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DOE OSTI2021

Factors Affecting Entrainment Rate in Deep Convective Clouds and Parameterizations

The parameterization of cloud entrainment rates has been problematic for many years, hindering the accurate representation of convective processes in large-scale models. Here, we extend our previous work on individual shallow convection to ensemble deep convection. Entrainment rates are estimated based on three-dimensional convective clouds from August 19-20 of 1999, during the Kwajalein Experiment, simulated using a high-resolution cloud-resolving model. They are found to be negatively correlated with both vertical velocity and buoyancy, and positively correlated with the vertical divergence of the vertical velocity and with the reciprocal of cloud radii. The physical mechanisms underlying these relationships are interpreted. It is found that the parameterizations with multiple properties perform better than those with a single property. Entrainment rates and relative humidity of entrained air are positively correlated at temperature higher than 0°C, but negatively correlated at temperature lower than 0°C. Relative humidity is also included in the parameterization of entrainment rates, which differs from our previous work on shallow cumulus clouds and other studies. Finally, two forms of parameterization for entrainment rate are recommended. The first treats the entrainment rate as a function of the vertical velocity and buoyancy for temperature higher than 0°C, but as a function of relative humidity and buoyancy for temperature lower than 0°C. The second involves an equation that relates entrainment rates to vertical velocity and buoyancy regardless of temperature.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1987

The atmosphere of Uranus - Results of radio occultation measurements with Voyager 2

The Uranian atmosphere is investigated on the basis of S-band and X-band occultation observations (including measurements of Doppler frequency perturbations) obtained during the Voyager 2 encounter with Uranus in January 1986. The data are presented in extensive tables and graphs and characterized in detail. The atmosphere is assumed to have an H2/He abundance ratio of about 85/15, but also to contain small amounts of CH4 at above-cloud relative humidity 30 percent, cloud-base relative humidity 78 percent, and below-cloud mixing ratio 2.3 percent by number density. Other parameters estimated include magnetic-field rotation period 17.24 h, 1-bar equatorial radius 25,559 + or - 4 km, polar radius 24,973 + or - 20 km, equatorial acceleration of gravity 8.69 + or - 0.01 m/sec sq, and atmospheric temperature 76 + or - 2 K (assuming 85 + or - 3 percent H2).

Lindal, G. F.↗

NASA NTRS1988

The roles of dry convection, cloud-radiation feedback processes and the influence of recent improvements in the parameterization of convection in the GLA GCM

The Goddard Laboratory for Atmospheres GCM is used to study the sensitivity of the simulated July circulation to modifications in the parameterization of dry and moist convection, evaporation from falling raindrops, and cloud-radiation interaction. It is shown that the Arakawa-Schubert (1974) cumulus parameterization and a more realistic dry convective mixing calculation yielded a better intertropical convergence zone over North Africa than the previous convection scheme. It is found that the physical mechanism for the improvement was the upward mixing of PBL moisture by vigorous dry convective mixing. A modified rain-evaporation parameterization which accounts for raindrop size distribution, the atmospheric relative humidity, and a typical spatial rainfall intensity distribution for convective rain was developed and implemented. This scheme led to major improvements in the monthly mean vertical profiles of relative humidity and temperature, convective and large-scale cloudiness, rainfall distributions, and mean relative humidity in the PBL.

Sud, Y.↗

DOE OSTI2024

Insights into Sustainable Nitrogen Fixation by Gas-phase Spectroscopic Measurements and Global Modeling of Reaction Intermediates in Humid Nitrogen Plasma

In this article, there is growing interest in reacting molecular nitrogen and water to sustainably synthesize fixed forms of nitrogen such as ammonia. In particular, low-temperature plasmas can activate these relatively inert feedstocks at or near room temperature without a catalyst. However, because of the enhanced reactivity and nonequilibrium chemistry, a diverse range of products is formed, and the underlying reaction mechanisms are exceedingly complex. In this work, we studied a simplified reactor consisting of a gaseous plasma containing controlled mixtures of nitrogen gas and water vapor. Densities of key chemical species such as N, H, OH, NH, and NO were measured by emission and laser-based spectroscopy as a function of the relative humidity. A global model was constructed and the reaction network was validated by comparing calculated species densities with experiments. We discover that N, a key initial intermediate for ammonia, strongly decreases in the presence of water vapor, and as a result, ammonia formation becomes limited at high relative humidity. This decrease is surprisingly not because N itself reacts, but because one of its main sources, an excited molecular nitrogen state, is reacted away. In addition, oxidation pathways for nitrogen, which lead to NO and related products, are found to be favored over reduction pathways because the corresponding reverse reactions are less significant. Together, this understanding helps explain previously reported observations of selectivity toward nitrogen oxides over ammonia, particularly at higher relative humidities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1995

