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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 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Improving Excited-State Potential Energy Surfaces via Optimal Orbital Shapes

In this work, we demonstrate that, rather than resorting to high-cost dynamic correlation methods, qualitative failures in excited-state potential energy surface predictions can often be remedied at no additional cost by ensuring that optimal molecular orbitals are used for each individual excited state. This approach also avoids the weighting choices required by state-averaging and dynamic weighting and obviates their need for expensive wave function response calculations when relaxing excited-state geometries. Although multistate approaches are of course preferred near conical intersections, other features of excited-state potential energy surfaces can benefit significantly from our single-state approach. In three different systems, including a double bond dissociation, a biologically relevant amino hydrogen dissociation, and an amino-to-ring intramolecular charge transfer, we show that state-specific orbitals offer qualitative improvements over the state-averaged status quo.

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

Photodissociation Dynamics of CH 2 OO on Multiple Potential Energy Surfaces: Experiment and Theory

UV excitation of the CH 2 OO Criegee intermediate across most of the broad span of the (B 1A') – (X 1A') spectrum results in prompt dissociation to two energetically accessible asymptotes: O ( 1 D) + H 2 CO (X 1 A 1 ) and O ( 3 P) + H 2 CO (a 3A"). Dissociation proceeds on multiple singlet potential energy surfaces that are coupled by two regions of conical intersection (CoIn). Velocity map imaging (VMI) studies reveal a bimodal total kinetic energy (TKER) distribution for the O ( 1 D) + H 2 CO (X 1 A 1 ) products with the major and minor components accounting for ca. 40% and ca. 20% on average of the available energy (E avl ), respectively. The unexpected low TKER component corresponds to highly internally excited H 2 CO (X 1 A 1 ) products accommodating ca. 80% of E avl . Full dimensional trajectory calculations suggest that the bimodal TKER distribution of the O ( 1 D) + H 2 CO (X 1 A 1 ) products originates from two different dynamical pathways: a primary pathway (69%) evolving through one CoIn region to products and a smaller component (20%) sampling both CoIn regions enroute to products. Those that access both CoIn regions likely give rise to the more highly internally excited H 2 CO (X 1 A 1 ) products. The remaining trajectories (11%) dissociate to O ( 3 P) + H 2 CO (a 3 A") products after traversing through both CoIn regions. Here, the complementary experimental and theoretical investigation provides insight on the photodissociation of CH 2 OO via multiple dissociation pathways through two regions of CoIn that control the branching and energy distributions of products.

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

Triple Emission of 5'-( para -R-Phenylene)vinylene-2-(2'-hydroxyphenyl)benzoxazole (PVHBO). Part I: Dual Emission from the Neutral Species

The effects of 5'-(para-R-phenylene)vinylene (PV) substituents on the emission properties of 2-(2'-hydroxyphenyl)benzoxazole (HBO) are analyzed using steady-state and time-resolved absorption and emission spectroscopies in addition to quantum chemical calculations. All members in the series of PVHBOs are capable of excited-state intramolecular proton transfer (ESIPT) with a solvent sensitivity that is typical of a HBO derivative to produce a normal (aka enol) emission and an excited-state tautomer (aka keto) emission. These two emission bands of the neutral dyes are discussed in the current paper. The intermolecular proton transfer, i.e., the deprotonation, of a PVHBO results in the third band of the triple emission, which is described in the succeeding paper. The placement of an electron-withdrawing substituent R on the PVHBO scaffold increases the intensity of the keto emission relative to the enol emission in hydrogen-bonding solvents. The R substituents do not significantly alter the wavelengths of the enol and keto emission bands, which are located in the blue and green regions, respectively, of the visible spectrum. The ultrafast time-resolved spectroscopies and quantum chemical calculations offer explanations on how the R group and the solvent affect the enol and keto emission properties (i.e., wavelength, lifetime, fluorescence quantum yield, and relative ratio of their emissions). Here, the key findings include the following: (1) the emission energies of both enol and keto forms are not sensitively dependent on the R substituent and (2) the solvent-engaged enol excited state is quenched more efficiently as the R substituent becomes more electron-withdrawing. A PVHBO acts as a fusion of HBO and stilbenoid that intersect at the hydroxyphenyl moiety. Depending on the solvent and other environmental conditions, PVHBOs may exhibit the ESIPT property of HBO or the substituent-dependent emission of stilbenoid. This paper and the succeeding article provide a photophysical model of PVHBOs to explain the wavelengths and relative abundances of the three emission bands (enol, keto, and anion) that these compounds are able to produce. Judicial selection of the environmental factors may drive the emission of a PVHBO into the spectral regions of blue, green, and, in a couple of cases, orange or red.

