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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Quantitative Stable-Isotope Probing (qSIP) with Metagenomics Links Microbial Physiology and Activity to Soil Moisture in Mediterranean-Climate Grassland Ecosystems

The growth and physiology of soil microorganisms, which play vital roles in biogeochemical cycling, are shaped by both current and historical soil environmental conditions. Here, we developed and applied a genome-resolved metagenomic implementation of quantitative stable isotope probing (qSIP) with an H 2 18 O labeling experiment to identify actively growing soil microorganisms and their genomic capacities. qSIP enabled measurement of taxon-specific growth because isotopic incorporation into microbial DNA requires production of new genome copies. We studied three Mediterranean grassland soils across a rainfall gradient to evaluate the hypothesis that historic precipitation levels are an important factor controlling trait selection. We used qSIP-informed genome-resolved metagenomics to resolve the active subset of soil community members and identify their characteristic ecophysiological traits. Higher year-round precipitation levels correlated with higher activity and growth rates of flagellar motile microorganisms. In addition to heavily isotopically labeled bacteria, we identified abundant isotope-labeled phages, suggesting phage-induced cell lysis likely contributed to necromass production at all three sites. Further, there was a positive correlation between phage activity and the activity of putative phage hosts. Contrary to our expectations, the capacity to decompose the diverse complex carbohydrates common in soil organic matter or oxidize methanol and carbon monoxide were broadly distributed across active and inactive bacteria in all three soils, implying that these traits are not highly selected for by historical precipitation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Rechargeable alkaline zinc–manganese oxide batteries for grid storage: Mechanisms, challenges and developments

Rechargeable alkaline Zn–MnO 2 (RAM) batteries are a promising candidate for grid-scale energy storage owing to their high theoretical energy density rivaling lithium-ion systems (~400 Wh/L), relatively safe aqueous electrolyte, established supply chain, and projected costs below $100/kWh at scale. In practice, however, many fundamental chemical and physical processes at both electrodes make it difficult to achieve commercially competitive energy density and cycle life. In this paper, we present a detailed and timely analysis of the constituent materials, current commercial status, electrode processes, and performance-limiting factors of RAM batteries. We also examine recently reported strategies in RAM and related systems to address these issues through additives and modifications to the electrode materials and electrolyte, special ion-selective separators and/or coatings, and unconventional cycling protocols. We conclude with a critical summary of these developments and discussion of how future studies should be focused toward the goal of energy-dense, scalable, and cost-effective RAM systems.

25 ENERGY STORAGE↗
DOE OSTI2022

Krylov subspace recycling for evolving structures

Krylov subspace recycling is a powerful tool when solving a long series of large, sparse linear systems that change only slowly over time. In PDE constrained shape optimization, these series appear naturally, as typically hundreds or thousands of optimization steps are needed with only small changes in the geometry. In this setting, however, applying Krylov subspace recycling can be a difficult task. As the geometry evolves, in general, so does the finite element mesh defined on or representing this geometry, including the numbers of nodes and elements and element connectivity. This is especially the case if re-meshing techniques are used. As a result, the number of algebraic degrees of freedom in the system changes, and in general the linear system matrices resulting from the finite element discretization change size from one optimization step to the next. Changes in the mesh connectivity also lead to structural changes in the matrices. In the case of re-meshing, even if the geometry changes only a little, the corresponding mesh might differ substantially from the previous one. Obviously, this prevents any straightforward mapping of the approximate invariant subspace of the linear system matrix (the focus of recycling in this work) from one optimization step to the next; similar problems arise for other selected subspaces. In this paper, we present an algorithm to map an approximate invariant subspace of the linear system matrix for the previous optimization step to an approximate invariant subspace of the linear system matrix for the current optimization step, for general meshes. This is achieved by exploiting the map from coefficient vectors to finite element functions on the mesh, combined with interpolation or approximation of functions on the finite element mesh. We demonstrate the effectiveness of our approach numerically with several proof of concept studies for a specific meshing technique.

