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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 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

The MicroBooNE Single-Photon Low-Energy Excess Search (Public Note 1087)

MicroBooNE is a short baseline neutrino experiment at Fermilab designed to address the low energy excess observed by the MiniBooNE experiment. This note describes and presents preliminary results for the MicroBooNE analysis developed to address this excess as a single photon plus one or zero protons in the final state. The analysis assumes neutrino neutral current Δ resonance production followed by Δ radiative decay on argon (NC Δ → Nγ ) as the "signal model"; event reconstruction and selection have been developed and optimized in order to maximize efficiency and reduce cosmogenic and other beam-related backgrounds to the NC Δ → Nγ signal. We present the analysis methodology and validation checks performed on limited-statistics open data sets, corresponding to 5 x10 19 protons on target (POT), following a blind analysis, as well as the projected sensitivities for testing the Standard Model (SM) predicted rate for the NC Δ → Nγ process and for testing the interpretation of the previously observed MiniBooNE low energy excess as NC Δ → Nγ events, using the full anticipated MicroBooNE data set of 12.25 x 10 20 POT.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Room-Temperature Optical Detection of 14 CO 2 below the Natural Abundance with Two-Color Cavity Ring-Down Spectroscopy

Radiocarbon’s natural production, radiative decay, and isotopic rarity make it a unique tool to probe carbonaceous systems in the life and earth sciences. However, the difficulty of current radiocarbon ( 14 C) detection methods limits scientific adoption. Here, two-color cavity ring-down spectroscopy detects 14 CO 2 in room-temperature samples with an accuracy of one-tenth the natural abundance in 3 min. The intracavity pump–probe measurement uses two cavity-enhanced lasers to cancel out cavity ring-down rate fluctuations and strong one-photon absorption interference (>10 000 1/s) from hot-band transitions of CO 2 isotopologues. Selective, room-temperature detection of small 14 CO 2 absorption signals (<1 1/s) reduces the technical and operational burdens for cavity-enhanced measurements of radiocarbon, which can benefit a wide range of applications like biomedical research and field-detection of combusted fossil fuels.

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

Increasing the Stability of Deep Blue Phosphor‐Sensitized OLEDs Using the Polariton‐Enhanced Purcell Effect

Abstract The stability of efficient, deep blue organic light‐emitting diodes (OLEDs) remains a major challenge in the field of organic electronics. Poor device stability originates from the high probability for destructive non‐radiative triplet exciton annihilation events. Phosphor‐sensitized fluorescence (PSF) is proposed to achieve an efficient, deep blue color by energy transfer from phosphors to fluorophores. Recently, the polariton‐enhanced Purcell (PEP) effect is introduced to decrease the triplet radiative lifetime and density, resulting in an increase in blue phosphorescent OLED lifetime. Here, the PEP effect is introduced to enhance the stability of the PSF‐OLEDs. It is shown that the PEP effect increases all radiative decay rates of the phosphors and fluorophores, leading to a reduction in the triplet annihilation events. Using a Pt‐complex phosphor sensitizer and a so‐called multi‐resonance fluorescent emitter in a PEP cavity, a 3.1‐fold lifetime increase is observed at a current density ofJ= 10 mA cm −2 , reduced EQE roll‐off and deep blue color with Commission Internationale de l'Eclairage coordinates of (0.13, 0.09). The PEP effect maximally extends PSF‐OLED lifetimes in devices with the highest triplet‐to‐singlet energy transfer rates. Moreover, this work suggests that the benefits of PEPs apply to all triplet‐based OLEDs.