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

An Experimental and Theoretical Study of the Valence Shell Electronic Structure of Nitromethane

Vibrationally resolved CH 3 NO 2 and CD 3 NO 2 photoelectron spectra and angular distribution parameters, β, have been measured in the photon energy range 20–80 eV. This allows a comprehensive investigation of conflicting literature interpretations of the two outermost photoelectron bands, complemented by high-level calculations characterizing the three O lone-pair-based orbital ionizations expected in this region. Franck–Condon simulations allow the regular vibrational progressions observed at the beginning of the first and second bands to be assigned as predominantly modes v 5 and v 6 of the D 0 and D 2 cation states, respectively. Irregular structuring observed midband in both bands is attributed to avoided crossings between the adiabatic D 0 /D 1 and D 1 /D 2 states as identified in potential surface cuts taken along the v 5 and v 6 normal mode coordinates. The associated D 0 /D 1 and D 1 /D 2 conical intersections were located and characterized, allowing possible vibronic coupling and its impact on the photoelectron spectra of the D 0 , D 1 , and D 2 states to be discussed. This helps rationalize the apparently missing D 1 ionization in this region, although some contribution by this state may be identifiable in the β-parameter spectra. Theoretical analysis of the complete valence region spectrum identifies the early breakdown of the independent electron model beyond these first two bands.

Powis, Ivan [University of Nottingham (United King↗
DOE OSTI2021

Suppressing Auger Recombination in Multiply Excited Colloidal Silicon Nanocrystals with Ligand-Induced Hole Traps

Nonradiative Auger recombination in multiply excited nanocrystals is a dominant efficiency loss pathway for nanocrystal-containing optoelectronic devices that rely on high-rate emission and absorption operating conditions. Overcoming Auger recombination in these quantum-confined systems is therefore a longstanding challenge to the synthetic nanocrystal as well as device manufacturing communities. Several successful strategies have been realized to reduce Auger recombination, but they rely on complex and time-consuming nanocrystal core/shell synthesis. Alternatively, controlling Auger rates by varying the nanocrystal–ligand-binding chemistry is a promising route to obtain functional tunability, which reduces the barrier to large-scale manufacturing. The covalent surface chemistry and the extremely long-lived photoexcited lifetimes of silicon nanocrystals (Si NCs) make them a unique system among colloidal semiconductor NCs to study the intersection between surface chemistry and photoexcited carrier dynamics. Here, we show that changing the functional group that binds a saturated dodecyl ligand to the surface of nonthermal plasma-synthesized Si NCs from alkyl to thiolate slows Auger recombination rates within multiply excited Si NCs. This reduction in Auger rate persists across Si NC sizes ranging from 3.5 to 8 nm in diameter, but the expected linear dependence of Auger rates on the NC volume is retained for both alkyl and alkylthiolate surface terminations. To understand the origin behind this elongation, we carry out steady-state and time-resolved photoluminescence measurements as well as time-resolved terahertz spectroscopy measurements. These measurements reveal that thiolate groups introduce mid-gap surface states, which, we argue, reduces the photoexcited electron–hole overlap and elongates Auger recombination times. These results highlight how a typically detrimental chemical species—mid-band gap NC surface states—can be beneficial under high-rate absorption/emission conditions.

