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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 883 records · Page 49
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Localized High Concentration Electrolytes for High Voltage Lithium-Metal Batteries: Correlation between the Electrolyte Composition and Its Reductive/Oxidative Stability

We demonstrate a first-principles screening methodology as an effective tool to explore electrolyte formulations for the new generation of high energy density rechargeable batteries. We study the liquid structure and electronic properties in dilute electrolytes, high concentration electrolytes (HCE), and localized high concentration electrolytes (LHCE), with focus on electrolyte formulations based on lithium bis(fluorosulfonyl)imide (LiFSI), dimethyl carbonate (DMC), and bis(2,2,2-trifluoroethyl) ether (BTFE) as a diluent. We describe the solvation complexes in the dilute electrolyte and explore structural changes triggered by the increase in lithium salt concentration for HCEs and the diluent effects in LHCEs. In HCE formulations, there is a 4-fold coordination environment of lithium-ions as in the dilute electrolyte, but the number of lithium-ion interactions with O atoms from FSI- anions dominates. In these solutions, the ability of the FSI- anions to interact with multiple lithium-ions allows complex 3D network formation and influences the reductive/oxidative behavior of the electrolyte. Interestingly, in LHCEs, the BTFE diluent molecules do not change the 3D solution structure when diluting the HCE formulation from 5.49 to 3.83 M. However, there is a composition threshold where the structural and electronic behavior may change. We show that diluting the HCE electrolyte with BTFE down to 1.77 M breaks the three-dimensional solution structure into an island-like solvation complex. We relate these structural changes to the electronic properties of the electrolytes finding a causal relationship between the reductive/oxidative behavior and the lithium-oxygen interaction mechanisms in the solvated complexes. The coordination with lithium-ions lowers the electrolyte LUMO and HOMO levels: the higher is the number of interactions with lithium-ions, the more likely the solvent molecule, FSI- anion, or diluent molecule is to be reduced and the less likely it is to become oxidized. The evolution of the solvated ion structure in HCE and LHCE suggests a close connection to a corresponding change in the lithium-ion transport mechanisms for these electrolytes.

anions, molecules, oxygen, solvents, electrolytes↗
DOE OSTI2020

Dynamics of Cation-Induced Conformational Changes in Nanometer-Sized Uranyl Peroxide Clusters

Conformational changes of the pyrophosphate (Pp)-functionalized uranyl peroxide nanocluster [(UO 2 ) 24 (O 2 ) 24 (P 2 O 7 ) 12 ] 48– ({U 24 Pp 12 }), dissolved as a Li/Na salt, can be induced by the titration of alkali cations into solution. The most symmetric conformer of the molecule has idealized octahedral ( O h ) molecular symmetry. One-dimensional 31 P NMR experiments provide direct evidence that both K + and Rb + ions trigger an O h -to- D 4 h conformational change within {U 24 Pp 12 }. Variable-temperature 31 P NMR experiments conducted on partially titrated {U 24 Pp 12 } systems show an effect on the rates; increased activation enthalpy and entropy for the D 4 h -to- O h transition is observed in the presence of Rb + compared to K + . Two-dimensional, exchange spectroscopy 31 P NMR revealed that magnetization transfer links chemically unique Pp bridges that are present in the D 4 h conformation and that this magnetization transfer occurs via a conformational rearrangement mechanism as the bridges interconvert between two symmetries. The interconversion is triggered by the departure and reentry of K (or Rb) cations out of and into the cavity of the cluster. This rearrangement allows Pp bridges to interconvert without the need to break bonds. Cs ions exhibit unique interactions with {U 24 Pp 12 } clusters and cause only minor changes in the solution 31 P NMR signatures, suggesting that O h symmetry is conserved. Single-crystal X-ray diffraction measurements reveal that the mixed Li/Na/Cs salt adopts D 2 h molecular symmetry, implying that while solvated, this cluster is in equilibrium with a more symmetric form. Thus, these results highlight the unusually flexible nature of the actinide-based {U 24 Pp 12 } and its sensitivity to countercations in solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Paired Simulations and Experimental Investigations into the Calcium-Dependent Conformation of Albumin

