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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Measurement of the conduction band spin-orbit splitting in $\mathrm{WSe_2}$ and $\mathrm{WS_2}$ monolayers

We have investigated charge tunable devices based on $\mathrm{WSe_2}$ and $\mathrm{WS_2}$monolayers encapsulated in hexagonal boron nitride. In addition to the well-known radiative recombination of neutral and charged excitons, stationary photoluminescence measurements highlight a weaker-intensity optical transition that appears when the monolayer is electrostatically doped with electrons. We have carried out a detailed characterization of this photoluminescence line based on its doping dependence, its variation as a function of the optical excitation power, its polarization characteristics, and its g factor measured under longitudinal magnetic field. We interpret this luminescence peak as an impurity-assisted radiative recombination of the intervalley negatively charged exciton (triplet trion). In addition to the standard direct recombination, the triplet trion has a second recombination channel triggered by elastic scattering off the short-range impurity potential. The energy difference between the emitted photons from these two possible recombination processes of the same triplet trion is simply the single-particle conduction band spin-orbit splitting Δ c . We measure Δ c = 12 ± 0.5 meV for the $\mathrm{WSe_2}$ monolayer and Δ c = 12 ± 1 meV for the $\mathrm{WS_2}$ monolayer. Here, these results demonstrate the importance of second-order exciton recombination processes in transition-metal dichalcogenide structures.

2-dimensional systems↗
DOE OSTI2025

Highly Tunable Valley Polarization of Potential-Trapped Moiré Excitons in WSe 2 /WS 2 Heterojunctions

Moiré superlattices created by stacking atomic layers of transition metal dichalcogenide semiconductors have emerged as a class of fascinating artificial photonic and electronic materials. An appealing attribute of these structures is the inheritance of the valley degree of freedom from the constituent monolayers. Recent studies show evidence that the valley polarization of the moiré excitons is highly tunable. In heterojunctions of WSe 2 /WS 2 , marked improvement in valley polarization is observed by increasing optical excitation power, a behavior that is quite distinct from the monolayers, and lacks a clear understanding so far. Here, in this Letter, we show that this highly tunable valley property arises from filling of the moiré superlattice, which provides an intriguing mechanism for engineering these quantum opto-valleytronic platforms. Our data further demonstrate that the long-range electron-hole exchange interaction, despite being significantly weakened in the junctions, is the dominant source of moiré exciton intervalley scattering at low population. Using magnetic field tuning, we quantitatively determine the exchange interaction strength to be 0.03 and 0.24 meV for 0° and 60° twisted samples, respectively, in our experiments, about 1 order of magnitude weaker than that in the monolayers.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Coupled Charge and Radiation Transport Processes in Thermophotovoltaic and Thermoradiative Cells

Accurate modeling of charge transport and both thermal and luminescent radiation is crucial to the understanding and design of radiative thermal energy converters. Charge-carrier dynamics in semiconductors are well-described by the Poisson-drift-diffusion equations, and thermal radiation in emitter-absorber structures can be computed using multilayer fluctuational electrodynamics. These two types of energy flows interact through radiation absorption or luminescence and charge-carrier generation or recombination. However, past research has typically only assumed limited interaction, with thermal radiation absorption as an input for charge-carrier models to predict device performance. To examine this assumption, we develop a fully coupled iterative model of charge and radiation transport in semiconductor devices, and we use our model to analyze near-field and far-field GaSb thermophotovoltaic and thermoradiative systems. By comparing our results with past methods that do not consider cross-influences between charge and radiation transport, we find that a fully coupled approach is necessary to accurately model photon recycling and near-field enhancement of external luminescence. As these effects can substantially alter device performance, our modeling approach can aid in the design of efficient thermophotovoltaic and thermoradiative systems.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2026

Using Explainable Artificial Intelligence to Predict Perovskite Solar Cell Electrical Metastability from Operando Photoluminescence Images in Accelerated Stress Testing