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

Insights into the Dynamic Interfacial and Bulk Composition of Copper-Modified, Hydrogen-Alloyed, Palladium Nanocubes under Electrocatalytic Conditions

Understanding and controlling the alloying properties of nanomaterials under electrochemical conditions are critically important for fields ranging from energy storage and catalysis to electrochromic window technology. Hydrogen-absorbing nanomaterials, like palladium, are especially interesting due to their ability to reversibly absorb and store hydrogen in their lattice at near-stoichiometric amounts. Palladium’s work function is also significantly deeper than that of most transition metals, which enables electrochemical underpotential deposition of conformal monolayer and submonolayer amounts of transition metals onto the palladium surface. The simultaneous existence of these two properties is unique and opens new and exciting avenues for electrochemical applications. However, the intersection of surface-modified, hydrogen-alloyed palladium nanomaterials is poorly understood, and specifically, how these structures evolve during electrochemical operating conditions remains an open question. Here, we synthesize {100}-terminated palladium nanocubes and deposit between 0.5 and 22 monolayers of copper at the palladium surface. We then electrochemically alloy these surface-modified structures with hydrogen. Using a combination of analytical electrochemistry, spectroscopy, and microscopy, we track the positional evolution of the Cu at the surface of Pd, its impact on palladium’s ability to absorb hydrogen, and copper’s effect on hydrogen evolution electrocatalysis. We show that Cu readily alloys into the palladium nanocube at potentials more negative than the Cu 2+/0 deposition, but a 0.5 monolayer thick copper layer remains at the Pd surface regardless of potential. Finally, we discuss the implications of these findings within the framework of CO 2 reduction catalysis for carbon–carbon bond-forming chemistry.

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

Entropy-Driven Charge Separation: A Potential Explanation for the Low Energy Loss Found in OPVs with Non-fullerene Acceptors

The recent development of non-fullerene acceptors (NFA) has led to an abrupt increase in the organic photovoltaic (OPV) efficiency from ~12% to ~20%. NFA OPVs can generate photocurrent efficiently without much energy loss, which contrasts with the large energy loss often needed for generating free charges from excitons in fullerene OPVs. Here, we argue that entropy-driven charge separation, which allows excitons to spontaneously gain heat from the environment, is responsible for the exceptionally low energy loss found in NFA OPVs. The entropic driving force is maximized when the delocalized electron and hole wave functions in the CT exciton intersect each other via pointlike junctions. Furthermore, these pointlike junctions are abundant in the polymer/NFA bulk heterojunction which consists of intertwined, stringlike donor and acceptor domains in which electron delocalizes anisotropically. Such microstructure favors entropy-driven charge separation, which can enable charge separation with a minimal energy loss.

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

Photoinduced Charge Transfer and Vibronic Coherence in CdSe Quantum Dots with Methyl Viologen Acceptors

We show herein that photoinduced charge transfer from CdSe quantum dots (QDs) to surface-bound methyl viologen (MV 2+ ) acceptors is mediated by a vibronically coherent, nonadiabatic mechanism. Broadband multidimensional electronic spectra and an analysis of coherences show that a mixed QD–MV charge-transfer (CT) state is populated on the <50 fs time scale after optical preparation of the X3 (1P 3/2 –1P e ) state, well prior to the appearance of the one-electron photoreduced ground state (MV +• ). A partial redistribution of charge from the core of the QD to the acceptor is revealed by excited-state coherences of an out-of-plane vibrational mode local to MV 2+ and of a low-frequency mode mixing a MV 2+ mode with the longitudinal optical (LO) phonon of the QD core. The ultrafast damping of these coherences indicates that excited-state wavepackets travel from the optically prepared, Franck–Condon structure through a conical intersection to reach the CT state. These results suggest that vibronically coherent processes generating CT intermediates can be exploited to improve the efficiency of QD-based solar cells and photocatalysts.

