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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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

High Fidelity CFD Simulations Supporting the KP-FHR

Kairos Power, LLC, is developing its version of the Fluoride-cooled High-temperature Reactor, the KP-FHR. The design uses a pebble bed core with fluoride salt as a coolant. The pebbles used in the KP-FHR have a diameter of 4 cm, with a shell fuel region where TRISO particles are embedded. A Pebble bed core design is adopted by several Gen IV reactors, They boast many benefits, such as fuel integrity, highly efficient heat transfer, and passive safety. However, it is challenging to accurately predict temperature and flow inside a pebble bed. Traditional approaches use the porous media model, which regards the pebble bed as a continuous medium, but with different temperature fields representing different levels, such as the fluid temperature, pebble surface temperature, and pebble center temperature. Empirical heat transfer correlations are adopted to calculate the heat transfer coefficient between different phases. However, empirical correlations are usually validated with experimental data, which usually lacks detail inside the pebble bed. The available experimental data is also generally at a high Reynolds number, which falls outside of the conditions of KP-FHR. Explicit computational fluid dynamics (CFD) simulations of randomly packed pebble beds have only become feasible recently. This is thanks to the rapid development of computational power and scalable algorithms. In this work, we used the Spectral Element Method (SEM) CFD code NekRS to simulate the randomly packed pebble bed in a cylindrical container. NekRS, which is the GPU variant of Nek5000, but refactored to utilize the computational power of GPUs using the OCCA library to run on hybrid architecture high performance computing systems. It was initially developed with the libParamunal library, but truncated and tuned for large-scale turbulence simulation. As a result, the SEM reaches higher precision with the same degrees of freedom by using a high-order Lagrange polynomial basis distributed on Gauss-Lobatto-Legendre quadrature inside each element, compared to lower-order methods, such the Finite Volume Method and Finite Element Method. The report is divided into five parts. We start with a general discussion of the pebble bed reactor, along with a specific investigation into the KP-FHR. The second part presents the numerical methodology. In the third part, we study a modular pebble bed with 1741 pebbles in a container of 7 pebble-diameter radius. Beyond LES simulations done by NekRS, we also leveraged the thermal radiation model in OpenFOAM to study heat transfer under no-forced-flow scenarios. Then, in the fourth part we simulated a pebble bed similar to the size of the Hermes Test Reactor. The total number of pebbles is in these simulations is 34,374. The container radius is 14 pebble-diameters. Finally, the report concludes in part five, with a discussion of future work.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Ultrafast charge transfer and carrier dynamics in a WS 2 /MoSe 2 few-layer van der Waals heterostructure

Photocarrier dynamics including interlayer charge transfer and intralayer valley scattering are studied in a heterostructure formed by trilayer WS 2 and MoSe 2 . The sample is fabricated by mechanical exfoliation and dry transfer and characterized by atomic force microscopy, Raman spectroscopy, and photoluminescence measurements. The conduction band minima of the two materials are nearly degenerate, representing a unique band alignment. Layer-selective pump–probe measurements are performed with three configurations to reveal a complete picture of the photocarrier dynamics. By comparing the heterostructure with the two individual trilayer materials in each experimental configuration, ultrafast interlayer charge transfer is unambiguously observed, which occurs on the same time scale as the intralayer valley scattering of the photocarriers. The quasi-equilibrium distribution of electrons in the two layers mediate the fast carrier recombination process. Furthermore, these results show that the band structures of the few-layer transition metal dichalcogenides can enable rich photocarrier dynamics with intermediate band alignments that are complementary to the previously studied monolayer–monolayer heterostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Inferring the Energetics of CO 2 –Aniline Adduct Formation from Vibrational Spectroscopy

Control of atmospheric CO 2 is an important contemporary scientific and engineering challenge. Towards this goal, the reaction of CO 2 with amines to form carbamate bonds is an established method for CO 2 capture. However, controllable reversal of this reaction remains difficult and requires tuning the energetics of the carbamate bond. Through IR spectroscopy, we show that a characteristic frequency observed upon carbamate formation varies as a function of the substituent’s Hammett parameter for a family of para- substituted anilines. We present computational evidence that the vibrational frequency of the adducted CO 2 serves as a predictor of the energy of formation of the carbamate. Electron donating groups typically enhance the driving force of carbamate formation by transferring more charge to the adducted CO 2 and thus increasing the occupancy of the anti-bonding orbital in the carbon-oxygen bonds. Increased occupancy of the anti-bonding orbital within adducted CO 2 indicates a weaker bond, leading to a red shift in the characteristic carbamate frequency. As a result, our work serves the large field of CO 2 capture research where spectroscopic observables, such as IR frequencies, are more easily obtainable and can stand in as a descriptor of driving forces.