42 ENGINEERING↗
DOE OSTI2022

The Influence of 10 Unique Chemical Elements in Shaping the Distribution of Kepler Planets

The chemical abundances of planet-hosting stars offer a glimpse into the composition of planet-forming environments. To further understand this connection, we make the first ever measurement of the correlation between planet occurrence and chemical abundances for ten different elements (C, Mg, Al, Si, S, K, Ca, Mn, Fe, and Ni). Leveraging data from the Apache Point Observatory Galactic Evolution Experiment (APOGEE) and Gaia to derive precise stellar parameters (${\sigma }_{{R}_{\star }}\approx 2.3 \% $, ${\sigma }_{{M}_{\star }}\approx 4.5 \% $) for a sample of 1018 Kepler Objects of Interest, we construct a sample of well-vetted Kepler planets with precisely measured radii (${\sigma }_{{R}_{p}}\approx 3.4 \% $). After controlling for biases in the Kepler detection pipeline and the selection function of the APOGEE survey, we characterize the relationship between planet occurrence and chemical abundance as the number density of nuclei of each element in a star's photosphere raised to a power, β. varies by planet type, but is consistent within our uncertainties across all ten elements. For hot planets (P = 1–10 days), an enhancement in any element of 0.1 dex corresponds to an increased occurrence of ≈20% for super-Earths (Rp = 1–1.9 R⊕) and ≈60% for sub-Neptunes (Rp = 1.9–4 R⊕). Trends are weaker for warm (P = 10–100 days) planets of all sizes and for all elements, with the potential exception of sub-Saturns (Rp = 4–8 R⊕). Finally, we conclude this work with a caution to interpreting trends between planet occurrence and stellar age due to degeneracies caused by Galactic chemical evolution and make predictions for planet occurrence rates in nearby open clusters to facilitate demographics studies of young planetary systems.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

A mathematical analysis of carbon fixing materials that grow, reinforce, and self-heal from atmospheric carbon dioxide

Carbon fixing materials are a new class of self-healing, self-reinforcing materials we have introduced that utilize ambient CO 2 to chemically add to an ever extending carbon backbone. This class of materials can utilize biological or non-biological photocatalysts and support a wide range of potential backbone chemistries. However, there is no analysis to date that describes their fundamental limits in terms of chemical kinetics and mass transfer. In this computational study, we employ a reaction engineering, and materials science analysis to answer basic questions about the maximum growth rate, photocatalytic requirements and limits of applicable materials. Our proposed mathematical framework envelops three main functions required for carbon fixing materials: (1) adsorption of CO 2 from air, (2) photocatalytic reduction of CO 2 into selected monomers, and (3) polymerization of CO 2 -derived monomers. First, by performing a Damköhler number analysis, we derive criteria for the cross over from kinetic control to mass transfer limited growth, setting upper limits on performance of a potential photocatalyst. Next, we analyze photocatalytic reduction of CO 2 to single carbon products, using known catalytic pathways and kinetic data. We identify formaldehyde as a C1 intermediate having unique potential for incorporation into the material backbone of carbon fixing materials. As an example, we find that a diamond-shaped reaction network graph for CO 2 reduction, passing through CO and HCOOH intermediates, accurately describes kinetic data for cobalt-promoted TiO 2 nanoparticles at room temperature and 1 atm CO 2 . Finally, as an applied case study, we consider and analyze the example of a carbon fixing poly(oxymethylene) system with embedded catalyst promoting the photocatalytic reduction of CO 2 to formaldehyde. The latter then trimerizes to a trioxane monomer which subsequently polymerizes to polyoxymethylene. This reaction engineering analysis introduces benchmarks for carbon fixing materials with respect to achievable rates of photocatalysis, adsorption, and polymerization. These results should prove valuable for the design, evaluation, and benchmarking of this emergent and new class of environmentally sustainable materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Radial structure and formation of the Milky Way disc