Cadmium selenide↗
DOE OSTI2022

Exact-Factorization-Based Surface Hopping for Multistate Dynamics

A surface-hopping algorithm recently derived from the exact factorization approach, SHXF, introduces an additional term in the electronic equation of surface hopping that couples electronic states through the quantum momentum. Furthermore, this term not only provides a first-principles description of decoherence, but here we show it is crucial to accurately capture nonadiabatic dynamics when more than two states are occupied at any given time. Using a vibronic coupling model of the uracil cation, we show that the lack of this term in traditional surface-hopping methods, including those with decoherence corrections, leads to failure to predict the dynamics through a three-state intersection, while SHXF performs similarly to the multiconfiguration time-dependent Hartree quantum dynamics benchmark.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

High-Level Reverse Intersystem Crossing and Molecular Rigidity Improve Spin Statistics for Triplet–Triplet Annihilation Upconversion

The structural factors affecting triplet−triplet annihilation (TTA) at the molecular level are not well-understood. Here, our steady-state photoluminescence and transient absorption results demonstrate that the spin statistical factor, η, decreases from 0.60 to 0.46 and 0.14 going from 9,10-diphenylanthracene (DPA) to the 1,5-DPA and 2,6-DPA isomers, respectively, during photon upconversion with a platinum octaethylporphyrin sensitizer. Density functional theory (DFT) shows that η depends on the energetics of hot triplet states and molecular rigidity. The significantly high conical intersection energy between the S 0 and T 1 states for 9,10-DPA gives its longer triplet lifetime. Time-dependent DFT calculations show that 9,10-DPA and 1,5-DPA can undergo high-level reverse intersystem crossing from their T 2 and T 3 states, respectively, to the bright S 1 state, increasing the limit of the spin statistical factor. Both factors ultimately serve to enhance the TTA efficiency. Furthermore, this work provides insight into designing molecules for efficient light-emitting and photon upconversion applications.

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

Signatures of Antisymmetric Vibrations in the Ultrafast Dynamics of Quadrupolar Dyes

Antisymmetric molecular vibrations are central to ultrafast, nonadiabatic photophysical and photochemical processes such as conical intersection dynamics, Herzberg–Teller couplings and, potentially, singlet fission. Direct spectroscopic identification of such vibrations is, however, challenging, since they are typically Raman inactive and affect optical transitions only weakly. Here, we report experimental signatures of vibronic couplings to a high-frequency antisymmetric vibration in the excited state dynamics of a quasi-quadrupolar molecule by ultrafast two-dimensional electronic spectroscopy (2DES). The early time, sub-50 fs 2DES maps reveal an asymmetric peak pattern with characteristic low-energy cross-peaks. We show that these peaks arise from stimulated emission transitions from an anharmonic, double-minimum excited state potential energy surface formed by vibronic coupling to a high-frequency antisymmetric mode. Simulations based on a phenomenological essential state model support the results. Our findings offer a new approach for identifying antisymmetric vibrations in ultrafast 2DES and track excited state wavepacket motion before relaxation washes out the spectra.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Complex and Unusual Excited-State Relaxation Dynamics of 9,9′-Bifluorenylidene Revealed by Comprehensive Time-Resolved Spectroscopy and MRSF-TDDFT Calculations

Design of novel photochemical molecular motors often requires molecular building blocks that exhibit rather unusual photoactivity, for which conventional analyses of spectroscopic data can lead to conflicting interpretations. We here systematically investigated the excited-state relaxation dynamics of one such molecule, 9,9′-bifluorenylidene (BF), through comprehensive and complementary integration of ultrafast transient absorption (TA) and femtosecond stimulated Raman (FSRS) spectroscopies and first-principles mixed-reference spin-flip time-dependent density functional theory (MRSF-TDDFT). TA and FSRS identified two sequentially formed transients following photoexcitation. The decay kinetics of the two intermediates differ in response to excitation wavelengths and the viscosity/polarity of solvents. MRSF-TDDFT calculations reveal a direct, barrierless internal-conversion pathway from the bright Franck−Condon state to a dark S1 minimum, where the excited-state population is transiently trapped, accounting for the first transient species observed in spectroscopic experiments. Further tracking down along the PES with MRSF-TDDFT mapped out two nonradiative relaxation pathways via conical intersections that connect the dark S 1 state to three configurations in the ground-state manifolds, within which a ring structure with a C8−C8′ bond and the vibrationally excited ground-state BF were identified from spectroscopic and kinetic data. The complexity of relaxation kinetics was attributed to the flexible torsional and twisting motions about the C9−C9′ bridge bond enabled by the diradical character of the S 1 state. These findings clarify unusual photoactive relaxation dynamics stemming from a novel correlation between structural flexibility and shifting electronic characteristics, and they demonstrate the importance of integrating spectroscopic and advanced electronic structure calculation studies for judicious clarification of complex, competing relaxation pathways of excited states.