Metal halide perovskite (MHP) solar cells exhibit a metastable response to bias governed by coupled ionic–electronic processes, complicating the conventional reciprocity relation between luminescence intensity and device open-circuit voltage (V oc ). This limits the use of luminescence as a diagnostic for device screening or accelerated stress testing, motivating new approaches that can interpret photoluminescence (PL) signals under nonequilibrium conditions. From the artificial intelligence perspective, we develop an explainable deep learning framework that integrates convolutional neural networks (CNN), long short-term memory (LSTM) layers, and an attention mechanism to learn spatiotemporal features from operando photoluminescence PL image sequences. The model achieves a mean absolute error of ±0.027 V in predicting open-circuit voltage transients and reduces extreme-tail errors by up to 78% compared to physics-based reciprocity calculations. Gradient-weighted Class Activation Mapping (Grad-CAM) provides interpretability by highlighting physically meaningful regions such as electrode edges and emergent defect features. From the engineering application perspective, this framework enables accurate, contactless prediction of device V oc and identification of degradation-relevant features during accelerated aging of perovskite solar cells. This approach demonstrates how explainable AI can enhance operando diagnostics and reliability analysis in photovoltaic devices under nonequilibrium conditions.

14 SOLAR ENERGY↗
DOE OSTI2022

Effect of localization on photoluminescence and zero-field splitting of silicon color centers

The study of defect centers in silicon has been recently reinvigorated by their potential applications in optical quantum information processing. A number of silicon defect centers emit single photons in the telecommunication O-band, making them promising building blocks for quantum networks between computing nodes. The two-carbon G-center, self-interstitial W-center, and spin-1/2 T-center are the most intensively studied silicon defect centers, yet despite this, there is no consensus on the precise configurations of defect atoms in these centers, and their electronic structures remain ambiguous. Here, in this work, we employ ab initio density functional theory to characterize these defect centers, providing insight into the relaxed structures, band structures, and photoluminescence spectra, which are compared to experimental results. Motivation is provided for how these properties are intimately related to the localization of electronic states in the defect centers. In particular, we present the calculation of the zero-field splitting for the excited triplet state of the G-center defect as the structure is linearly interpolated from the A-configuration to the B-configuration, showing a sudden increase in the magnitude of the D zz component of the zero-field-splitting tensor. By performing projections onto the local orbital states of the defect, we analyze this transition in terms of the symmetry and bonding character of the G-center defect, which sheds light on its potential application as a spin-photon interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Single detector laser-induced fluorescence imager and raman spectral instrument

Apparatus include divergence optics removably coupled to receive a probe beam in a first imaging mode to cause the probe beam to diverge before impinging on a first area of a target surface, and to not receive the probe beam in a second imaging mode to cause the probe beam to impinge on a second area of the target surface smaller than the first area, collection optics configured to receive, in response to the probe beam, luminescence light emitted from the first area and spectral light emitted from the second area, and an optical detector coupled to the collection optics, wherein the optical detector includes a luminescence imaging detector portion and a spectral imaging detector portion adjacent to the luminescence imaging detector portion, wherein the luminescence imaging detector portion is configured to receive the luminescence light emitted from the first area and the spectral imaging detector portion is configured to receive the spectral light from the second area.

Gasda, Patrick J.↗
DOE OSTI2022

Photophysics and Spin-Physics Studies on Persistent Upconversion Luminescence from Nonlinearly Polarizable Ferroelectric-Like Lattice Prepared by Orderly Packing Donor–Acceptor Structures under Multiphoton Excitation