The formation of the Galactic disc is an enthusiastically debated issue. Numerous studies and models seek to identify the dominant physical process(es) that shaped its observed properties; for example, satellite accretion, starburst, quenching, gas infall, and stellar radial migration. Taking advantage of the improved coverage of the inner Milky Way provided by the SDSS DR16 APOGEE catalogue and of the ages published in the APOGEE-AstroNN Value Added Catalogue (VAC), we examined the radial evolution of the chemical and age properties of the Galactic stellar disc with the aim of better constraining its formation. Using a sample of 199 307 giant stars with precise APOGEE abundances and APOGEE-AstroNN ages, selected in a ±2 kpc layer around the galactic plane, we assessed the dependency as a function of guiding radius of (i) the median metallicity, (ii) the ridge lines of the [Fe/H] – [Mg/Fe] and age–[Mg/Fe] distributions, and (iii) the age distribution function (ADF). The giant star sample allows us to probe the radial behaviour of the Galactic disc from R g = 0 to 14–16 kpc. The thick disc [Fe/H] – [Mg/Fe] ridge lines follow closely grouped parallel paths, supporting the idea that the thick disc did form from a well-mixed medium. However, the ridge lines present a small drift in [Mg/Fe], which decreases with increasing guiding radius. At sub-solar metallicity, the intermediate and outer thin disc [Fe/H] – [Mg/Fe] ridge lines follow parallel sequences shifted to lower metallicity as the guiding radius increases. We interpret this pattern as the signature of a dilution of the interstellar medium from R g ~ 6 kpc to the outskirts of the disc, which occurred before the onset of the thin disc formation. The APOGEE-AstroNN VAC provides stellar ages for statistically significant samples of thin disc stars from the Galactic centre up to R g ~ 14 kpc. An important result provided by this dataset is that the thin disc presents evidence of an inside-out formation up to R g ~ 10 – 12 kpc. Moreover, about ~7 Gyr ago, the [Mg/Fe] ratio in the outer thin disc (R g > 10 kpc) was higher by about ~0.03–0.05 dex than in the more internal regions of the thin disc. This could be the fossil record of a pollution of the outer disc gas reservoir by the thick disc during its starburst phase.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Spatially resolved mass–metallicity relation at $z$ ~ 0.26 from the MUSE-Wide Survey

Galaxies in the local universe have a spatially resolved star-forming main sequence (rSFMS) and mass–metallicity relation (rMZR). We know that the global mass–metallicity relation (MZR) results from the integral of the rMZR, and it evolves with redshift. However, the evolution of the rMZR with redshift is still unclear because the spatial resolution and signal-to-noise ratio are low. Currently, too few observations beyond the local universe are available, and only simulations can reproduce the evolution of the rMZR with redshift. We selected ten emission-line galaxies with an average redshift of $z$ ~ 0.26 from the MUSE-Wide DR1. We obtained the spatially resolved star formation rate (SFR) and metallicity from integral field spectroscopy (IFS), as well as the stellar mass surface density from 3D-HST photometry. We derived the rSFMS and rMZR at $z$ ~ 0.26 and compared them with those of local galaxies. We find that the rSFMS of galaxies at $z$ ~ 0.26 has a slope of ~0.771. The rMZR exists at z ~ 0.26, showing a similar shape to that of the local universe, but a lower average metallicity that is about ~0.11 dex lower than the local metallicity. In addition, we also study the spatially resolved fundamental metallicity relation (rFMR) of these galaxies. However, there is no obvious evidence that an rFMR exists at $z$ ~ 0.26, and it is not an extension of rMZR at a high SFR. Similar to their global versions, the rSFMS and rMZR of galaxies also evolve with redshift. At fixed stellar mass, galaxies at higher redshift show a higher SFR and lower metallicity. In conclusion, these suggest that the evolution of the global galaxy properties with redshift may result from integrating the evolution of the spatially resolved galaxy properties.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Coordination and divergence in community assembly processes across co-occurring microbial groups separated by cell size