Amines↗
DOE OSTI2025

Similarity Metric for Data Optimization and Efficient Training of Reactive Machine Learning Force Fields for Hydrocarbon Radiolysis

Radiolysis is a common approach to sterilize polymers, chemically modify them for upcycling, and accelerate their decomposition for recycling purposes. Reactive molecular dynamics (MD) simulations provide a powerful tool to generate atomic-level trajectories of the reactive processes and quantify radiolytic chemical degradation pathways. For this, machine learning (ML) surrogate models for reactive force fields with quantum mechanical accuracy are now widely used, which require ML training data sets that can provide information on atomic environments for target chemical systems. However, radiolysis chemistry can be highly complex and diverse, which poses significant challenges for generating training data to parametrize ML models. In this regard, we developed a method for optimizing the training data set using a cosine similarity metric to help guide training set selection for radiolysis of polyethylene, a model hydrocarbon polymer, as well as to enhance the transferability of our reactive ML force field (MLFF) to a variety of molecular and polymeric systems. Our approach performs atom-by-atom comparisons between local atomic environments to pinpoint important data points associated with rare and localized events, such as radiolysis damage within structures. We apply this approach to train the Chebyshev Interaction Model for Efficient Simulation (ChIMES) MLFF model, which expresses the atomic interaction potentials in terms of linear combinations of many-body Chebyshev polynomials. We first show that our method can reduce our training set size by ∼70% while improving overall accuracy compared to more standard MD model fitting approaches. We then validate our optimum model against diverse hydrocarbon simulation data, including simple alkanes and systems with unsaturated carbon bonds, over a wide range of thermodynamic conditions. Finally, we use our ChIMES model to perform MD simulations of radiolytic damage with large-scale systems that help avoid system size effects. Overall, our approach yields an MD force field that retains most of the accuracy of the underlying quantum method while yielding many orders of improvement in computational efficiency. In conclusion, our efforts will have impact on future hydrocarbon polymer radiolysis studies, where the chemical details of the polymer–radiation interactions can have a strong effect on the resulting products observed in experiments.

Hydrocarbons↗
DOE OSTI2024

Novel microbial based enzymatic CO2 fixation mechanisms: Conformational control of enzymatic reactivity

The broad, long-term goal of the research is to provide insight into the mechanism of novel carboxylation and electron bifurcation reactions as paradigms to study how enzyme utilized protein conformational change to protect reactive intermediates and/or control the pathway in a catalytic cycle. catalyzed by enzymes involved in bacterial alkene, ketone, and epoxide metabolism. We are examining two paradigms in which conformational change is a key mechanistic feature of 1) protecting reaction intermediates that are sensitive to breakdown in the presence of water and 2) directing electron flow in reactions that split electron pairs along two pathways in reactions that fine tune metabolic efficiency in microbial metabolism. Both paradigms are of key importance in defining the molecular determinants of reactions relevant to CO 2 capture and fuel upcycling. In the first paradigm the compounds acetone and bicarbonate are activated by the addition of phosphate creating reaction intermediates (phosphoenolacetone and carboxyphosphate) that are very sensitive to breakdown in the presence of water. We are studying the mechanism of how the enzyme protects these reactive intermediates from water by encapsulating them upon their formation within a hydrophobic protein channel leading to an enzyme active site approximately 40 Å away. In the second paradigm, we are examining how the direction of electron transfer reactions can be modulated through protein conformational change that alters either the difference driving force or distance or both between electron transfer pathways in enzymes that catalyze electron bifurcation. We are using a combination of enzyme kinetics, mass spectrometry, spectroscopy, and structural analysis through X-ray diffraction and scattering methods to characterize the mechanism of conformational changes along the catalytic path. Within the context of the mission of the Department of Energy and the core activities of the Energy Biosciences, the results obtained in the study will reveal new insights into the fundamentals of novel carboxylation / CO 2 capture chemical transformations and electron transfer reactions that equate to biological fuel upcycling.