The ultralong-lived upconversion luminescence with the lifetime of 0.48 s in a broad spectral range (530–650 nm) is observed in CD49 (9-(3-(5-bromopyridin-3-yl)prop-2-yn-1-yl)-9H-carbazole) crystal designed with donor–acceptor (carbazole–pyridine) structures under infrared excitation, simultaneously accompanied with second harmonic generation (SHG). This phenomenon indicates orderly packing donor–acceptor structures form a nonlinearly polarizable ferroelectric-like lattice with ultralong-lived light-emitting states, leading to much prolonged nonlinear optical behaviors. The persistent upconversion luminescence together with SHG is largely reduced when lowering crystallinity. This implies that nonlinearly polarizable ferroelectric-like lattice provides the necessary condition to generate persistent upconversion luminescence. Evidently, persistent upconversion luminescence becomes completely lacking when only using ultralong-lived light-emitting states without nonlinearly polarizable ferroelectric-like lattice, exampled by 4-(dimethylamino)benzonitrile dispersed in polyvinyl alcohol matrix. Magneto-photoluminescence shows that persistent upconversion luminescence is essentially a super-delayed fluorescence from crystalline intermolecular charge-transfer excitons formed in the nonlinearly polarizable ferroelectric-like lattice. Magnetodielectrics indicate crystalline intermolecular charge-transfer excitons are coupled with nonlinearly polarizable ferroelectric-like lattice, leading to prolonged nonlinear optical behaviors shown as persistent upconversion luminescence through super delayed fluorescence. In conclusion, therefore, crystalline intermolecular charge-transfer excitons formed in nonlinearly polarizable ferroelectric-like lattice provide an interesting platform to generate prolonged nonlinear optical behaviors toward developing persistent upconversion luminescence under multiphoton excitation.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe 2 with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Directive giant upconversion by supercritical bound states in the continuum

Photonic bound states in the continuum (BICs), embedded in the spectrum of free-space waves with diverging radiative quality factor, are topologically non-trivial dark modes in open-cavity resonators that have enabled important advances in photonics. However, it is particularly challenging to achieve maximum near-field enhancement, as this requires matching radiative and non-radiative losses. Here we propose the concept of supercritical coupling, drawing inspiration from electromagnetically induced transparency in near-field coupled resonances close to the Friedrich–Wintgen condition. Supercritical coupling occurs when the near-field coupling between dark and bright modes compensates for the negligible direct far-field coupling with the dark mode. This enables a quasi-BIC field to reach maximum enhancement imposed by non-radiative loss, even when the radiative quality factor is divergent. Our experimental design consists of a photonic-crystal nanoslab covered with upconversion nanoparticles. Near-field coupling is finely tuned at the nanostructure edge, in which a coherent upconversion luminescence enhanced by eight orders of magnitude is observed. The emission shows negligible divergence, narrow width at the microscale and controllable directivity through input focusing and polarization. This approach is relevant to various physical processes, with potential applications for light-source development, energy harvesting and photochemical catalysis.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Luminescent solar concentrators and related methods of manufacturing

Luminescent solar concentrators in accordance with various embodiments of the invention can be designed to minimize photon thermalization losses and incomplete light trapping using various components and techniques. Cadmium selenide core, cadmium sulfide shell (CdSe/CdS) quantum dot (“QD”) technology can be implemented in such devices to allow for near-unity QDs and sufficiently large Stokes shifts. Many embodiments of the invention include a luminescent solar concentrator that incorporates CdSe/CdS quantum dot luminophores. In further embodiments, anisotropic luminophore emission can be implemented through metasurface/plasmonic antenna coupling. In several embodiments, red-shifted luminophores are implemented. Additionally, top and bottom spectrally-selective filters, such as but not limited to selectively-reflective metasurface mirrors and polymeric stack filters, can be implemented to enhance the photon collection efficiency. In some embodiments, luminescent solar concentrator component is optically connected in tandem with a planar Si subcell, forming a micro-optical tandem luminescent solar concentrator.

Needell, David R.↗
DOE OSTI2020

Symmetry Effects in Photoinduced Electron Transfer in Chlorin-Quinone Dyads: Adiabatic Suppression in the Marcus Inverted Region

In donor–acceptor dyads undergoing photoinduced electron transfer (PET), a direction or pathway for electron movement is usually dictated by the redox properties and the separation distance between the donor and acceptor subunits, while the effect of symmetry is less recognized. We have designed and synthesized two isomeric donor–acceptor assemblies in which electronic coupling between donor and acceptor is altered by the orbital symmetry control with the reorganization energy and charge transfer exothermicity being kept unchanged. Analysis of the optical absorption and luminescence spectra, supported by the DFT and TD-DFT calculations, showed that PET in these assemblies corresponds to the Marcus inverted region (MIR) and has larger rate for isomer with weaker electronic coupling. This surprising observation provides the first experimental evidence for theoretically predicted adiabatic suppression of PET in MIR, which unambiguously controlled solely by symmetry.