Setting the pace of life and constraining the role of members in food webs, body size can affect the structure and dynamics of communities across multiple scales of biological organization (e.g., from the individual to the ecosystem). However, its effects on shaping microbial communities, as well as underlying assembly processes, remain poorly known. Here, we analyzed microbial diversity in the largest urban lake in China and disentangled the ecological processes governing microbial eukaryotes and prokaryotes using 16S and 18S amplicon sequencing. We found that pico/nano-eukaryotes (0.22–20 μm) and micro-eukaryotes (20–200 μm) showed significant differences in terms of both community composition and assembly processes even though they were characterized by similar phylotype diversity. We also found scale dependencies whereby micro-eukaryotes were strongly governed by environmental selection at the local scale and dispersal limitation at the regional scale. Interestingly, it was the micro-eukaryotes, rather than the pico/nano-eukaryotes, that shared similar distribution and community assembly patterns with the prokaryotes. This indicated that assembly processes of eukaryotes may be coupled or decoupled from prokaryotes’ assembly processes based on eukaryote cell size. While the results support the important influence of cell size, there may be other factors leading to different levels of assembly process coupling across size classes. Additional studies are needed to quantitatively parse the influence of cell size versus other factors as drivers of coordinated and divergent community assembly processes across microbial groups. Regardless of the governing mechanisms, our results show that there are clear patterns in how assembly processes are coupled across sub-communities defined by cell size. These size-structured patterns could be used to help predict shifts in microbial food webs in response to future disturbance.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Metabolic interactions shape emergent biofilm structures in a conceptual model of gut mucosal bacterial communities

Abstract The gut microbiome plays a major role in human health; however, little is known about the structural arrangement of microbes and factors governing their distribution. In this work, we present an in silico agent-based model (ABM) to conceptually simulate the dynamics of gut mucosal bacterial communities. We explored how various types of metabolic interactions, including competition, neutralism, commensalism, and mutualism, affect community structure, through nutrient consumption and metabolite exchange. Results showed that, across scenarios with different initial species abundances, cross-feeding promotes species coexistence. Morphologically, competition and neutralism resulted in segregation, while mutualism and commensalism fostered high intermixing. In addition, cooperative relations resulted in community properties with little sensitivity to the selective uptake of metabolites produced by the host. Moreover, metabolic interactions strongly influenced colonization success following the invasion of newcomer species. These results provide important insights into the utility of ABM in deciphering complex microbiome patterns.

Biotechnology & Applied Microbiology↗
DOE OSTI2023

Atomic-scale in situ observation of electron beam and heat induced crystallization of Ge nanoparticles and transformation of Ag@Ge core-shell nanocrystals

Crystallization of amorphous materials by thermal annealing has been investigated for numerous applications in the fields of nanotechnology, such as thin-film transistors and thermoelectric devices. The phase transition and shape evolution of amorphous germanium (Ge) and Ag@Ge core–shell nanoparticles with average diameters of 10 and 12 nm, respectively, were investigated by high-energy electron beam irradiation and in situ heating within a transmission electron microscope. The transition of a single Ge amorphous nanoparticle to the crystalline diamond cubic structure at the atomic scale was clearly demonstrated. Depending on the heating temperature, a hollow Ge structure can be maintained or transformed into a solid Ge nanocrystal through a diffusive process during the amorphous to crystalline phase transition. Selected area diffraction patterns were obtained to confirm the crystallization process. In addition, the thermal stability of Ag@Ge core–shell nanoparticles with an average core of 7.4 and a 2.1 nm Ge shell was studied by applying the same beam conditions and temperatures. The results show that at a moderate temperature (e.g., 385 °C), the amorphous Ge shell can completely crystallize while maintaining the well-defined core–shell structure, while at a high temperature (e.g., 545 °C), the high thermal energy enables a freely diffusive process of both Ag and Ge atoms on the carbon support film and leads to transformation into a phase segregated Ag–Ge Janus nanoparticle with a clear interface between the Ag and Ge domains. In conclusion, this study provides a protocol as well as insight into the thermal stability and strain relief mechanism of complex nanostructures at the single nanoparticle level with atomic resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Homologous recombination shapes the architecture and evolution of bacterial genomes

