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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Material Failure Mechanisms of Alkaline Zn Rechargeable Conversion Electrodes

Zinc (Zn) alkaline electrodes hold great importance and promise in the battery technology community, yet their behavior in real-world applications is still poorly understood. Here, we report a study of failure mechanisms and material evolution during cycling of 27 zinc–manganese dioxide (Zn–MnO 2 ) cells wherein the percent utilization of the Zn electroactive material is systematically varied between 1 and 16%. Cell fabrication is kept typical of the prevailing industrial cell design. The cycle life ranges from 2800 to 60, depending inversely on the Zn utilization. In all cases, the Zn material microstructure sheds the polytetrafluoroethylene (PTFE) binder and forms zinc oxide (ZnO) rods, with longer rods formed by lower current per Zn mass. Irreversible side reactions such as the hydrogen evolution reaction (HER), short circuits, or gas crossover cause the Zn anode’s charging efficiency to average 92% (as low as 86%), which in turn causes the baseload of metallic Zn to gradually disappear. Cell failure occurs after the baseload of metallic Zn is exhausted. The total lifetime discharge capacity remains constant near 12 ± 5 Ah/g Zn invariant of Zn utilization, which suggests that the aforementioned processes of Zn microstructural evolution and side-reaction destruction of baseload metallic zinc both progress linearly with cell capacity throughput. Manual reproduction of individual Zn failure mechanisms is performed in 22 fresh cells. Tight packing of the microstructure can lead to poor mass transfer, which causes supersaturation of soluble Zn and finally produces a high overvoltage during discharge. Here, the low charging current density yields poor coulombic efficiency due either to the competitive HER or soft short circuits.

25 ENERGY STORAGE↗
DOE OSTI2024

First-Principles Study on the Role of Cu and Cl-Based Dopants in NiO

Utilization of wide band gap oxide-based materials in thin-film solar energy technologies has increased in recent years. Among the numerous candidate oxide materials, NiO has shown many desirable optoelectronic properties that are applicable to thin-film PV technologies such as cadmium telluride PV. However, one critical factor requiring further investigation is the p-type doping behavior of NiO, specifically when the cadmium telluride solar cell undergoes conventional processes such as copper doping and chlorine-based activation treatment. The previous literature has shown a large degree of variability in hole concentrations in NiO when copper is used as the primary dopant. This study uses first-principles computational modeling based on density functional theory coupled with defect equilibria calculations to quantitatively explore the role of copper and chlorine-based extrinsic dopants in the p-type doping activity of NiO. The study reveals the importance of extrinsic dopants and their binding interactions with nickel vacancies to effectively p-dope NiO. It is suggested that both the formation of V Ni + Cu Ni and V Ni + Cl O defect pairs under a supersaturated state of NiO are potential mechanisms for increasing hole densities. On the other hand, the production of 2Cu Ni severely limits the effectiveness of p-doping in NiO, even in the presence of the aforementioned defect pairs. Furthermore, the study provides a guideline for experimentalists interested in using copper or chlorine species to understand how to controllably p-dope NiO during thin-film synthesis.

chlorine↗
DOE OSTI2021

Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films

Perovskite solar cells have received substantial attention due to their potential for low-cost photovoltaic devices on flexible or rigid substrates. Thiocyanate (SCN)-containing additives, such as MASCN (MA = methylammonium), have been shown to control perovskite film crystallization and the film microstructure to achieve effective room-temperature perovskite absorber processing. Nevertheless, the crystallization pathways and mechanisms of perovskite formation involved in MASCN additive processing are far from clear. Using in situ X-ray diffraction and photoluminescence, we investigate the crystallization pathways of MAPbI 3 and reveal the mechanisms of additive-assisted perovskite formation during spin coating and subsequent N 2 drying. In this work, we confirm that MASCN induces large precursor aggregates in solution and, during spin coating, promotes the formation of the perovskite phase with lower nucleation density and overall larger initial nuclei size, which forms upon reaching supersaturation in solution, in addition to intermediate solvent-complex phases. Finally, during the subsequent N 2 drying, MASCN facilitates the dissociation of these precursor aggregates and the solvate phases, leading to further growth of the perovskite crystals. Our results show that the nature of the intermediate phases and their formation/dissociation kinetics determine the nucleation and growth of the perovskite phase, which subsequently impact the film microstructure. These findings provide mechanistic insights underlying room-temperature, additive-assisted perovskite processing and help guide further development of such facile room-temperature synthesis routes.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nucleation Rate Theory for Coordination Number: Elucidating Water-Mediated Formation of a Zigzag Na 2 SO 4 Morphology