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

Random Knotting in Fractal Ring Polymers

Many ring polymer systems of physical and biological interest exhibit both pronounced topological effects and nontrivial self-similarity, but the relationship between these two phenomena has not yet been clearly established. Here, we use theory and simulation to formulate such a connection by studying a fundamental topological property—the random knotting probability—for ring polymers with varying fractal dimension, d f . Using straightforward scaling arguments, we generalize a classic mathematical result, showing that the probability of a trivial knot decays exponentially with chain size, N, for all fractal dimensions: P 0 (N) ∝ exp(–N/N 0 ). However, no such simple considerations can account for the dependence of the knotting length, N 0 , on d f , necessitating a more involved analytical calculation. This analysis reveals a complicated double-exponential dependence, which is well supported by numerical data. By contrast, functional forms typical of simple scaling theories fail to adequately describe the observations. These findings are equally valid for two-dimensional ring polymer systems, where “knotting” is defined as the intersection of any two segments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Frequency Conversion in a Time-Variant Dielectric Metasurface

The color of light is a fundamental property of electromagnetic radiation; as such, control of the frequency is a cornerstone of modern optics. Nonlinear materials are typically used to generate new frequencies, however the use of time-variant systems provides an alternative approach. Utilizing a metasurface that supports a high-quality factor resonance, we demonstrate that a rapidly shifting refractive index will induce frequency conversion of light that is confined in the nanoresonator meta-atoms. We experimentally observe this frequency conversion and develop a time-dependent coupled mode theory model that well describes the system. Finally, the intersection of high quality-factor resonances, active materials, and ultrafast transient spectroscopy leads to the demonstration of metasurfaces operating in a time-variant regime that enables enhanced control over light–matter interaction.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

3D Nanomagnetism in Low Density Interconnected Nanowire Networks

Free-standing, interconnected metallic nanowire networks with densities as low as 40 mg/cm 3 have been achieved over centimeter-scale areas, using electrodeposition into polycarbonate membranes that have been ion-tracked at multiple angles. Networks of interconnected magnetic nanowires further provide an exciting platform to explore 3-dimensional nanomagnetism, where their structure, topology, and frustration may be used as additional degrees of freedom to tailor the materials properties. New magnetization reversal mechanisms in cobalt networks are captured by the first-order reversal curve method, which demonstrate the evolution from strong demagnetizing dipolar interactions to intersection-mediated domain wall pinning and propagation, and eventually to shape-anisotropy dominated magnetization reversal. These findings open up new possibilities for 3-dimensional integrated magnetic devices for memory, complex computation, and neuromorphics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Manipulating Interlayer Excitons for Near-Infrared Quantum Light Generation

Interlayer excitons (IXs) formed at the interface of van der Waals materials possess various novel properties. In parallel development, strain engineering has emerged as an effective means for creating 2D quantum emitters. Here, exploring the intersection of these two exciting areas, we use MoS2/WSe2 heterostructure as a model system and demonstrate how strain, defects, and layering can be utilized to create defect-bound IXs capable of bright, robust, and tunable quantum light emission in the technologically important near-infrared spectral range. Our work presents defect-bound IXs as a promising platform for pushing the performance of 2D quantum emitters beyond their current limitations.