Homologous recombination is a key evolutionary force that varies considerably across bacterial species. However, how the landscape of homologous recombination varies across genes and within individual genomes has only been studied in a few species. Here, we used Approximate Bayesian Computation to estimate the recombination rate along the genomes of 145 bacterial species. Our results show that homologous recombination varies greatly along bacterial genomes and shapes many aspects of genome architecture and evolution. The genomic landscape of recombination presents several key signatures: rates are highest near the origin of replication in most species, patterns of recombination generally appear symmetrical in both replichores (i.e. replicational halves of circular chromosomes) and most species have genomic hotspots of recombination. Furthermore, many closely related species share conserved landscapes of recombination across orthologs indicating that recombination landscapes are conserved over significant evolutionary distances. We show evidence that recombination drives the evolution of GC-content through increasing the effectiveness of selection and not through biased gene conversion, thereby contributing to an ongoing debate. Finally, we demonstrate that the rate of recombination varies across gene function and that many hotspots of recombination are associated with adaptive and mobile regions often encoding genes involved in pathogenicity.

Torrance, Ellis L [University of North Carolina, G↗
DOE OSTI2025

Tailoring spectral properties for entangled photon generation

The linear intensity scaling of entangled two-photon absorption (ETPA) offers a fundamental mechanism to enable nonlinear optical spectroscopy and microscopy under a substantially lower excitation power than is currently feasible. However, the long data acquisition time and low signal-to-noise ratio in reported ETPA-based spectroscopic and microscopic studies prevent its widespread application. To gain the full potential of this novel quantum light approach, it is essential to optimize entangled photon generation for significantly enhanced ETPA responses. Here, we report a new quantum light source by combining entangled photon generation with free-space femtosecond pump-pulse shaping. Here, through measurements of singles and coincidence counts by varying the patterns applied to a spatial light modulator to control the spectral widths of the pump pulses, we reveal strong dependence of the singles and coincidence count rates as well as their ratios on the spectral widths of pump pulses. An optimal spectral width for the highest ratios between the coincidence photon and the signal or idler photon count rates is also determined. Identification of such optimal spectral widths for entangled photon generation in the presence of postgeneration spectral selection makes this quantum light source a promising choice for ETPA-based spectroscopy and imaging.

Photon pairs & parametric down-conversion↗
DOE OSTI2020

Polarimetric Radar Characteristics of Simulated and Observed Intense Convective Cores for a Midlatitude Continental and Tropical Maritime Environment

This study contrasts midlatitude continental and tropical maritime deep convective cores using polarimetric radar observables and retrievals from selected deep convection episodes during the MC3E and TWPICE field campaigns. The continental convective cores produce stronger radar reflectivities throughout the profiles, while maritime convective cores produce more positive differential reflectivity Z dr and larger specific differential phase K dp above the melting level. Hydrometeor identification retrievals revealed the presence of large fractions of rimed ice particles (snow aggregates) in the continental (maritime) convective cores, consistent with the Z dr and K dp observations. The regional cloud-resolving model simulations with bulk and size-resolved bin microphysics are conducted for the selected cases, and the simulation outputs are converted into polarimetric radar signals and retrievals identical to the observational composites. Both the bulk and the bin microphysics reproduce realistic land and ocean (L-O) contrasts in reflectivity, polarimetric variables of rain drops, and hydrometeor profiles, but there are still large uncertainties in describing Z dr and K dp of ice crystals associated with the ice particle shapes/orientation assumptions. Sensitivity experiments are conducted by swapping background aerosols between the continental and maritime environments, revealing that background aerosols play a role in shaping the distinct L-O contrasts in radar reflectivity associated with raindrop sizes, in addition to the dominant role of background thermodynamics.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Near-infrared Spectral Characterization of Solar-type Stars in the Northern Hemisphere