Predicting and controlling nanostructure formation during nucleation can pave the way to synthesizing novel energy materials via crystallization. However, such control over nucleation and crystallization remains challenging due to an inadequate understanding of critical factors that govern evolving atomistic structures and dynamics. Here, in this paper, we utilize coordination number as a reaction coordinate and rate theory to investigate how sodium sulfate, commonly known as a phase-change energy material, nucleates in a supersaturated aqueous solution. In conjunction with ab initio and force field-based molecular dynamics simulation, the rate theoretical analysis reveals that sodium sulfate from an initially dissolved metastable state transits to a heterogeneous mixture of prenucleated clusters and finally to a large cylindrical zigzag morphology. Measurements of Raman spectra and their ab initio modeling confirm that this nucleated morphology contains a few waters for every sulfate. Rate processes such as solvent exchange and desolvation exhibit high sensitivity to the evolving prenucleation/nucleation structures, providing a means to distinguish between critical nucleation precursors. Desolvation and forming the first-shell interionic coordination structure via monomer-by-monomer addition around sulfates are found to explain the formation of large nuclei. Thus, a detailed understanding of the step-by-step structure formation across scales has been achieved. This can be leveraged to predict nucleation-related structures and dynamics and potentially control the synthesis of novel phase-change materials for energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Uptake of Pb and the Formation of Mixed (Ba,Pb)SO 4 Monolayers on Barite During Cyclic Exposure to Lead-Containing Sulfuric Acid

Barite (BaSO 4 ) is a common additive in lead-acid batteries, where it acts as a nucleating agent to promote the reversible formation and dissolution of PbSO 4 during battery cycling. However, little is known about the molecular-scale mechanisms the nucleation and cyclic evolution of PbSO 4 over a battery’s lifetime. In this study, we explore the responses of a barite (001) surface to cycles of high and low lead concentrations in the presence of 100 mM sulfuric acid using in-situ atomic force microscopy and high-resolution X-ray reflectivity. Here we find that PbSO 4 epitaxial films readily nucleate on the barite surface, even from solutions that are undersaturated relative to bulk PbSO 4 . Despite this, barite (001) proves to be an ineffective nucleator of bulk PbSO 4 , as multilayer growth is suppressed even in highly supersaturated solutions. Instead, we find evidence that Pb 2+ ions can directly exchange with Ba 2+ to create mixed (Ba,Pb)SO 4 surfaces. These chemically mixed surfaces do not host PbSO4 monolayers as readily as pristine barite, and the original reactivity is not regained until a fresh surface is reestablished by aggressive etching. Our results can be partly explained by traditional models of Stranski-Krastanov (S-K) growth, in which monolayer films are stabilized by a reduction in surface energy, but multilayer growth is inhibited by epitaxial strain. Complementary density functional theory calculations confirmed the basic energetic-terms of traditional S-K models, but also showed evidence form more complex, thickness-dependent, energetics than would be predicted from the S-K models. The experimental results can be better understood by extending the S-K model to consider the formation of mixed surfaces and films, which can have reduced strain and interfacial energies relative to pure films, while also being stabilized by entropy of mixing. These insights into non-stoichiometric heteroepitaxy will enable better predictions of how barite affects PbSO 4 nucleation in battery environments.