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

Fluid dynamic and thermal performance of a slotted cylinder at low Reynolds number

The fluid dynamic and thermal performance of a circular cylinder with a slot parallel to the flow is numerically investigated. The study utilized the semi-implicit finite volume multi-material algorithm MPM-ICE, a component of the Uintah framework. The normalized slot width s/D ranges from 0.1 - 0.3, introducing an additional heat transfer surface area between ~ 10 and ~ 50%, and a mass reduction between ~ 13 and ~ 38% in the cylinder. We assumed two-dimensional incompressible flow and simulated a Reynolds number Re D between 100 and 1000. The slotted cylinders are found to have a total drag force reduction up to ~ 45%, compared to a solid cylinder despite the additional viscous drag force in the slot. Convection heat transfer is enhanced up to ~ 70%. Further, the slotted cylinder performance index, defined as the ratio of the heat rate to the drag force, increases up to maximum of ~ 3, indicating better overall thermal fluid performance. An entropy analysis showed the best performance index occurs at the highest Re D . Correlations for drag coefficient and Nusselt number are proposed along with an entropy optimization method.

42 ENGINEERING↗
DOE OSTI2023

Experiments and Simulations to Describe Alkalinity Release from Particle-Containing Oil-in-Water Emulsions and Particle Suspensions

Among the most common amendments added to groundwater during site remediation are compounds used to adjust or maintain the pH. This research describes an approach to encapsulate mineral particles (MgO and CaCO 3 ) within oil droplets suspended within an aqueous phase for the purpose of delivery to the subsurface environment. A series of batch experiments was combined with mathematical modeling to illustrate the encapsulation and understand the influence of particle encapsulation on rates and extents of alkalinity release. The encapsulation of the alkalinity-releasing particles results in slower rates of amendment release as compared to rates obtained using suspensions of bare mineral particles, allowing for the possibility of control as a function of the pH. The results indicate that the alkalinity release from particle suspensions followed a mineral dissolution mechanism that could not explain the rate of the alkalinity release of the encapsulated particles. The reduction in mineral dissolution rates observed with the encapsulated particles was found to result from a mass transfer limitation. This limitation was well described using a linear driving force expression to account for the resistance to mass transfer at the oil–water interface.

EVO↗
DOE OSTI2022

Revisiting the Bonding Model for Gold(I) Species: The Importance of Pauli Repulsion Revealed in a Gold(I)‐Cyclobutadiene Complex

Abstract Understanding the bonding of gold(I) species has been central to the development of gold(I) catalysis. Herein, we present the synthesis and characterization of the first gold(I)‐cyclobutadiene complex, accompanied with bonding analysis by state‐of‐the‐art energy decomposition analysis methods. Analysis of possible coordination modes for the new species not only confirms established characteristics of gold(I) bonding, but also suggests that Pauli repulsion is a key yet hitherto overlooked element. Additionally, we obtain a new perspective on gold(I)‐bonding by comparison of the gold(I)‐cyclobutadiene to congeners stabilized by p‐, d‐, and f‐block metals. Consequently, we refine the gold(I) bonding model, with a delicate interplay of Pauli repulsion and charge transfer as the key driving force for various coordination motifs. Pauli repulsion is similarly determined as a significant interaction in Au I ‐alkyne species, corroborating this revised understanding of Au I bonding.

Wong, Zeng Rong↗
DOE OSTI2022

Revisiting the Bonding Model for Gold(I) Species: The Importance of Pauli Repulsion Revealed in a Gold(I)–Cyclobutadiene Complex

Understanding the bonding of gold(I) species has been central to the development of gold(I) catalysis. Herein, we present the synthesis and characterization of the first gold(I)-cyclobutadiene complex, accompanied with bonding analysis by state-of-the-art energy decomposition analysis methods. Analysis of possible coordination modes for the new species not only confirms established characteristics of gold(I) bonding, but also suggests that Pauli repulsion is a key yet hitherto overlooked element. Additionally, we obtain a new perspective on gold(I)-bonding by comparison of the gold(I)-cyclobutadiene to congeners stabilized by p-, d-, and f-block metals. Consequently, we refine the gold(I) bonding model, with a delicate interplay of Pauli repulsion and charge transfer as the key driving force for various coordination motifs. Finally, Pauli repulsion is similarly determined as a significant interaction in Au I -alkyne species, corroborating this revised understanding of Au I bonding.