Serum albumin is the most abundant protein in blood plasma, and it is involved in multiple biological processes. Serum albumin has recently been adapted for improving biomaterial integration with bone tissue, and studies have shown the importance of this protein in bone repair and regeneration. However, the mechanism of action is not yet clear. In stark contrast, other studies have demonstrated that albumin blocks cell adhesion to surfaces, which is seen as a limitation to its bone healing role. These apparent contradictions suggest that the conformation of albumin facilitates its bioactivity, leading to enhanced bone repair. Serum albumin is known to play a major role in maintaining the calcium ion concentration in blood plasma. Due to the prevalence of calcium at bone repair and regeneration sites, it has been hypothesized that calcium binding to serum albumin triggers a conformational change, leading to bioactivity. In the current study, molecular modeling approaches including molecular docking, atomic molecular dynamics (MD) simulation, and coarse-grained MD simulation were used to test this hypothesis by investigating the conformational changes induced in bovine serum albumin by interaction with calcium ions. The computational results were qualitatively validated with experimental Fourier-transform infrared spectroscopy analysis. We find that free calcium ions in solution transiently bind with the three major loops in albumin, triggering a conformational change where N-terminal and C-terminal domains separate from each other in a partial unfolding process. The separation distance between these domains was found to correlate with the calcium ion concentration. The experimental data support the simulation results showing that albumin has enhanced conformational heterogeneity upon exposure to intermediate levels of calcium, without any significant secondary structure changes.

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

Hydrophilic and Apolar Hydration in Densely Grafted Cationic Brushes and Counterions with Large Mobilities

We employ all-atom molecular dynamics (MD) simulation framework to unravel water microstructure and ion properties for cationic [Poly(2-(methacryloyloxy)ethyl trimethylammonium chloride] (PMETAC) brushes with chloride ions as counterions. First, we identify locally separate water domains (or first hydration shells) each around the {N(CH 3 ) 3 } + and the C=O functional groups of the PMETAC chain and one around the Cl - ion. These first hydration shells around the respective moieties overlap and the extent of the overlap depends on the nature of the species triggering it. Second, despite the overlap, the water molecules in these domains demonstrate disparate properties dictated by the properties of the atoms/groups around which they are located. For example, the presence of the methyl groups make the {N(CH 3 ) 3 } + group trigger apolar hydration as evidenced by the corresponding orientation of the dipole of the water molecules around the {N(CH 3 ) 3 } + moiety. These water molecules around the N(CH 3 ) 3 } + group also have enhanced tetrahedrality as compared to the water molecules constituting the hydration layer around the C=O group and the Cl - counterion. Our simulations also identify that there is an intervening water layer between the Cl - ion and {N(CH 3 ) 3 } + group: this layer prevents the Cl - ion from coming very close to the {N(CH 3 ) 3 } + group. As a consequence, there is a significantly large mobility of the Cl - ions inside the PMETAC brush layer. Furthermore, the C=O group of the PE chain, due to the partial negative charge on the oxygen atom and the specific structure of the PMETAC brush system, demonstrates strongly hydrophilic behavior and enforces a specific dipole response of water molecules analogous to that experienced by water around anionic species of high charge density. As a result, our findings confirm that PMETAC brushes undergo hydrophilic hydration at one site, apolar hydration at another site, and ensures large mobility of the supported Cl- counterions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Photoactivation Transition State and Dynamical Response of the Orange Carotenoid Protein

The orange carotenoid protein (OCP) regulates light harvesting in cyanobacteria by acting as a photoreceptor in its resting form, OCP O , and by effecting the quenching of bilin excitons upon binding to the core of the phycobilisome in its photoactivated red form, OCP R . We show herein using fluorescence anisotropy measurements and the action spectra for the rate constants of the two light-driven steps in the mechanism that the photoactivation of the OCP from Synechocystis sp. PCC 6803 is triggered by excited-state motions of the canthaxanthin chromophore that yield a twisted and bent conformation. Well-tempered metadynamics simulations reveal that a bicycle-pedal configuration, due to twisting of the two adjacent C=C bonds at the C13−C14 and C15−C15′ positions in the center of canthaxanthin’s π-conjugated isoprenoid backbone, can be accommodated by the binding site in the OCP, with the energy of a captured photon required to cross the local activation energy barriers from the dark equilibrium structure. The bicycle-pedal configuration breaks the conserved hydrogen-bonding interactions between the carbonyl substituent of the β-ionone end ring of canthaxanthin and the adjacent W288 and Y201 residues in the C-terminal domain. The action spectra are modulated by the vibronic excitation prepared by absorption transitions to the S 2 state, indicating that the photoactivation reactions are triggered by the canthaxanthin chromophore well prior to vibrational equilibration. These findings show that an ultrafast structural response of the OCP protein to the excited-state motions of the canthaxanthin chromophore controls the photoactivation yield and the sensing of blue light.