25 ENERGY STORAGE↗
DOE OSTI2020

Crystal Growth, Single Crystal Structure, and Biological Activity of Thiazolo-Pyridine Dicarboxylic Acid Derivatives

Four novel TPDCA derivatives were prepared via a supersaturation method combining TPDCA with water, N-methyl-2-pyrrolidone (NMP), Na(PO 2 H 2 ), and ammonia solution: 2(C 9 H 7 NO 5 S)H 2 O (1), (C 9 H 7 NO 5 S)C 5 H 9 NO (2), (C 9 H 7 NO 5 S)Na(PO 2 H 2 ) (3), and (C 9 H 5 NO 5 S)(NH 4 )2(H 2 O) (4). Their crystal structures were determined by single-crystal X-ray diffraction. Compounds (1) and (2) crystallize in the monoclinic space groups P2 1 and P2 1 /c, respectively, whereas compounds (3) and (4) crystallize in the triclinic space group P1 - . Weak and moderate hydrogen bonds were detected in the four compounds. In the biological tests, (1) and (3) exhibited significant antibacterial activity against Escherichia coli and Staphylococcus aureus; in addition, (1) was cytotoxic against leukemia HL-60 cells with the IC 50 value of 158.5 ± 12.5 μM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Density Measurements of Molten LiF–BeF 2 and LiF–BeF 2 –LaF 3 Salt Mixtures by Neutron Radiography

The densities of eutectic (LiF) 2 –BeF 2 and mixtures of this salt (FLiBe) with LaF 3 were measured by dilatometry and by neutron attenuation from 673 K to 1,073 K. Because LaF 3 has a limited solubility in FLiBe, it was necessary to determine the amount of LaF 3 in solution before the density could be determined. The FLiBe density determination was favorably benchmarked against the literature data. A simple comparison was not available for the LaF 3 –FLiBe mixtures, so extrapolation of published data was necessary based on analysis using the Molten Salt Thermal Properties Database-Thermochemistry, or MSTDB-TC, developed by the US Department of Energy. Solubilities for LaF 3 in FLiBe ranged from 1 to 4 mol % over 673 to 1,073 K. The salt system was heated and cooled over 24 h to evaluate potential changes in composition and hysteresis during the measurement. Changes in the meniscus were observed, and these were included in the correction for density determinations. Salt surface tension may have led to supersaturation of LaF 3 in the salt because the solubility curve was nonlinear with respect to the inverse temperature, as would be expected for an ideal system. Surface tension measurements are currently underway to test this hypothesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Experimental Investigation of Uranium and Iron Condensation from High-Temperature Plasma Conditions

We used a plasma flow reactor (PFR) to generate synthetic fallout nanoparticles from vapor-phase condensation of two different input concentrations of uranium and iron analytes (U/Fe = 1:1 and 1:2). Synthetic fallout from complex chemical matrices (e.g., mixtures of U and Fe) has not been generated in this setup before and allows for the observation of relative condensation and fractionation of nuclear debris. Experiments were conducted under two different temperature histories with variations in particle flow patterns along the PFR. Transmission electron microscopy (TEM) observation and analysis of the nanoparticles revealed variations in speciation of uranium oxides (UO 2 and α-UO 3 ) depending on the competition between flow mixing and oxygen sequestration by iron. A ternary metal oxide, UFeO 4 , was observed in addition to iron oxides (e.g., FeO and Fe 3 O 4 ), which suggests that fallout models should account for chemical speciation of ternary metal oxides (i.e., UFeO 4 ) and their relative condensation behaviors in addition to those of singular metal oxides (e.g., FeO and UO 2 ). X-ray Energy Dispersive Spectroscopy (EDS) elemental maps showed that some particles had Fe-rich cores surrounded by U-rich regions. This suggests that either condensed U oxides coagulate onto molten Fe oxides or that the increase in iron analyte concentration might drive the system toward a higher degree of supersaturation, leading to earlier formation of iron oxide particles and providing an energetically favored pathway for nucleation of uranium oxides around iron oxide particles.

and nuclear chemistry↗
DOE OSTI2024

Concerted Formation of Reversibly Precipitated Sulfur Species and Its Importance for Lean Electrolyte Lithium–Sulfur Batteries