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

Preface: special issues on photosystem II

Here, the appearance of oxygenic photosynthesis 3–4 billion years ago is arguably one of the most important evolutionary developments which radically transformed both the biotic and abiotic landscapes of Earth. The presence of molecular oxygen enabled the evolution of complex lifeforms requiring large amounts of chemical energy which could only be produced by aerobic respiration. Additionally, molecular oxygen remodeled the geochemistry of the planet during its transition from a reducing to an oxidizing atmosphere during the Great Oxidation Event. Central to these processes is Photosystem II (PS II), the light energy-driven, water-plastoquinone oxidoreductase which initially evolved in cyanobacteria and subsequently was incorporated, along with Photosystem I (PS I), the cytochrome b 6 f complex and the Ndh complex, into all algae and higher plants by the process of endosymbiosis. This membrane protein complex releases molecular oxygen and protons as the byproducts of water splitting and produces plastoquinol, which provides reducing equivalents that are used sequentially by the cytochrome b 6 /f complex, PS I, and ultimately, as NADPH + H + , by the Calvin–Benson–Bassham cycle. Additionally, the protons released by PS II (and those pumped by the cytochrome b 6 /f complex and the NDH complex (during cyclic electron transfer)) form the proton motive force that drives ATP synthesis via the ATP Synthase, thus providing the chemical energy source for carbon fixation.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Low-thermal-budget synthesis of monolayer molybdenum disulfide for silicon back-end-of-line integration on a 200 mm platform

Two-dimensional (2D) materials are promising candidates for future electronics due to their excellent electrical and photonic properties. Although promising results on the wafer-scale synthesis (≤150 mm diameter) of monolayer molybdenum disulfide (MoS 2 ) have already been reported, the high-quality synthesis of 2D materials on wafers of 200 mm or larger, which are typically used in commercial silicon foundries, remains difficult. The back-end-of-line (BEOL) integration of directly grown 2D materials on silicon complementary metal–oxide–semiconductor (CMOS) circuits is also unavailable due to the high thermal budget required, which far exceeds the limits of silicon BEOL integration (<400 °C). This high temperature forces the use of challenging transfer processes, which tend to introduce defects and contamination to both the 2D materials and the BEOL circuits. Here we report a low-thermal-budget synthesis method (growth temperature < 300 °C, growth time ≤ 60 min) for monolayer MoS 2 films, which enables the 2D material to be synthesized at a temperature below the precursor decomposition temperature and grown directly on silicon CMOS circuits without requiring any transfer process. We designed a metal–organic chemical vapour deposition reactor to separate the low-temperature growth region from the high-temperature chalcogenide-precursor-decomposition region. We obtain monolayer MoS 2 with electrical uniformity on 200 mm wafers, as well as a high material quality with an electron mobility of ~35.9 cm 2 V -1 s -1 . Finally, we demonstrate a silicon-CMOS-compatible BEOL fabrication process flow for MoS 2 transistors; the performance of these silicon devices shows negligible degradation (current variation < 0.5%, threshold voltage shift < 20 mV). We believe that this is an important step towards monolithic 3D integration for future electronics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

νBDX: a Coherent Elastic Neutrino Nucleus Scattering (CEνNS) experiment at Jefferson Lab

Particle physics is an ever-changing field seeking to explain phenomena that lie at the limits of our current knowledge. Among discovered and hypothesized interactions, Coherent Elastic Neutrino-Nucleus Scattering (CE?NS) stands out as a fascinating and elusive phenomenon, offering a unique window into the nature of neutrinos and their interactions with matter. CE?NS, a process predicted by the Standard Model, represents one of the subtle ways in which neutrinos can interact with atomic nuclei. Unlike other neutrinonucleus interactions, CE?NS occurs coherently, meaning that the entire nucleus collectively responds to the neutrino-mediated weak force, resulting in small energy transfers to the nucleus as a whole. The extremely rare nature of CE?NS events presents a formidable challenge to experimenters seeking to detect and study these interactions. Recent advances in detector technologies and the implementation of large-scale experiments, such as coherent neutrino scattering experiments at research facilities around the world, have opened up new avenues for exploring this elusive phenomenon. These experiments aim not only to observe CE?NS directly but also to extract valuable information on neutrino properties, nuclear structure, and potential deviations from the Standard Model. This thesis aims to study the feasibility of an experiment to study CE?NS at The Thomas Jefferson National Accelerator Facility, Newport News, VA, USA. This would be an experiment that exploits the production of neutrinos by an electron beam dumped on a thick target (the beam dump). The large quantity of neutrinos produced and their energy profile are well suited to the purpose of studying the CE?NS. In my thesis, I will start from previous studies on CE?NS and from theoretical considerations regarding the process, then quantify the expected events for a hypothetical experiment and possible backgrounds through simulations aimed at optimizing the geometry of the future detector. I will also show some tests on selected detector components that will be part of a first prototype.