2D heterostructures↗
DOE OSTI2023

Spin Solar Cell Phenomenon on a Single-Molecule Magnet (SMM) Impacted CoFeB-Based Magnetic Tunnel Junctions

The single-molecule magnet (SMM) is demonstrated here to transform conventional magnetic tunnel junctions (MTJs), a memory device used in present-day computers, into solar cells. For the first time, we demonstrated an electronic spin-dependent solar cell effect on an SMM-transformed MTJ under illumination from unpolarized white light. We patterned cross-junction-shaped devices to form a CoFeB/MgO/CoFeB-based MTJ. The MgO barrier thickness at the intersection between the two exposed junction edges was less than the SMM extent, which enabled the SMM molecules to serve as channels to conduct spin-dependent transport. The SMM channels yielded a region of long-range magnetic ordering around these engineered molecular junctions. Our SMM possessed a hexanuclear [Mn 6 (μ 3 -O) 2 (H 2 N-sao) 6 (6-atha) 2 (EtOH) 6 ] [H 2 N-saoH = salicylamidoxime, 6-atha = 6-acetylthiohexanoate] complex and thioesters end groups to form bonds with metal films. SMM-doped MTJs were shown to exhibit a solar cell effect and yielded ≈80 mV open-circuit voltage and ≈10 mA/cm 2 saturation current density under illumination from one sun equivalent radiation dose. A room-temperature Kelvin Probe AFM (KPAFM) study provided direct evidence that the SMM transformed the electronic properties of the MTJ’s electrodes over a lateral area in excess of several thousand times larger in extent than the area spanned by the molecular junctions themselves. As a result, the decisive factor in observing this spin-photovoltaic effect is the formation of SMM spin channels between the two different ferromagnetic electrodes, which in turn is able to catalyze the long-range transformation in each electrode around the junction area.

14 SOLAR ENERGY↗
DOE OSTI2021

Shape-Selective Synthesis of Alkylcyclopentenyl Cations in Zeolites and Spectroscopic Distinction of Constitutional Isomers

Alkylcyclopentenyl cations belong to the long-lived intermediates that make up the “hydrocarbon pool” during the catalytic conversion of methanol on zeolites, and recent works show that such cations contribute to olefin and aromatics formation. From liquid phase chemistry, two types of alkylcyclopentenyl cations are known and distinguished by the substituent at the central carbon (C-2) of the allylic system: a more stable type with a methyl group at the C-2 and a less stable type with hydrogen at the C-2. The following three linked objectives are pursued: (i) IR spectroscopic distinction of the different substitution patterns at the allylic system of alkylcyclopentenyl cations, (ii) the role of the zeolite framework in determining the substitution pattern, and (iii) identification of alkylcyclopentenyl cations from precursors relevant to methanol-to-olefins conversion. UV–vis and IR spectroscopy are applied in situ to characterize alkylcyclopentenyl cations produced by adsorption of a pentaalkylcyclopentadiene or by adsorption and thermally induced cyclization of 2,6-dimethyl-2,4,6-octatriene. Prior knowledge of electronic spectra is combined with DFT-computed and experimental IR spectra to establish the frequency of the C–H vibration of the C-2 hydrogen-substituted type, and a characteristic red shift of the asymmetric allylic stretching vibration (Δν ≈ -20 to -30 cm –1 ) after replacing hydrogen by methyl at the central carbon of the allylic system. Although DFT demonstrates that both types of ions fit into medium- and large-pore zeolites and that the C-2 methyl-substituted type is thermodynamically favored even in the pores of the considered zeolites, formation of alkylcyclopentenyl cations is found by UV–vis and IR spectra to be shape-selective. The bulkier C-2 methyl-substituted type is detected in large-pore zeolites (MOR, BEA) and in the intersections of medium-pore zeolites (MFI), whereas in channels of medium size (TON), the less bulky C-2 hydrogen-substituted type is exclusively formed. Finally, the type of ion formed and its overall size are dictated by the zeolite framework and are independent of the precursor; the same type of alkylcyclopentenyl cation as found through cyclization of dimethyloctatriene could be generated from ethene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