Achieving high energy densities for lithium-sulfur batteries remain elusive. Largely limited by the volume of electrolyte used, lean electrolyte conditions (electrolyte/sulfur mass ratio <3) present enormous challenges that have led to very poor specific capacity and rate performance. Previous studies have identified that the high concentration of polysulfide is responsible for the poor discharge voltage. However, there still lacks sufficient understanding of the processes occurring at lean electrolyte conditions. Here, in this work we uncovered a polysulfide concentration regulating mechanism that operates through the precipitation and redissolution of solid sulfur-based species (reversibly precipitated sulfur species, RPSS). This occurs in a concerted manner in a global sense through the cathode and can be measured using impedance spectroscopy. It was found that the more RPSS that is formed, the higher the energy density of discharge. We propose that high concentration of polysulfide tends to supersaturate, which impeded the formation of RPSS. Employing an electrolyte with low Li ion concentration along with using poorly dissociating lithium salts allowed for more RPSS formation and ultimately enabled discharge at >2.0 V at 0.05 C, at E/S = 2.5, and at room temperature without the use of an engineered cathode.

25 ENERGY STORAGE↗
DOE OSTI2020

Impacts of Aerosol and Environmental Conditions on Maritime and Continental Deep Convective Systems Using a Bin Microphysical Model

A series of model simulations were conducted to investigate the effects of cloud condensation nuclei (CCN) loading and convective available potential energy (CAPE) on tropical maritime and midlatitude continental deep convection. Dynamical downscaling from global aerosol reanalysis was used to represent aerosol fields for the two convective regimes. We describe a control run and multiple sensitivity experiments using a limited-area model, employing spectral-bin cloud microphysics. The CCN loading is perturbed between the target maritime and continental conditions, roughly 40–2,000 cm -3 at 850 hPa and 1% supersaturation. Surface precipitation rates monotonically increase with increasing CCN loading for both the maritime and continental situations, while these monotonic increases are disrupted in the simulations with reduced CAPE. The increase in precipitation is in the form of convective precipitation, at the expense of stratiform precipitation. CCN increases promote increases in supercooled cloud water, in agreement with previous modeling studies. However, in the simulations investigated herein, the changes in supercooled water have different impacts on the cloud microphysics in the maritime and continental simulations. Increased supercooled water contents lead to more hail and less graupel in the continental simulation. For the maritime simulation, enhanced supercooled cloud water contents promote an increase in graupel since little or no hail is produced. This distinction is due to the difference in relative magnitudes and peak altitudes of supercooled water and snow amounts, which is further attributable to moisture and dynamical differences in the two cases.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Development and Evaluation of Chemistry‐Aerosol‐Climate Model CAM5‐Chem‐MAM7‐MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol

Abstract An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m −2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m −2 . Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m −2 . Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m −2 .

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Invigoration or Enervation of Convective Clouds by Aerosols?

Are convective clouds strengthened by the addition of aerosol particles? We present new theoretical calculations which starkly contrast previous results. Prior foundational work suggested that aerosols strongly invigorate convective cloud updrafts via changes to cold-phase processes. We show that the peak magnitude of invigoration by this mechanism is substantially reduced for cold-based storms. For warm-based storms, the updrafts are weakened, not strengthened, by aerosol-induced changes to cold-phase processes. Our calculations show that if invigoration occurs, it is driven primarily by changes to warm-phase processes and may be largest well before the storm reaches maturity. The calculations are based on a new formulation of the moist adiabatic lapse rate that accounts for freezing, supersaturation, and condensate loading. The results significantly reshape our understanding of the impact of aerosols on convective updrafts.