Grazzi, Stefano↗
DOE OSTI2024

Adjusting the Energy Profile for CH–O Interactions Leads to Improved Stability of RNA Stem-Loop Structures in MD Simulations

The role of ribonucleic acid (RNA) in biology continues to grow, but insight into important aspects of RNA behavior is lacking, such as dynamic structural ensembles in different environments, how flexibility is coupled to function, and how function might be modulated by small molecule binding. In the case of proteins, much progress in these areas has been made by complementing experiments with atomistic simulations, but RNA simulation methods and force fields are less mature. It remains challenging to generate stable RNA simulations, even for small systems where well-defined, thermostable structures have been established by experiments. Further many different aspects of RNA energetics have been adjusted in force fields, seeking improvements that are transferable across a variety of RNA structural motifs. In this work, the role of weak CH···O interactions is explored, which are ubiquitous in RNA structure but have received less attention in RNA force field development. By comparing data extracted from high-resolution RNA crystal structures to energy profiles from quantum mechanics and force field calculations, it is shown that CH···O interactions are overly repulsive in the widely used Amber RNA force fields. A simple, targeted adjustment of CH···O repulsion that leaves the remainder of the force field unchanged was developed. Then, the standard and modified force fields were tested using molecular dynamics (MD) simulations with explicit water and salt, amassing over 300 μs of data for multiple RNA systems containing important features such as the presence of loops, base stacking interactions as well as canonical and noncanonical base pairing. In this work and others, standard force fields lead to reproducible unfolding of the NMR-based structures. Including a targeted CH···O adjustment in an otherwise identical protocol dramatically improves the outcome, leading to stable simulations for all RNA systems tested.

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

IRIS-DMEM: Efficient Memory Management for Heterogeneous Computing

This paper proposes an efficient data memory management approach for the Intelligent RuntIme System (IRIS) heterogeneous computing framework along with new data transfer policies. IRIS provides a task-based programming model for extreme heterogeneous computing (e.g., CPU, GPU, DSP, FPGA) with support for today's most important programming languages (e.g., OpenMP, OpenCL, CUDA, HIP, OpenACC). However, the IRIS framework either forces the programmer to introduce data transfer commands for each task or relies on suboptimal memory management for automatic and transparent data transfers. The work described here extends IRIS with novel heterogeneous memory handling and introduces novel data transfer policies by employing the Distributed data MEMory handler (DMEM) for efficient and optimal movement of data among the various computing resources. The proposed approach achieves performance gains of up to 7× for tiled LU factorization and tiled DGEMM (i.e., matrix multiplication) benchmarks. Moreover, this approach also reduces data transfers by up to 71% when compared to previous IRIS heterogeneous memory management handlers. This work compares the performance results of the IRIS framework's novel DMEM with the StarPU runtime and MAGMA math library for GPUs. Experiments show a performance gain of up to 1.95× over StarPU and 2.1× over MAGMA.

Miniskar, Narasinga Rao↗
DOE OSTI2020

Spectroscopic Studies of Charge-Transfer Character and Photoresponses of F 4 TCNQ-Based Donor–Acceptor Complexes

F 4 TCNQ (2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane) is used widely as a hole-doping agent in photoresponsive organic semiconducting materials, yet relatively little is known about the photoresponses of the F 4 TCNQ· - anion generated via doping. Furthermore, there is still relatively little systematic exploration of how the properties of the local material or chemical environment impacts the driving force for generating these charge-transfer complexes. Here we present spectroscopic and photophysical studies of F 4 TCNQ in charge-transfer complexes (CTCs) with the electron donor N,N’-Diphenyl-N-N’-di-p-tolylbenzene-1,4-diamine (MPDA) both in dichloroethane solution and polystyrene matrices. Integer charge transfer (ICT) between donor and acceptor occurs readily in dichloroethane solvent to form F 4 TCNQ· - :MPDA + CTCs, due to a ~150 mV difference in MPDA + /MPDA and F 4 TCNQ/F 4 TCNQ· - reduction potentials. Ultrafast spectroscopic studies of the CTC as well as electrochemically generated F 4 TCNQ· - and MDPA + reveal that the photoresponses of these CTCs are dominated by that of the dopant anion, including rapid deactivation (800 fs) after excitation to the anion D 1 excited state, followed by slower (~10 ps) vibrational cooling in the anion D 0 state. Excitation to the higher-lying D 2 state results in a rapid relaxation to the D 1 state, in contrast to direct D 2 -D 0 relaxation previously observed for F 4 TCNQ· - in gas phase. CTCs embedded in polystyrene (PS) matrices are observed to lose their integer charge-transfer character upon evaporation of solvent, as evidenced by changes to electronic and vibrational absorption features associated with F 4 TCNQ· - . This change is attributed to the loss of solvent stabilization of the ion pair formed through the charge-transfer reaction. Ultrafast spectral measurements reveal that the photoresponses of the partial charge-transfer (PCT) species embedded in PS are still highly similar to those of the ICT species and unlike that of neutral F 4 TCNQ, implying the electronic properties of the PCT state are likewise dominated by properties of the reduced acceptor molecule. We conclude that excitation of ICT or PCT states introduces optical losses for photoresponses of doped organic semiconductor materials due to the large anion absorption cross section and its rapid, dissipative deactivation dynamics.