Tropospheric Lapse Rate and Methane on Titan

We have reanalyzed the Voyager radio occultation data for Titan with two alternative approaches to methane condensation. In one approach, methane condensation is enhanced by the presence of nitrogen. In the other approach, methane condensation does not occur. As pointed out by Thompson, nitrogen lowers the condensation level for a methane/nitrogen Mixture and we find that the upper limit on surface relative humidity of methane obtained from the Voyager occultation data is lowered from 0.7 to 0.6. However, 140% supersaturation of methane in the troposphere, suggested by Courtin et al., allows all surface humidities to be consistent with the Voyager occultation data and the upper limit is set by other considerations. We conclude that if supersaturation is not included then the surface relative humidity of methane is between 0.08 and 0.6, with values close to 0.6 indicated. If supersaturation is included then the surface relative humidity of methane is between 0.08 and 0.85, again, with values close to 0.6 indicated. The tropospheric lapse rate on Titan appears to be determined by radiative equilibrium. It is everywhere stable against dry convection but is unstable to moist convection. This is consistent with a supersaturated atmosphere in which condensation - and hence moist convection - is inhibited. The absence of dry convection in the troposphere of Titan can be explained by a simple grey model which shows that the radiative profile of any gas for which the ratio of the gas constant to the specific heat at constant pressure is greater than 0.25 never becomes unstable to dry convection.

McKay, C. P.↗

DOE OSTI2020

Determining Proton Transport in Pseudo Catalyst Layers Using Hydrogen Pump DC and AC Techniques

Optimizing electrode morphology with a more uniform ionomer distribution is key to reducing ohmic losses and increasing electrocatalyst utilization in polymer electrolyte fuel cells (PEFCs). Inherent ionomer conductivity, volume fraction and tortuosity determine effective ionic conductivity. We use hydrogen pump (HP) method to measure effective ionic conductivity of a pseudo catalyst layer (PCL) comprised of Vulcan XC-72 carbon black and 3M 825 EW ionomer with ionomer to carbon (I/C) ratios of 0.6, 1 and 1.4 and relative humidity (RH) range of 50 to 120%. These direct current (DC) experiments are then compared with electrochemical impedance spectroscopy (EIS). Both DC and EIS methods show good agreement, indicating that EIS can be used as an alternative to DC method in HP experiment. Ionic conductivity for PCL with I/C of 1 and 1.4 was found to be about one order of magnitude higher than I/C of 0.6 for most of the RH range. At 90% RH tortuosities for I/C = 1 and 1.4 were close to 1, whereas tortuosity for I/C = 0.6 was 3. With decrease in relative humidity tortuosities increased linearly and at 50% relative humidity a PCL with I/C = 0.6 had the highest tortuosity of 6.1.

25 ENERGY STORAGE↗

NASA NTRS2012

Constraints on the Profiles of Total Water PDF in AGCMs from AIRS and a High-Resolution Model

Atmospheric general circulation model (AGCM) cloud parameterizations generally include an assumption about the subgrid-scale probability distribution function (PDF) of total water and its vertical profile. In the present study, the Atmospheric Infrared Sounder (AIRS) monthly-mean cloud amount and relative humidity fields are used to compute a proxy for the second moment of an AGCM total water PDF called the RH01 diagnostic, which is the AIRS mean relative humidity for cloud fractions of 0.1 or less. The dependence of the second moment on horizontal grid resolution is analyzed using results from a high-resolution global model simulation.The AIRS-derived RH01 diagnostic is generally larger near the surface than aloft, indicating a narrower PDF near the surface, and varies with the type of underlying surface. High-resolution model results show that the vertical structure of profiles of the AGCM PDF second moment is unchanged as the grid resolution changes from 200 to 100 to 50 km, and that the second-moment profiles shift toward higher values with decreasing grid spacing.Several Goddard Earth Observing System, version 5 (GEOS-5), AGCM simulations were performed with several choices for the profile of the PDF second moment. The resulting cloud and relative humidity fields were shown to be quite sensitive to the prescribed profile, and the use of a profile based on the AIRS-derived proxy results in improvements relative to observational estimates. The AIRS-guided total water PDF profiles, including their dependence on underlying surface type and on horizontal resolution, have been implemented in the version of the GEOS-5 AGCM used for publicly released simulations.