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

A scintillator attenuation spectrometer for intense gamma-rays

A new type of compact high-resolution high-sensitivity gamma-ray spectrometer for short-pulse intense gamma-rays (250 keV to 50 MeV) has been developed by combining the principles of scintillators and attenuation spectrometers. The first prototype of this scintillator attenuation spectrometer (SAS) was tested successfully in Trident laser experiments at LANL. Later versions have been used extensively in the Texas Petawatt laser experiments in Austin, TX, and more recently in OMEGA-EP laser experiments at LLE, Rochester, NY. The SAS is particularly useful for high-repetition-rate laser applications. Furthermore, we give a concise description of the design principles, capabilities, and sample preliminary results of the SAS.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Molecular Origins of Near-Infrared Luminescence in Molybdenum and Tungsten Oxyhalide Perovskites

Materials with near-infrared (near-IR) luminescence are desirable for applications in communications and sensing, as well as biomedical diagnostics and imaging. The most used inorganic near-IR emitters rely on precise doping of host crystal structures with select rare-earth or transition metal ions. Recently, another class of materials with intrinsic near-IR emission has been reported. The compositions of these materials were initially described as vacancy-ordered halide double perovskites Cs 2 MoCl 6 and Cs 2 WCl 6 , but further investigation by some of us on the compound reported as Cs2WCl6 revealed an oxyhalide instead, with a composition Cs 2 WO x Cl 6–x , where 1 < x < 2. Here we demonstrate that the Mo compounds similarly possess the composition Cs 2 MoO x Cl 6–x or Cs 2 MoO x Br 6–x where 1 < x < 2. Preparing the pure halide appears harder for Mo than for W, and we have not succeeded in doing so. The distinctly different composition requires the coordination environment and oxidation state for the Mo and W centers to be reconsidered from what was assumed for the pure halides. In this work, we examine the mechanism for near-IR emission in these materials given their true structures and compositions. We demonstrate that the luminescence is due to the specific d-orbital splitting caused by the presence of oxygen in the distorted [MOX 5 ] 2– octahedra (X is Cl or Br). The fine structure in the emission spectra at low temperatures has been resolved and is attributed to vibronic coupling to the Mo–O and W–O bond stretches. Understanding the true structure and composition of these interesting materials, besides explaining the near-IR luminescence, suggests how this desirable emission can be realized and manipulated.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Back in bismuth: controlling triplet energy transfer, phosphorescence, and radioluminescence via supramolecular interactions

Five bismuth(III)-organic phases that consist of supramolecular assemblies of Bi-2,6-pyridinedicarboxylate structural units and substituted 1,10-phenanthroline molecules (R-Phen; R = H, 5-methyl, 5-chloro, 2,9-dimethyl, and 2,9-dicholoro) were synthesized. All five compounds exhibited solid-state photoluminescence. Whereas the phases containing 2,9-dimethylphenanthroline (Me 2 Phen) and 2,9-dichlorophenanthroline (Cl 2 Phen) displayed solely phosphorescence, the structures built from 5-methylphenanthroline and 5-chlorophenanthroline showed exclusively fluorescence. The remaining phase, consisting of phenanthrolinium, exhibited both fluorescence and phosphoresence. It was determined that phosphorescence arises from triplet state emission (T 1 → S 0 ) of substituted R-Phen units while fluorescence originates from Bi(III) coordinated pyrdinedicarboxylate ligands. Bismuth induces spin–orbit coupling for triplet state population and additionally acts as a heavy metal attenuator for X-ray luminescence (radioluminescence). The electronic structure was mapped and excitation pathway investigated via density functional theory calculations. Computational findings indicate favorable conditions for triplet energy transfer from donor Bi(III)-organic units to acceptor R-Phen derivatives. It is proposed that for the phosphorescent compounds, strong π–π interactions promote electron transfer, whereas the compounds that exhibit purely fluorescence lack any such π–π interactions and undergo triplet energy transfer. In conclusion, these results provide a useful platform for probing structure–property relationships of luminescent bismuth-organic compounds, and specifically highlights the role of noncovalent interactions in achieving room temperature phosphorescence and radioluminescence.