58 GEOSCIENCES↗
DOE OSTI2021

The NPF Effect on CCN Number Concentrations: A Review and Re-Evaluation of Observations From 35 Sites Worldwide

The new particle formation (NPF) effect on cloud condensation nuclei (CCN) differs from region to region and remains highly uncertain. In this work, we re-evaluate the NPF-initiated enhancements in CCN number concentrations (E_N CCN ) by compiling results from 35 field sites worldwide and five global models. We show the E_N CCN at sites close to the anthropogenic sources are more than 2-fold as large as that at remote sites with supersaturations of 0.1%–1.0%. The enhancements anti-correlate with the time scales for the new particles to grow to CCN size, which are 5–10 and 20–30 hr at polluted and remote sites, respectively. We further reveal that under polluted environments the condensational growth of new particles may be accelerated, leading to larger E_N CCN . The models fail to simulate the E_NCCN in polluted regions. Our study highlights the importance of parameterizing the time scale of NPF to affect CCN differently for remote and polluted regions in models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Remote Sensing of Electric Fields Observed Within Winter Precipitation During the 2020 Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Snowstorms (IMPACTS) Field Campaign

Aircraft electric fields from NASA's Lightning Instrument Package (LIP) were coupled with other airborne and ground-based, and in situ measurements to understand electrification in winter clouds that did not produce lightning. The measurements were made during seven research flights by a NASA ER-2 during the 2020 Investigation of Microphysics and Precipitation for Atlantic Coast-Threatening Snowstorms (IMPACTS) campaign. Observed total electric field magnitudes were as high as 80 V m -1 and variability in the electric field was observed along the flight path of the ER-2, indicating horizontal and/or vertical inhomogeneity in the cloud's electrical structure. X-band airborne radar data indicated 20-dBZ echo tops above 5 km in regions where electrification exceeded 10 V m -1 . In these regions, 85-GHz brightness temperatures (TB) from an airborne radiometer were lower than 265 K, with the lowest T B (~210 K) associated with ice scattering collocated with the strongest electric fields. In situ microphysical measurements from the NASA P-3 aircraft on February 7 indicated that regions near strong electric field contained supercooled water, rimed ice hydrometeors, ice water p- content as high as 1 g m -3 , liquid water content as high as 0.15 g m -3 , and supersaturation as high as 3.5%. Furthermore, these observations support the role of mixed phase microphysics in the generation of electric fields in clouds. In three case studies, ground based S-band polarimetric radar observed depolarization streaks in differential reflectivity near areas where the strongest electrification was observed. This observation reinforces the utility of depolarization streaks to identify areas of electrification prior to lightning occurrence.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Microphysical Piggybacking in the Weather Research and Forecasting Model

Abstract This paper presents incorporation of the microphysical piggybacking into the Weather Research and Forecasting (WRF) model. Microphysical piggybacking is to run a single simulation applying two microphysical schemes, the first scheme driving the simulation and the second piggybacking this simulated flow. “Driving the simulation” means that the simulated microphysical processes, affect the cloud buoyancy and thus force the simulated flow. In contrast, the piggybacking variables are advected by the simulated flow and undergo microphysical transformation, but they do not affect the simulated flow (like in prescribed flow—kinematic—simulations). The two sets of variables (driver and piggybacker) include temperature, water vapor mixing ratio, and all microphysical variables. We provide details of implementing piggybacking into the WRF model, illustrate its applications, and demonstrate the benefits of this methodology in two idealized three‐dimensional cases: (a) a squall line case applying two microphysics schemes, the Thompson bulk microphysics scheme and the University of Pécs/NCAR bin (UPNB) scheme. The piggybacking simulations revealed that the microphysics‐dynamics interaction plays a more important role than the pure microphysical size sorting effect in the transition zone formation. (b) A case of daytime shallow‐to‐deep convective development over land. This case uses the UPNB scheme and contrasts convection developing in environments with either pristine or polluted cloud condensation nuclei (CCN). The piggybacking results indicated that the increase of cloud cover and decrease of supersaturation are mainly associated with the microphysical effect of increasing CCN while the change of precipitation on the ground is also influenced by microphysics‐dynamics interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Maritime Aerosol and CCN Profiles Derived From Ship₋Based Measurements Over Eastern North Pacific During MAGIC