Although solar-analog stars have been studied extensively over the past few decades, most of these studies have focused on visible wavelengths, especially those identifying solar-analog stars to be used as calibration tools for observations. As a result, there is a dearth of well-characterized solar analogs for observations in the near-infrared, a wavelength range important for studying solar system objects. We present 184 stars selected based on solar-like spectral type and V−J and V−K colors whose spectra we have observed in the 0.8–4.2 μm range for calibrating our asteroid observations. Each star has been classified into one of three ranks based on spectral resemblance to vetted solar analogs. Of our set of 184 stars, we report 145 as reliable solar-analog stars, 21 as solar analogs usable after spectral corrections with low-order polynomial fitting, and 18 as unsuitable for use as calibration standards owing to spectral shape, variability, or features at low to medium resolution. We conclude that all but five of our candidates are reliable solar analogs in the longer wavelength range from 2.5 to 4.2 μm. The average colors of the stars classified as reliable or usable solar analogs are V−J = 1.148, V−H = 1.418, and V−K = 1.491, with the entire set being distributed fairly uniformly in R.A. across the sky between −27° and +67° in decl.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

A Universal Model of Cation Effects in Electrocatalysis

Electrolyte cations are conventionally viewed as inert spectators in electrocatalysis. However, a wealth of observations show that catalytic rates are often highly sensitive to cation identity. Despite their prevalence, these cation effects have resisted a unified mechanistic explanation, with different physical phenomena implicated across reaction chemistries, catalyst compositions, and choice of solvent. In this perspective, we describe a general framework for understanding cation effects in electrocatalysis based on electrostatics. We argue that cations influence reaction rates by modifying the strength of the electric field present at the catalyst surface, which alters the energetics of adsorbed intermediates and transition states according to their dipole moments and polarizabilities. The magnitude of this field depends on how cations arrange at the electrode surface, controlled by their size, shape, solvation, and packing efficiency. Cations that can arrange more densely result in a steeper potential drop at the electrode surface and consequently a stronger electric field. Our model further identifies two criteria for observing cation effects: (1) the operating potential must be negative of the electrode’s potential of zero total charge, ensuring that cations accumulate at the interface, and (2) the energetics of the kinetically relevant elementary step must be field sensitive. This framework reconciles previously inconsistent trends, including why cation effects appear only for some catalysts, why reaction selectivity is sensitive to cation identity, and why activity can increase with cation size on certain metals but decrease on others. Supported by kinetic measurements, spectroscopy, and atomistic simulations, the model provides both conceptual value for building intuition about catalysis at charged interfaces and predictive value for anticipating trends for new reactions, catalysts, and electrolytes. We conclude by highlighting the importance of electric fields across electrochemical, thermochemical, and biological catalysis and propose that considering the electrostatic environment around active sites offers new opportunities for improving activity and selectivity.

cation effects↗
DOE OSTI2021

Liquid-induced topological transformations of cellular microstructures

The fundamental topology of cellular structures—the location, number and connectivity of nodes and compartments—can profoundly affect their acoustic, electrical5, chemical, mechanical and optical properties, as well as heat, fluid and particle transport. Approaches that harness swelling, electromagnetic actuation and mechanical instabilities in cellular materials have enabled a variety of interesting wall deformations and compartment shape alterations, but the resulting structures generally preserve the defining connectivity features of the initial topology. Achieving topological transformation presents a distinct challenge for existing strategies: it requires complex reorganization, repacking, and coordinated bending, stretching and folding, particularly around each node, where elastic resistance is highest owing to connectivity. Here we introduce a two-tiered dynamic strategy that achieves systematic reversible transformations of the fundamental topology of cellular microstructures, which can be applied to a wide range of materials and geometries. Our approach requires only exposing the structure to a selected liquid that is able to first infiltrate and plasticize the material at the molecular scale, and then, upon evaporation, form a network of localized capillary forces at the architectural scale that ‘zip’ the edges of the softened lattice into a new topological structure, which subsequently restiffens and remains kinetically trapped. Reversibility is induced by applying a mixture of liquids that act separately at the molecular and architectural scales (thus offering modular temporal control over the softening–evaporation–stiffening sequence) to restore the original topology or provide access to intermediate modes. Guided by a generalized theoretical model that connects cellular geometries, material stiffness and capillary forces, we demonstrate programmed reversible topological transformations of various lattice geometries and responsive materials that undergo fast global or localized deformations. In conclusion, we then harness dynamic topologies to develop active surfaces with information encryption, selective particle trapping and bubble release, as well as tunable mechanical, chemical and acoustic properties.