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

Photonic Crystal Waveguides for >90% Light Trapping Efficiency in Luminescent Solar Concentrators

Luminescent solar concentrators are currently limited in their potential concentration factor and solar conversion efficiency by the inherent escape cone losses present in conventional planar dielectric waveguides. Here, we demonstrate that photonic crystal slab waveguides tailored for luminescent solar concentrator applications can exhibit >90% light trapping efficiency. This is achieved by use of quantum dot luminophores embedded within the waveguide that absorb light at photon energies corresponding to photonic crystal leaky modes that couple to incoming sunlight. The luminophores then emit at lower photon energies into photonic crystal bound modes that enable highly efficient light trapping in slab waveguides of wavelength-scale thickness. Photonic crystal waveguides thus nearly eliminate escape cone losses, and overcome the performance limitations of previously proposed wavelength-selective dielectric multilayer filters. We describe designs for hole-array and rod-array photonic crystals comprised of hydrogenated amorphous silicon carbide using CdSe/CdS quantum dots. Our analysis suggests that photonic crystal waveguide luminescent solar concentrators using these materials these can achieve light trapping efficiency above 92% and a concentration factor as high as 100.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Observation of quadrupolar and dipolar excitons in a semiconductor heterotrilayer

Van der Waals (vdW) materials have opened up many avenues for discovery through layer assembly, as epitomized by interlayer dipolar excitons that exhibit electrically tunable luminescence, lasing and exciton condensation. Extending interlayer excitons to more vdW layers, however, raises fundamental questions concerning coherence within excitons and coupling between moiré superlattices at multiple interfaces. Here, by assembling angle-aligned WSe 2 /WS 2 /WSe 2 heterotrilayers, we demonstrate the emergence of quadrupolar excitons. We confirm the exciton’s quadrupolar nature by the decrease in its energy of 12 meV from coherent hole tunnelling between the two outer layers, its tunable static dipole moment under an external electric field and the reduced exciton–exciton interactions. At high exciton density, we also see signatures of a phase of oppositely aligned dipolar excitons, consistent with a staggered dipolar phase predicted to be driven by attractive dipolar interactions. Furthermore, our demonstration paves the way for discovering emergent exciton orderings for three vdW layers and beyond

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Light-driven C–H activation mediated by 2D transition metal dichalcogenides

C–H bond activation enables the facile synthesis of new chemicals. While C–H activation in short-chain alkanes has been widely investigated, it remains largely unexplored for long-chain organic molecules. Here, we report light-driven C–H activation in complex organic materials mediated by 2D transition metal dichalcogenides (TMDCs) and the resultant solid-state synthesis of luminescent carbon dots in a spatially-resolved fashion. We unravel the efficient H adsorption and a lowered energy barrier of C–C coupling mediated by 2D TMDCs to promote C–H activation and carbon dots synthesis. Our results shed light on 2D materials for C–H activation in organic compounds for applications in organic chemistry, environmental remediation, and photonic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Highly luminescent ultra-thin films with rare earth for plasmonic applications

Amphiphilic complexes with luminescent rare earth metal ions suitable for Lanmuir-Blodgett (LB) deposition have been synthesized. LB monolayers with closely packed Eu complexes deposited directly on silver demonstrate significant far-field emission in contrast to the theoretical predictions of full quenching. Angular radiation and polarization patterns of the electric and magnetic dipole emission of Eu 3+ point to a high excitation efficiency of surface plasmon polaritons. Different luminescent behavior of closely packed emitters in comparison to diluted systems is tentatively attributed to the collective state of emitters in LB layers formed via near-field coupling with surface plasmons.

Munga, J.↗