Atmospheric aerosols are widely recognized to give rise to a substantial radiative forcing to the climate by scattering and absorbing radiation and by modifying the microphysical, lifetime, and radiative properties of clouds. During the Marine ARM GPCI Investigation of Clouds (MAGIC) over the Eastern North Pacific (ENP), the ship-based measured cloud condensation nuclei (CCN) concentration at 0.2% supersaturation (N CCN,0.2 ) and condensation nuclei concentration (N CN ) had mean values of 116.7 and 219.4 cm ⁻3 , with the highest concentrations found closest to LA due to an increase in aerosol sources. Moving westward, both N CCN,0.2 and N CN gradually decreased until stabilizing near 100 cm ⁻3 and 200 cm ⁻3 , respectively. Using the methods proposed by Ghan and Collins (2004), https://doi.org/10.1175/1520-0426(2004)021<0387:uoisdt>2.0.co;2 and Ghan et al. (2006), https://doi.org/10.1029/2004jd005752, N CCN,0.2 profiles are retrieved using the surface measured N CCN,0.2 as a constraint. For coupled conditions, correlations between the retrieved N CCN,0.2 profiles and cloud-droplet number concentration (N C ) increase from 0.26 at the surface to 0.38 near cloud base, particularly true for non-drizzling clouds. Although the correlations are lower than expected, the percentage increase (46.2%) is encouraging. Finally, the relationships between cloud breakup (CB) and the stratocumulus to cumulus transition (SCT) with environmental conditions and associated aerosols are also studied. The decreased N CN trend east of CB is mainly caused by precipitation scavenging, while the increased N CN trend west of CB is strongly associated with the increased surface wind speed and fewer drizzle events. A further study is needed using high-resolution models to simulate these events.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Formation Process of Particles and Cloud Condensation Nuclei Over the Amazon Rainforest: The Role of Local and Remote New-Particle Formation

Understanding the formation processes of particles and cloud condensation nuclei (CCN) in pristine environments is a major challenge in accurately assessing anthropogenic radiative forcing. Here, using a state-of-the-art model that systematically simulates the chemical processes controlling new-particle formation (NPF) and multi-scale chemical transport, we find that NPF contributes ~90% of the particle number and ~80% of the CCN at 0.5% supersaturation (CCN0.5%) in the pristine Amazon boundary layer during the wet season. The corresponding contributions are only ~30% and ~20% during the dry season because of prevalent biomass burning. In both seasons, about half of the NPF-induced particles and ~85% of the NPF-induced CCN0.5% in the boundary layer originate from the long-range transport of new particles formed hundreds to thousands of kilometers away. Moreover, about 50–65% of the NPF-induced particles and 35–50% of the NPF induced CCN0.5% originate from the downward transport of new particles formed in the free troposphere.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cloud Condensation Nuclei Closure Study Using Airborne Measurements Over the Southern Great Plains

Abstract Airborne measurements of non‐refractory bulk aerosol chemical composition, aerosol size distributions, and cloud condensation nuclei (CCN) were conducted onboard a research aircraft during the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems field campaign in the spring and summer of 2016. A CCN closure study for the entire campaign period was performed where measured CCN concentrations at 0.24% and 0.46% supersaturation were compared with the predicted CCN concentrations calculated using κ ‐Köhler theory, three different assumptions of aerosol mixing state, and various assumptions about hygroscopicity, density, and the insoluble fraction of organic particles. We found that the Closure Ratio (CR), calculated as the ratio of predicted to measured CCN concentrations, was equal to one under two different aerosol mixing state assumptions: (a) all particles are composed of 100% organic particles, and (b) particles are externally mixed and composed of pure sulfates, nitrates, and organic particles assuming hygroscopicity values for organic particles ( ) between 0.04 and 0.17. The use of internal mixing state assumption often led to overprediction of CCN concentrations but the agreement within ±20% with the measured CCN concentrations was observed under certain closure permutations. A similar agreement, that is, within ±20%, was also observed using permuted parameters concerning density (1 and 1.5 g cm −3 ) and an insoluble fraction (0% and 20%) of organic particles. These findings may provide constraints on to predict CCN concentrations at a remote continental Southern Great Plains site.

54 ENVIRONMENTAL SCIENCES↗