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

Numerical modelling of impact seismic sources using the stress glut theory

SUMMARY Meteorite impacts have proved to be a significant source of seismic signal on the Moon, and have now been recorded on Mars by InSight seismometers. Understanding how impacts produce seismic signal is key to the interpretation of this unique data, and to improve their identification in continuous seismic records. Here, we use the seismic Representation Theorem, and particularly the stress glut theory, to model the seismic motion resulting from impact cratering. The source is described by equivalent forces, some resulting from the impactor momentum transfer, and others from the stress glut, which represents the mechanical effect of plasticity and non linear processes in the source region. We condense these equivalent forces into a point-source with a time-varying single force and nine-component moment tensor. This analytical representation bridges the gap between the complex dynamics of crater formation, and the linear point-source representation classically used in seismology. Using the multiphysics modelling software HOSS, we develop a method to compute the stress glut of an impact, and the associated point-source from hypervelocity impact simulations. For a vertical and an oblique impact at 1000 m s−1, we show that the moment tensor presents a significant deviatoric component. Hence, the source is not an ideal isotropic explosion contrary to previous assumptions, and draws closer to a double couple for the oblique impact. The contribution of the point force to the seismic signal appears negligible. We verify this model by comparing two signals: (1) HOSS is coupled to SPECFEM3D to propagate the near-source signal elastically to remote seismic stations; (2) the point-source model derived from the stress-glut theory is used to generate displacements at the same distance. The comparison shows that the point-source model is accurately simulating the low-frequency impact seismic waveform, and its seismic moment is in trend with Lunar and Martian impact data. High-frequencies discrepancies exist, which are partly related to finite-source effects, but might be further explained by the difference in mathematical framework between classical seismology and HOSS’ numerical modelling.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Interface-modulated kinetic differentials in electron and hole transfer rates as a key design principle for redox photocatalysis by Sb2VO5/QD heterostructures

The efficient conversion of solar energy to chemical energy represents a critical bottleneck to the energy transition. Photocatalytic splitting of water to generate solar fuels is a promising solution. Semiconductor quantum dots (QDs) are prime candidates for light-harvesting components of photocatalytic heterostructures, given their size-dependent photophysical properties and band-edge energies. A promising series of heterostructured photocatalysts interface QDs with transition-metal oxides which embed midgap electronic states derived from the stereochemically active electron lone pairs of p-block cations. Here, we examine the thermodynamic driving forces and dynamics of charge separation in Sb2VO5/CdSe QD heterostructures, wherein a high density of Sb 5s2-derived midgap states are prospective acceptors for photogenerated holes. Hard-x-ray valence band photoemission spectroscopy measurements of Sb2VO5/CdSe QD heterostructures were used to deduce thermodynamic driving forces for charge separation. Interfacial charge transfer dynamics in the heterostructures were examined as a function of the mode of interfacial connectivity, contrasting heterostructures with direct interfaces assembled by successive ion layer adsorption and reaction (SILAR) and interfaces comprising molecular bridges assembled by linker-assisted assembly (LAA). Transient absorption spectroscopy measurements indicate ultrafast (<2 ps) electron and hole transfer in SILAR-derived heterostructures, whereas LAA-derived heterostructures show orders of magnitude differentials in the kinetics of hole (<100 ps) and electron (∼1 ns) transfer. The interface-modulated kinetic differentials in electron and hole transfer rates underpin the more effective charge separation, reduced charge recombination, and greater photocatalytic efficiency observed for the LAA-derived Sb2VO5/CdSe QD heterostructures.

Chemistry↗