Fluorescence↗
DOE OSTI2025

Depolymerization as a Design Strategy: Depolymerization Etching of Polymerization-Induced Microphase Separations

Thermally triggered depolymerization has traditionally been viewed through the lens of sustainability and recycling, not as a constructive tool for materials design. Herein, we show that selective, thermally triggered depolymerization to gaseous monomer serves as a solvent-free strategy for generating porosity in nanostructured polymer materials, offering a means to bypass the mass transport limitations inherent in conventional solution-based etching. As a demonstration platform, we employed polymerization-induced microphase separation (PIMS) to generate disordered bicontinuous block copolymer structures with embedded depolymerizable domains. By incorporating a methacrylate block susceptible to thermal depolymerization within a cross-linked, depolymerization-resistant styrenic matrix, we developed a process we term depolymerization etching of polymerization-induced microphase separations (DEPIMS). This approach enables highly selective and efficient domain removal via reversion to monomer to produce mesoporous materials with high surface areas (>200 m 2 /g). Subsequent surface functionalization yielded mesoporous adsorbents with tunable uptake kinetics and among the highest dye adsorption capacities reported for PIMS-derived materials, demonstrating the adaptability of the DEPIMS platform for chemical separations. DEPIMS can also be extended to a gram-scale, one-pot approach to yield mesoporous materials with recoverable monomer in under 12 h. These findings reposition thermal depolymerization from a sustainability tool to a broadly enabling strategy for scalable, on-demand fabrication of functional nanostructured materials.

Depolymerization↗
DOE OSTI2021

Holes in Optical Lightning Flashes: Identifying Poorly Transmissive Clouds in Lightning Imager Data

Space-based optical lightning sensors including the lightning imaging sensor (LIS) and geostationary lightning mapper (GLM) are pixelated imagers that detect lightning as transient increases in cloud top illumination. Detection requires optical emissions to escape the cloud top to space with sufficient energy to trigger a pixel on the imaging array. Through scattering and absorption, certain clouds are able to block most light from reaching the instrument, causing a reduction in detection efficiency (DE) and possibly location accuracy (LA). Radiant lightning emissions that illuminate large cloud top areas are used to examine scenarios where clouds block light from reaching orbit. In some cases, these anomalies in the spatial radiance distribution from the lightning pulse lead to “holes” in the optical lightning flash where certain pixels fail to trigger. Such holes are identified algorithmically in the Tropical Rainfall Measuring Mission satellite LIS record and the microphysical properties of the coincident storm region are queried. We find that holes primarily occur in tall (IR T b < 235 K) convection (87%) and overhanging anvil clouds (10%). The remaining 3% of holes occur in moderate-to-weak convection or in clear air breaks between stormclouds. We further demonstrate how an algorithm that assesses the spatial radiance patterns from energetic lightning pulses might be used to construct an optical transmission gridded stoplight product for GLM that could help operators identify clouds with a potentially reduced DE and LA.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Simulating the Effects of Surface Energy Partitioning on Convective Organization: Case Study and Observations in the US Southern Great Plains

Realistic cloud-resolving simulations were performed to study the effects of surface energy partitioning (surface sensible and latent heat fluxes) on the organization of isolated convection into larger mesoscale convective systems (MCSs) near the US Southern Great Plains. The role of cold pools in mediating surface-convection interactions was explored. Better organized MCSs tended to occur in the experiments with perturbed wetter soil (and more active vegetation), regardless of the effects of soil moisture on the diurnal timing of convective triggering. Wetter soil led to shallower boundary layers and more convective available potential energy than drier soil. The roles of cold pools on convection are lifecycle-stage dependent: A dry surface allows more numerous colliding cold pools, thereby aiding in convective triggering by reducing entrainment in the early stages, and providing gust-front uplift in later stages. However, horizontal propagation of the cold-pool density current can outrun the convective system, creating a slantwise updraft and thus weakening the gust front uplift in later stages. This effect calls into question previous cold pool parameterizations, in which the gust front uplift is mainly proportional to the negative buoyancy of cold air. Finally, both the model and observation show an enhancement of surface latent heat flux during the passage of a gust front at night, suggesting that a positive feedback between the surface and convection helps MCSs to persist into the nighttime.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Observed Global Increases in Tropical Cyclone-Induced Ocean Cooling and Primary Production