Molod, Andrea↗

DOE OSTI2025

Nearby Sites Show Similar Upwind Sources and Differing Semivolatile Concentrations in Coastal Aerosol Particles

The Eastern Pacific Cloud Aerosol Precipitation Experiment (EPCAPE) characterized aerosol composition using measurements at two sites within 3 km (Scripps Pier and Mt. Soledad) from 15 February 2023 to 14 February 2024. Comparing the two sites shows the strong influence of upwind sources that results in similar monthly compositions at both sites. The seasonal changes in chemical mass concentrations were largely driven by the upwind source regions, with coastal northwesterly back-trajectories occurring 63−65% of the year and bringing submicrometer mass concentrations that were lower than the EPCAPE average for all trajectories at each site. In contrast, refractory black carbon (rBC) and nonrefractory (NR)-organics and nitrate mass concentrations exceeded EPCAPE average concentrations for back-trajectories from urban areas such as Los Angeles-Long Beach. For hourly measurements, NR-organics and non-sea-salt (NSS)-sulfate mass concentrations at Mt. Soledad were correlated strongly (r = 0.73−0.82) to those measured at Scripps Pier, but NR-nitrate was correlated only moderately (r = 0.63). The explanation for the lower correlation of NR-nitrate is both emissions between the sites and semivolatility, with semivolatility accounting for site-to-site changes in daily averages of +0.01 μg m −3 per percentage site-to-site difference in relative humidity and −0.07 μg m −3 per degree Celsius site-to-site difference in temperature. On average, comparing Scripps Pier to Mt. Soledad, NR-nitrate was higher by 29% because of relative humidity and lower by −26% because of temperature. NR-nitrate and rBC mass concentrations at Scripps Pier for nighttime were 13−15% higher than those for daytime because land breezes brought higher inland concentrations. Concentrations of rBC were 52% higher at Mt. Soledad than those measured at Scripps Pier, accompanied by increases in tracers for brake wear because of traffic on the steep roads within 10 m of that site. The implications are that these nearby sites had comparable monthly concentrations of measured components due to their similar backtrajectories, but hourly and daily concentration differences supported quantification of the meteorological effects from relative humidity and temperature on semivolatile NR-nitrate as well as minor differences from land−sea breezes and local emissions.

Aerosols↗

NASA NTRS1975

Semiconducting polymers for gas detection

Conjugated polyenes, and polyesters containing phthalocyanine in their backbone, were synthesized. These polymers were characterized by chemical analysis, thermogravimetric analysis, spectral analysis, and X-ray diffraction studies for crystallinity, as well as for their film-forming capability and gas/polymer interactions. Most of the polymers were relatively insensitive to water vapor up to 50 percent relative humidity, but the polyester/phthalocyanine (iron) polymer was relatively insensitive up to 100 percent RH. On the other hand, poly(p-dimethylaminophenylacetylene) was too conductive at 100 percent RH. Of the gases tested, the only ones that gave any evidence of interacting with the polymers were SO2, NOx, HCN and NH3. Poly(imidazole)/thiophene responded to each of these gases at all relative humidities, while the other polymers gave varying response, depending upon the RH. Thus, since most of these gases were electron-accepting, the electron-donating character of poly(imidazole)/thiophene substantiates the concept of electronegativity being the operating principle for interaction effects. Of the six polymers prepared, poly(imidazole)/thiophene first showed a very good response to smoldering cotton, but it later became nonresponsive; presumably due to oxidation effects.

