply sourced magma due to the thin crust there.

Bennett, K. A.↗

NASA NTRS2015

Meridional Distribution of Aerosol Optical Thickness over the Tropical Atlantic Ocean

Previous studies showed that, over the global ocean, there is hemispheric asymmetry in aerosols and no noticeable asymmetry in cloud fraction (CF). In the current study, we focus on the tropical Atlantic (30 Deg N 30 Deg S) which is characterized by significant amounts of Saharan dust dominating other aerosol species over the North Atlantic. We found that, by contrast to the global ocean, over a limited area such as the tropical Atlantic, strong meridional asymmetry in dust aerosols was accompanied by meridional CF asymmetry. During the 10-year study period (July 2002 June 2012), NASA Aerosol Reanalysis (aka MERRAero) showed that, when the meridional asymmetry in dust aerosol optical thickness (AOT) was the most pronounced (particularly in July), dust AOT averaged separately over the tropical North Atlantic was one order of magnitude higher than dust AOT averaged over the tropical South Atlantic. In the presence of such strong meridional asymmetry in dust AOT in July, CF averaged separately over the tropical North Atlantic exceeded CF averaged over the tropical South Atlantic by 20%. Our study showed significant cloud cover, up to 0.8 - 0.9, in July along the Saharan Air Layer which contributed to above-mentioned meridional CF asymmetry. Both Multi-Angle Imaging SpectroRadiometer (MISR) measurements and MERRAero data were in agreement on seasonal variations in meridional aerosol asymmetry. Meridional asymmetry in total AOT over the Atlantic was the most pronounced between March and July, when dust presence over the North Atlantic was maximal. In September and October, there was no noticeable meridional asymmetry in total AOT and meridional CF distribution over the tropical Atlantic was almost symmetrical.

Cloud Fraction↗

NASA NTRS2016

Demonstration of Robustness and Integrated Operation of a Series-Bosch System

Manned missions beyond low Earth orbit will require highly robust, reliable, and maintainable life support systems that maximize recycling of water and oxygen. Bosch technology is one option to maximize oxygen recovery, in the form of water, from metabolically-produced carbon dioxide (CO2). A two stage approach to Bosch, called Series-Bosch, reduces metabolic CO2 with hydrogen (H2) to produce water and solid carbon using two reactors: a Reverse Water-Gas Shift (RWGS) reactor and a carbon formation (CF) reactor. Previous development efforts demonstrated the stand-alone performance of a NASA-designed RWGS reactor designed for robustness against carbon formation, two membrane separators intended to maximize single pass conversion of reactants, and a batch CF reactor with both transit and surface catalysts. In the past year, Precision Combustion, Inc. (PCI) developed and delivered a RWGS reactor for testing at NASA. The reactor design was based on their patented Microlith® technology and was first evaluated under a Phase I Small Business Innovative Research (SBIR) effort in 2010. The RWGS reactor was recently evaluated at NASA to compare its performance and operating conditions with NASA's RWGS reactor. The test results will be provided in this paper. Separately, in 2015, a semi-continuous CF reactor was designed and fabricated at NASA based on the results from batch CF reactor testing. The batch CF reactor and the semi-continuous CF reactor were individually integrated with an upstream RWGS reactor to demonstrate the system operation and to evaluate performance. Here, we compare the performance and robustness to carbon formation of both RWGS reactors. We report the results of the integrated operation of a Series-Bosch system and we discuss the technology readiness level.

Abney, Morgan B.↗

NASA NTRS2019

Evaluation of NASA's High-Resolution Global Composition Simulations: Understanding a Pollution Event in the Chesapeake Bay During the Summer 2017 OWLETS Campaign

Recirculation of pollutants due to a bay breeze effect is a key meteorological mechanism impacting air quality near urban coastal areas, but regional and global chemical transport models have historically struggled to capture this phenomenon. We present a case study of a high ozone (O3) episode observed over the Chesapeake Bay during the NASA Ozone Water-Land Environmental Transition Study (OWLETS) in summer 2017. OWLETS included a complementary suite of ground-based and airborne observations, with which we characterize the meteorological and chemical context of this event and develop a framework to evaluate model performance. Two publicly-available NASA global high-resolution coupled chemistry-meteorology models (CCMMs) are investigated: GEOS-CF and MERRA2-GMI. The GEOS-CF R squared value for comparisons between the NASA Sherpa C-23 aircraft measurements to the GEOS-CF resulted in good agreement (R squared: 0.67) on July 19th and fair agreement (R squared: 0.55) for July 20th. Compared to surface observations, we find the GEOS-CF product with a 25 x 25 km squared grid box, at an hourly (R squared: 0.62 to 0.87) and 15-minute (R squared: 0.64 to 0.87) interval for six regional sites outperforms the hourly nominally 50 x 50 km squared gridded MERRA2-GMI (R squared: 0.53 to 0.76) for four of the six sites, suggesting it is better capable of simulating complex chemical and meteorological features associated with ozone transport within the Chesapeake Bay airshed. When the GEOS-CF product was compared to the TOLNet LiDAR observations at both NASA Langley Research Center (LaRC) and the Chesapeake Bay Bridge Tunnel (CBBT), the median differences at LaRC were -6 to 8% and at CBBT were ± 7% between 400 to 2000 m ASL. This indicates that, for this case study, the GEOS-CF is able to simulate surface level ozone diurnal cycles and vertical ozone profiles at small scales between the surface level and 2000 m ASL. Evaluating global chemical model simulations at sub-regional scales will help air quality scientists understand the complex processes occurring at small spatial and temporal scales within complex surface terrain changes, simulating nighttime chemistry and deposition, and the potential to use global chemical transport simulations in support of regional and sub-regional field campaigns.