Tropical cyclones (TC) provide an important source of mixing for the upper ocean, bringing cold, nutrient-rich water to the surface and triggering phytoplankton blooms. TCs are changing in response to global warming, yet the impacts of those changes on the upper ocean are poorly known. Here we show a significant increasing trend in global TC-induced sea surface temperature (SST) cooling of 0.054oC per decade since 1982. The enhanced cooling has been driven primarily by an increase in the intensity of strong TCs (maximum wind speed > 33 m s-1) and associated strengthening of TC-induced mixing. Consistent with the enhanced mixing and SST cooling, we find a significant increase in TC-induced surface chlorophyll-a concentration of 3.7 x 10-3 mg m-3 per decade in oligotrophic areas. This enhancement of oceanic primary production by TCs is expected to partially offset its projected global decline under climate change.

Dac Da, Nguyen↗
DOE OSTI2022

Wintertime Brine Discharge at the Surface of a Cold Polar Glacier and the Unexpected Absence of Associated Seismicity

A subglacial groundwater system beneath Taylor Glacier, Antarctica, discharges hypersaline, iron-rich brine episodically at the glacier surface to create Blood Falls. However, the triggering mechanism for these brine release events is not yet understood. Identifying which fracture processes are observed seismically can help us better characterize the hydrological system at Taylor Glacier, and more generally, provide us with a broader understanding of englacial hydrologic activity in cold glaciers. We document wintertime brine discharge using time-lapse photography. Subfreezing air temperatures during the brine discharge indicate that surface melt-induced hydrofracture is an unlikely trigger for brine release. Further, we analyze local seismic data to test a hypothesis that fracturing generates elevated surface wave energy preceding and/or coinciding with brine release events. Our results show no discernible elevated Rayleigh wave activity prior to or during Blood Falls brine release. Instead, we find a pattern of seismic events dominated by a seasonal signal, with more Rayleigh events occurring in the summer than the winter from the Blood Falls source area. We calculate that the volumetric opening of cracks that would generate Rayleigh waves at our detection limits are of similar size to myriad cracks in glacier ice, lake ice, and frozen sediment in the terminus area. We therefore propose that any fracturing coincident with brine release activity likely consists of a series of smaller opening events that are masked by other seismicity in the local environment.

58 GEOSCIENCES↗
DOE OSTI2021

Climatic Controls on Soil Carbon Accumulation and Loss in a Dryland Ecosystems

Arid and semiarid ecosystems drive year-to-year variability in the strength of the terrestrial carbon (C) sink, yet there is uncertainty about how soil C gains and losses contribute to this variation. For this work, to address this knowledge gap, we embedded C-depleted soil mesocosms, containing litter or biocrust C inputs, within an in situ dryland ecosystem warming experiment. Over the course of one year, changes in microbial biomass and total soil organic C pools were monitored alongside hourly measurements of soil CO 2 flux. We also developed a biogeochemical model to explore the mechanisms that gave rise to observed soil C dynamics. Field data and model simulations demonstrated that water exerted much stronger control on soil biogeochemistry than temperature, with precipitation events triggering large CO 2 pulses and transport of litter- and biocrust-derived C into the soil profile. We expected leaching of organic matter would result in steady accumulation of C within the mineral soil over time. Instead, the size of the total organic C pool fluctuated throughout the year, largely in response to microbial growth: increases in the size of microbial biomass were negatively correlated with the quantity of C residing in the top 2 cm, where most biogeochemical changes were observed. Our data and models suggest that microbial responses to precipitation events trigger rapid metabolism of dissolved organic C inputs, which strongly limit accumulation of autotroph-derived C belowground. Accordingly, changes in the magnitude and/or frequency of precipitation events in this dryland ecosystem could have profound impacts on the strength of the soil C sink.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Cloud Phase Simulation at High Latitudes in EAMv2: Evaluation using CALIPSO Observations and Comparison with EAMv1