Byrd, N. R.↗

NASA NTRS1979

Satellite monitoring of sea surface pollution

The author has identified the following significant results. Image processing techniques developed are well adapted to the exploration and isolation of local areas which exhibit small temperature differences between themselves and their surroundings. In the worst case of imagery of small areal extent of sea surface having no coastal boundary in the area, there is yet no method of distinguishing unambiguously an oil spill from fog, cloud, the effect produced by shallow sediments, or the effects of naturally occuring thermal fronts. In the case of uniform slicks of liquid North Sea oil in still air, laboratory simulation experiments show that, for oil thicknesses in excess of 1 or 2 mm, there is, under equilibrium conditions, little dependence of oil surface temperature on the thickness of the oil layer. The surface temperature of oil is consistently higher than that of water, the difference being about 1 K at low values of relative humidity, but tending to increase as the relative humidity increases.

Fielder, G.↗

DOE OSTI2025

Brittle-to-Ductile Transitions of Polyelectrolyte Complexes: Humidity, Temperature, and Salt

Polyelectrolyte complexation is an entropically driven, associative phase separation that results in a polymer-rich polyelectrolyte complex (PEC) and a polymer-poor supernatant. PECs show promise as a new class of sustainable materials since they can be processed using aqueous solutions rather than organic solvents. Previous reports have looked at the mechanical properties and glass transitions of PECs as a function of temperature, relative humidity (rH), and salt concentration (CS), but establishing a universal understanding of how these parameters affect PEC mechanics has yet to be achieved. We examined the effects of temperature, rH, and CS on the mechanical properties of PECs formed from poly(methacrylic acid) and poly(trimethyl aminoethyl methacrylate) with a goal of establishing design rules for their mechanical response. Relative humidity was shown to have the most dramatic effect on the mechanical properties, with temperature and salt concentration having far less of an impact. Furthermore, we observed that the glass transition of PECs is tied to both temperature and relative humidity, creating a glass transition rH g /T g line that can be modulated by added salt. Finally, we looked at the thermodynamics behind the glass transition of PECs, which yielded similar energies as the condensation of water. Here, we propose the use of water and/or salt as a low energy and efficient method of processing PECs for various applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

High protonic resistance of hydrocarbon-based cathodes in PEM fuel cells under low humidity conditions: Origin, implication, and mitigation

Hydrocarbon-based electrodes for proton-exchange membrane fuel cells face challenges in closing the performance gap with electrodes based on perfluorosulfonic acid ionomers, particularly under low humidity conditions. Alongside increased oxygen transport resistance and higher kinetic-induced overpotentials, the protonic resistance of these fluorine-free electrodes is the primary hurdle to improved performance. This study systematically investigates the origin and impact of the cathode protonic resistance on fuel cell performance, utilizing sulfonated phenylated polyphenylenes as hydrocarbon ionomers. Electrochemical characterization at low relative humidity (≤50 %) reveal a high protonic resistance arising from both lower conductivity of the hydrocarbon thin film compared to the bulk membrane and increased cathode tortuosity at a gas transport-optimized ionomer to carbon (I/C) ratio of 0.2. The poor protonic resistance at low relative humidities leads to a non-homogeneous current distribution across the thickness of the cathode electrode, resulting in lower catalyst utilization. To address this issue, reducing the thickness of the cathode CL while maintaining a constant Pt loading (i.e., increasing the Pt on carbon ratio) significantly reduces protonic resistance. This improvement compensates for the kinetic disadvantages of highly loaded carbon particles and results in a considerable performance increase by 40 % at 0.75 V under low relative humidities.

25 ENERGY STORAGE↗

DOE OSTI2022

Environmental controls on simulated deep moist convection initiation occurring during RELAMPAGO-CACTI

This study synthesizes the results of 13 high-resolution simulations of deep convective updrafts forming over idealized terrain using environments observed during the RELAMPAGO and CACTI field projects. Using composite soundings from multiple observed cases, and variations upon them, we explore the sensitivity of updraft properties (e.g., size, buoyancy, and vertical pressure gradient forces) to influences of environmental relative humidity, wind shear, and mesoscale orographic forcing that support or suppress deep convection initiation (CI). Emphasis is placed on differentiating physical processes affecting the development of updrafts (e.g., entrainment-driven dilution of updrafts) in environments typifying observed successful and null (i.e., no CI despite affirmative operational forecasts) CI events. Thermally-induced mesoscale orographic lift favors the production of deep updrafts originating from ~1–2-km-wide boundary layer thermals. Simulations without terrain forcing required much larger ( ~5-km-wide) thermals to yield precipitating convection. CI outcome was quite sensitive to environmental relative humidity; updrafts with increased buoyancy, depth, and intensity thrived in otherwise inhospitable environments by simply increasing the free tropospheric relative humidity. This implicates the entrainment of free-tropospheric air into updrafts as a prominent governor of CI, consistent with previous studies. Sensitivity of CI to the environmental wind is manifested by: 1) low-level flow affecting the strength and depth of mesoscale convergence along the terrain, and 2) clouds encountering updraft-suppressing pressure gradient forces while interacting with vertical wind shear in the free-troposphere. Among the ensemble of thermals occurring in each simulation, the widest deep updrafts in each simulation were the most sensitive to environmental influences.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1983