NASA Ozone Water-Land Environmental Transition Stu↗

NASA NTRSDate not supplied

TPSAS-NF1676L-11082-DND

Analysis of one decade of radar-lidar and Geostationary Operational Environmental Satellite (GOES) observations at the Atmospheric Radiation Measurement (ARM) Program Southern Great Plains (SGP) site reveals that there is excellent agreement in the long-term mean cloud fractions (CF) derived from the surface and GOES data, and the CF is independent of temporal resolution and spatial scales for grid boxes of size 0.5o to 2.5Â°. When computed over a 0.5-hr (4-hr) period, cloud frequency of occurrence (FREQ) and amount when present (AWP) derived from the point surface data agree very well with the same quantities determined from GOES for a 0.5o (2.5o) region centered on the ARM SGP site. The values of FREQ (AWP) derived from the radar-lidar observations at a given altitude increase (decrease) as the averaging period increases from 5 min to 6 hours. Similarly, CF at a given altitude increases as the vertical resolution increases from 90 to 1000 m. The profiles of CF have distinct bimodal vertical distributions with a lower peak between 1 and 2 km and a higher one between 8 and 11 km. The 10-year mean total CF, 46.9%, varies seasonally from a summer minimum of 39.8% to a maximum of 54.6% during the winter. The annual mean CF is 1-2% less than that from previous studies, ~48-49%, because fewer clouds occurred during 2005 and 2006, especially during winter. The differences in single- and multi-layered CFs between this study and an earlier analysis can be explained by the different temporal resolutions used in the two studies where single-layered CFs decrease but multilayered CFs increase from a 5-min resolution to a 1-hr resolution. The vertical distribution of nighttime GOES high-cloud tops agrees well with surface observations, but during daytime, fewer high clouds are retrieved by the GOES analysis than seen from the surface observations. The frequencies of occurrence for both daytime and nighttime GOES low-cloud tops are significantly higher than surface observations, but the cloud fractions are in good agreement.

B Xi↗

NASA NTRSDate not supplied

Evaluation of the GEOS-Chem UCX Stratosphere in the GEOS Composition Forecast System

The NASA GEOS Composition Forecast (GEOS-CF) system provides 3-dimensional atmospheric composition analyses and forecasts to the public in near-real time at the high spatial resolution of 25 km. While the main focus of this new product is on tropospheric air quality information, the GEOS-Chem chemistry model (v12) used in this system includes the UCX stratospheric chemistry mechanism. Here, we describe the GEOS-CF system and provide comparisons against remote-sensed observations for stratospheric composition, including measurements of HCl, ClO, NO2, and O3. The GEOS-CF nudges the stratospheric ozone towards the GEOS Forward Processing (GEOS FP) assimilated ozone product; as a result the stratospheric ozone analysis in theGEOS-CF agrees well with observations. Additionally, with the inclusion of the GEOS-Chem UCX stratospheric chemistry mechanism in GEOS-CF, 5-day forecasts, especially during the abnormal 2020 NH polar spring, capture the chemical and dynamical changes missed by the GEOS FP system, which tends towards climatology. The GEOS-CF is a new tool for the research community providing near-real time 3-dimensional gridded information on atmospheric composition throughout the troposphere and stratosphere.

Stratosphere↗

NASA NTRS2023

Observational Evidence of Strong Forcing from Aerosol Effect on Low Cloud Coverage

Aerosols cool Earth’s climate indirectly by increasing low cloud brightness and their coverage (Cf), constituting the aerosol indirect forcing (AIF). The forcing partially offsets the greenhouse warming and positively correlates with the climate sensitivity. However, it remains highly uncertain. Here, we show direct observational evidence for strong forcing from Cf adjustment to increased aerosols and weak forcing from cloud liquid water path adjustment. We estimate that the Cf adjustment drives between 52% and 300% of additional forcing to the Twomey effect over the ocean and a total AIF of −1.1 ± 0.8 W m -2 . The Cf adjustment follows a power law as a function of background cloud droplet number concentration, N d . It thus depends on time and location and is stronger when N d is low. Cf only increases substantially when background clouds start to drizzle, suggesting a role for aerosol-precipitation interactions. Our findings highlight the Cf adjustment as the key process for reducing the uncertainty of AIF and thus future climate projections.

Tianle Yuan↗