This study performs a comprehensive evaluation of the simulated cloud phase in the U.S. Department of Energy (DOE) Energy Exascale Earth System Model (E3SM) atmosphere model version 2 (EAMv2) and version 1 (EAMv1). Enabled by the CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) simulator, EAMv2 and EAMv1 predicted cloud phase is compared against the GCM-Oriented CALIPSO Cloud Product (CALIPSO-GOCCP) at high latitudes where mixed-phase clouds are prevalent. Our results indicate that the underestimation of cloud ice in simulated high-latitude mixed-phase clouds in EAMv1 has been significantly reduced in EAMv2. The increased ice clouds in the Arctic mainly result from the modification on the WBF (Wegner-Bergeron-Findeisen) process in EAMv2. The impact of the modified WBF process is moderately compensated by the low limit of cloud droplet number concentration (CDNC) in cloud microphysics and the new dCAPE_ULL trigger used in deep convection in EAMv2. Moreover, it is found that the new trigger largely contributes to the better cloud phase simulation over the Norwegian Sea and Barents Sea in the Arctic and the Southern Ocean where large errors are found in EAMv1. However, errors in simulated cloud phase in EAMv1, such as the overestimation of supercooled liquid clouds near the surface in both hemispheres and the underestimation of ice clouds over Antarctica, persist in EAMv2. In conclusion, this study highlights the impact of deep convection parameterizations, which has received little attention, on high-latitude mixed-phase clouds, and the importance of continuous improvement of cloud microphysics in climate models for accurately representing mixed-phase clouds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

The Effect of Normal Stress Oscillations on Fault Slip Behavior Near the Stability Transition From Stable to Unstable Motion

Tectonic fault zones are subject to normal stress variations with a wide range of spatio-temporal scales. Stress perturbations cover a wide range of frequencies and amplitudes from high frequency seismic waves generated by earthquakes to low frequency transients associated with solid Earth tides. These perturbations can reactivate critically stressed faults and trigger earthquakes. Here, we describe lab experiments to illuminate the physics of such changes in friction and the mechanics of earthquake triggering and fault reactivation. Friction tests were done in a double direct shear configuration for conditions near the stability transition from stable to unstable motion. We studied simulated fault gouge composed of quartz powder and conducted experiments at reference normal stress from 10 to 13.5 MPa. After shearing to steady state sliding, we applied sinusoidal normal stress oscillations of amplitude 0.5–2 MPa, and period of 0.5–50 s. We performed numerical simulations using measured values of rate and state friction (RSF) parameters to assess our data. Our results show that low frequency stress oscillations cause a Coulomb-like response of shear strength that transitions from stable slip to slow lab earthquakes as frequency increases. At the critical frequency predicted by RSF we observe periodic stick-slip behavior. Perturbations of high amplitude and short period weaken the fault, while lower amplitudes strengthen the fault. We find that a modified RSF formulation is able to accurately match our laboratory data. Our findings highlight the complex effects of stress perturbations on fault strength and the mode of fault slip.

58 GEOSCIENCES↗
DOE OSTI2024

Causes of Reduced Climate Sensitivity in E3SM From Version 1 to Version 2

The effective climate sensitivity in the Department of Energy's Energy Exascale Earth System Model (E3SM) has decreased from 5.3 K in version 1 to 4.0 K in version 2. This reduction is mainly due to a weaker positive cloud feedback that leads to a stronger negative radiative feedback. Present-day atmosphere-only experiments with uniform 4 K sea surface temperature warming are used to separate the contributions of individual model modifications to the reduced cloud feedback. We find that the reduced cloud feedback is mostly driven by changes over the tropical marine low cloud regime, mainly related to a new trigger function for the deep convection scheme and modifications in the cloud microphysics scheme. The new trigger function helps weaken the low cloud reduction by increasing the cloud water detrainment at low levels from deep convection under warming. Changes to the formula of autoconversion rate from liquid to rain and an introduced minimum cloud droplet number concentration threshold in cloud microphysical calculations help sustain clouds against dissipation by suppressing precipitation generation with warming. In the midlatitudes, the increased Wegener-Bergeron-Findeisen (WBF) efficiency strongly reduces present-day liquid water and leads to a stronger negative cloud optical depth feedback. The reduced trade cumulus cloud feedback in v2 is closer to estimates from recent observational and large-eddy modeling studies but might not be due to the right physical reasons. The reduced mid-latitude cloud feedback may be more plausible because more realistic present-day mixed-phase clouds are produced through the change in the WBF efficiency.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Why Firn Quakes

Snow dampens sounds, but anecdotal reports concisely describe audible propagating collapse events—firnquakes—in Antarctic and Arctic snowfields. We propose combining granular and continuum mechanics to form a testable theory for conditioning, triggering, and propagation of firnquakes consistent with scarce data. A central condition for collapse events is unconsolidated firn at depth. As firn grains compact, stresses are transmitted along force chains which carry the overburden and transition into a continuous medium by pressure sintering. This granular legacy creates solid-like supports of denser layers that keep the material below unconsolidated. Dynamic amplification triggers local brittle failure of the supports, which induces a cascade of collapse propagation. Using bulk density from ice cores as proxy for stiffness, we find the flexural wave speed by collapsing supports matches the recorded firnquake velocities on the order of 100 m/s. Our theory is to be tested in firn sheets and other compacting granular materials.