42 ENGINEERING↗
DOE OSTI2025

Measuring Vibronic Coupling and Ultrafast Charge Delocalization on Nanocrystal Surfaces Using Ligand-Specific Vibrational Probes

The primary goal of this proposal was to measure and quantify how vibronic ligand-exciton interactions at the inorganic-organic interface of semiconductor nanocrystals (NCs) govern femtosecond non-radiative relaxation and charge delocalization mechanisms as a function of nanocrystal and ligand structures – including NC size, shape, and ligand identity. Molecular-scale chemical and physical properties and interactions of surface ligands dictate nanocrystal exciton dynamics on the femto-to-microsecond timescales. Improvements in synthesis, experimental, and theoretical characterizations have enhanced our understanding of NC photophysics. However, quantitative descriptions of complex ligand-exciton interactions at the NC surface have remained elusive, which limits elucidation of relaxation mechanisms that determine overall carrier transfer dynamics at the exciton-ligand interface. Thus, the central motivation for this proposal was to fill a significant knowledge gap for judicious selection of ligand-functionalized nanocrystals for targeted isolation and capture of charge carriers to drive selective organic photocatalytic transformations in NC photocatalysts and NC-assembled photonic materials. Our unique two-pronged experimental approach combining nanocrystal synthesis and ligand-specific nonlinear spectroscopy has resulted in (i) four peer-reviewed publications; (ii) 12+ invited and contributed posters and talks at national and international scientific meetings and seminars, (iii) two completed PhD theses, (iv) training of two postdoctoral researchers, three PhD students, and two undergraduate students, and (v) two manuscripts under preparation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The completed SDSS-IV extended baryon oscillation spectroscopic survey: geometry and growth from the anisotropic void–galaxy correlation function in the luminous red galaxy sample

ABSTRACT We present an analysis of the anisotropic redshift-space void–galaxy correlation in configuration space using the Sloan Digital Sky Survey extended Baryon Oscillation Spectroscopic Survey (eBOSS) Data Release 16 luminous red galaxy (LRG) sample. This sample consists of LRGs between redshifts 0.6 and 1.0, combined with the high redshift z > 0.6 tail of the Baryon Oscillation Spectroscopic Survey Data Release 12 CMASS sample. We use a reconstruction method to undo redshift-space distortion (RSD) effects from the galaxy field before applying a watershed void-finding algorithm to remove bias from the void selection. We then perform a joint fit to the multipole moments of the correlation function for the growth rate fσ8 and the geometrical distance ratio DM/DH, finding $f\sigma _8(z_\rm {eff})=0.356\pm 0.079$ and $D_M/D_H(z_\rm {eff})=0.868\pm 0.017$ at the effective redshift $z_\rm {eff}=0.69$ of the sample. The posterior parameter degeneracies are orthogonal to those from galaxy clustering analyses applied to the same data, and the constraint achieved on DM/DH is significantly tighter. In combination with the consensus galaxy BAO and full-shape analyses of the same sample, we obtain fσ8 = 0.447 ± 0.039, DM/rd = 17.48 ± 0.23, and DH/rd = 20.10 ± 0.34. These values are in good agreement with the ΛCDM model predictions and represent reductions in the uncertainties of $13{{\ \rm per\ cent}}$, $23{{\ \rm per\ cent}}$, and $28{{\ \rm per\ cent}}$, respectively, compared to the combined results from galaxy clustering, or an overall reduction of 55 per cent in the allowed volume of parameter space.

Nadathur, Seshadri↗