Tribological measurements on a Charnley-type artificial hip joint

A total hip simulator was used to determine the friction and wear properties of Charnley-type (316L stainless steel balls and sterile ultrahigh molecular weight polyethylene cups) hip prostheses. Three different sets of specimens were tested to 395,000, 101,500 and 233,000 walking cycles, respectively. All tests were run unlubricated, at ambient conditions (22 to 26 C, 30 to 50 percent relative humidity), at 30 walking cycles per minute, under a dynamic load simulating walking. Polyethylene cup wear rates ranged from 1.4 to 39 ten billions cu m which corresponds to dimensional losses of 4.0 to 11 microns per year. Although these wear rates are lower than those obtained from other hip simulators and from in vivo X-ray measurements, they are comparable when taking run-in and plastic deformation into account. Maximum tangential friction forces ranged from 93 to 129 N under variable load (267 to 3090 N range) and from 93 to 143 N under a static load of 3090 N. A portion of one test 250,000 walking cycles) run under dry air ( 1 percent relative humidity) yielded a wear rate almost 6 times greater than that obtained under wet air ( 70 percent relative humidity) conditions.

Jones, W. R., Jr.↗

DOE OSTI2026

Employing Machine Learning for New Particle Formation Identification and Mechanistic Analysis: Insights From a Six‐Year Observational Study in the Southern Great Plains

We present a supervised machine learning (ML) framework to automatically identify new particle formation (NPF) events and analyze key atmospheric factors associated with their occurrence and growth. We applied ML to detect NPF events using start time and particle concentrations across size ranges, while identifying atmospheric variables including ambient temperature, relative humidity, solar radiation intensity (SRI), wind speed, wind direction, boundary layer height, total organics, sulfate, nitrate, total surface area concentration, sulfur dioxide, and turbulent kinetic energy (TKE). We analyzed a 6-year data set from the Atmospheric Radiation Measurement at the Southern Great Plains (SGP) site in Oklahoma, USA. Using long-term ground-based measurements, we identified NPF events and applied Random Forest Classifiers, which achieved 90%–95% prediction accuracy. Feature importance analysis highlighted SRI, relative humidity, and ambient temperature as the most influential variables, contributing normalized importances of 28%, 17%, and 10%. Partial Dependence Plots (PDPs) indicated that higher SRI and lower relative humidity were critical in promoting NPF formation at SGP. Seasonally, NPF events were more frequent in winter (42.1%) and spring (35.5%), and least in summer (4.0%). Particle growth rates also exhibited a seasonal variation, with the lowest in winter (below 2 nm hr −1 ) and highest in late spring and early summer (exceeding 5 nm hr −1 ). Temperature, turbulent kinetic energy, and aerosol properties were the primary factors of growth rate variability. This study advances predictive modeling of NPF, offers insights for future campaign deployments, and demonstrates the effectiveness of ML in understanding the formation and growth of atmospheric aerosols.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Lawrence Berkley National Laboratory Building 59

The building management system in Building 59 is monitoring and archiving building-level electricity usage, HVAC and lighting system states (e.g., setpoint, temperature, flow rate, pressure), indoor environmental conditions (air temperature, relative humidity, CO2), on-site weather (air temperature, relative humidity), and especially occupant counts as well as other metrics such as Wi-Fi signal. This dataset could support multiple use cases, such as model predictive control and occupant related demand management.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2021

Lawrence Berkley National Laboratory Building 59 (Raw)

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2021

Lawrence Berkeley National Lab Building 59

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