Voigtländer, A. [Lawrence Berkeley National Labora↗
DOE OSTI2021

Design of COVID-19 staged alert systems to ensure healthcare capacity with minimal closures

Community mitigation strategies to combat COVID-19, ranging from healthy hygiene to shelter-in-place orders, exact substantial socioeconomic costs. Judicious implementation and relaxation of restrictions amplify their public health benefits while reducing costs. We derive optimal strategies for toggling between mitigation stages using daily COVID-19 hospital admissions. With public compliance, the policy triggers ensure adequate intensive care unit capacity with high probability while minimizing the duration of strict mitigation measures. In comparison, we show that other sensible COVID-19 staging policies, including France’s ICU-based thresholds and a widely adopted indicator for reopening schools and businesses, require overly restrictive measures or trigger strict stages too late to avert catastrophic surges. As proof-of-concept, we describe the optimization and maintenance of the staged alert system that has guided COVID-19 policy in a large US city (Austin, Texas) since May 2020. As cities worldwide face future pandemic waves, our findings provide a robust strategy for tracking COVID-19 hospital admissions as an early indicator of hospital surges and enacting staged measures to ensure integrity of the health system, safety of the health workforce, and public confidence.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2021

Thermoresponsive polymer assemblies via variable temperature liquid-phase transmission electron microscopy and small angle X-ray scattering

Abstract Herein, phase transitions of a class of thermally-responsive polymers, namely a homopolymer, diblock, and triblock copolymer, were studied to gain mechanistic insight into nanoscale assembly dynamics via variable temperature liquid-cell transmission electron microscopy (VT-LCTEM) correlated with variable temperature small angle X-ray scattering (VT-SAXS). We study thermoresponsive poly(diethylene glycol methyl ether methacrylate) (PDEGMA)-based block copolymers and mitigate sample damage by screening electron flux and solvent conditions during LCTEM and by evaluating polymer survival via post-mortem matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI-IMS). Our multimodal approach, utilizing VT-LCTEM with MS validation and VT-SAXS, is generalizable across polymeric systems and can be used to directly image solvated nanoscale structures and thermally-induced transitions. Our strategy of correlating VT-SAXS with VT-LCTEM provided direct insight into transient nanoscale intermediates formed during the thermally-triggered morphological transformation of a PDEGMA-based triblock. Notably, we observed the temperature-triggered formation and slow relaxation of core-shell particles with complex microphase separation in the core by both VT-SAXS and VT-LCTEM.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Observation of solid-state bidirectional thermal conductivity switching in antiferroelectric lead zirconate (PbZrO 3 )

Materials with tunable thermal properties enable on-demand control of temperature and heat flow, which is an integral component in the development of solid-state refrigeration, energy scavenging, and thermal circuits. Although gap-based and liquid-based thermal switches that work on the basis of mechanical movements have been an effective approach to control the flow of heat in the devices, their complex mechanisms impose considerable costs in latency, expense, and power consumption. As a consequence, materials that have multiple solid-state phases with distinct thermal properties are appealing for thermal management due to their simplicity, fast switching, and compactness. Thus, an ideal thermal switch should operate near or above room temperature, have a simple trigger mechanism, and offer a quick and large on/off switching ratio. In this study, we experimentally demonstrate that manipulating phonon scattering rates can switch the thermal conductivity of antiferroelectric PbZrO 3 bidirectionally by –10% and +25% upon applying electrical and thermal excitation, respectively. Our approach takes advantage of two separate phase transformations in PbZrO 3 that alter the phonon scattering rate in different manners. In this study, we demonstrate that PbZrO 3 can serve as a fast (<1 second), repeatable, simple trigger, and reliable thermal switch with a net switching ratio of nearly 38% from ~1.20 to ~1.65 W m –1 K –1 .

25 ENERGY STORAGE↗