Chemistry↗
DOE OSTI2021

Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides

Abstract Low‐dimensional hybrid metal halides are emerging as a highly promising class of single‐component white‐emitting materials for their unique broadband emission from self‐trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure–property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C 5 N 2 H 16 Pb 2 Br 6 , which possesses a highly distorted structure with an initial PLQY of 10%. Compression reduces the overlap between STE states and ground state, leading to a suppressed phonon‐assisted non‐radiative decay. The PL evolution is systematically demonstrated to be controlled by the pressure‐regulated exciton–phonon coupling which can be quantified using Huang–Rhys factor S . Detailed studies of the S ‐PLQY relation for a series of 1D hybrid metal halides (C 5 N 2 H 16 Pb 2 Br 6 , C 4 N 2 H 14 PbBr 4 , C 6 N 2 H 16 PbBr 4 , and (C 6 N 2 H 16 ) 3 Pb 2 Br 10 ) reveal a quantitative structure–property relationship that regulating S factor toward 28 leads to the maximum emission.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Pressure–Modulated Luminescence Enhancement and Quenching in a Hydrogen–Bonded Organic Framework

Light emission in the solid state is central for illumination, sensing, and imaging applications. Unlike luminescence in dilute solutions, where the excited states are unimolecular in nature, intermolecular interaction plays a significant role in the quantum yield of solid-state luminophores, manifested as competing aggregation-caused quenching (ACQ) and aggregation-induced enhancement (AIE). Both effects are extensively studied in various systems; however, it remains unclear how their competition depends on molecular conformation and intermolecular stacking. Here the direct observation of pressure-modulated AIE-ACQ competition in a crystalline hydrogen-bonded organic framework (HOF) is reported. Using in situ spectroscopies and computational modeling, the intramolecular vibration and intermolecular π–π stacking directly responsible for the non-radiative decay of the excited state are identified. The extent of these two contributions is modulated by hydrostatic pressure and guest molecules in the HOF pores. Furthermore, this work demonstrates a physically neat model system to understand and control solid-state luminescence, and a potential material platform for piezoluminescent sensing.

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

Annihilation of electroweak dumbbells

We study the annihilation of electroweak dumbbells and the dependence of their dynamics on initial dumbbell length and twist. Untwisted dumbbells decay rapidly while maximally twisted dumbbells collapse to form a compact sphaleron-like object, before decaying into radiation. The decay products of a dumbbell include electromagnetic magnetic fields with energy that is a few percent of the initial energy. The magnetic field from the decay of twisted dumbbells carries magnetic helicity with magnitude that depends on the twist, and handedness that depends on the decay pathway.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides

The capability of quantum dots to generate both single and multiexcitons can be harnessed for a wide variety of applications, including those that require high optical gain. Here, we use time-correlated photoluminescence (PL) spectroscopy to demonstrate that the isolation of single CdSeTe/ZnS core–shell, nanocrystal quantum dots (QDs) in Zero Mode Waveguides (ZMWs) leads to a significant modification in PL intensity, blinking dynamics, and biexciton behavior. QDs in aluminum ZMWs (AlZMWs) exhibited a 15-fold increase in biexciton emission, indicating a preferential enhancement of the biexciton radiative decay rate as compared to the single exciton rate. The increase in biexciton behavior was accompanied by a decrease in blinking events due to a shortening in the dark state residence time. These results indicate that plasmon mediated enhanced decay rates of QDs in AlZMWs lead to substantial changes in the photophysical properties of single quantum dots, including an increase in biexciton behavior.

photon correlation↗
DOE OSTI2021

Source of Bright Near-Infrared Luminescence in Gold Nanoclusters

Gold nanoclusters with near-infrared (NIR) photoluminescence (PL) have great potential as sensing and imaging materials in biomedical and bioimaging applications. In this work, Au 21 (S-Adm) 15 and Au 38 S 2 (S-Adm) 20 are used to unravel the underlying mechanisms for the improved quantum yields (QY), large Stokes shifts and long PL lifetimes in gold nanoclusters. Both nanoclusters show decent PL QY. In particular, the Au 38 S 2 (S-Adm) 20 nanocluster shows a bright NIR PL at 900 nm with QY up to 15% in normal solvents (such as toluene) at ambient conditions. The relatively lower QY for Au 21 (S-Adm) 15 (4%) compared to Au 38 S 2 (S-Adm) 20 is attributed to the lowest-lying excited state being symmetry-disallowed, as evidenced by the pressure-dependent anti-spectral shift of the absorption spectra compared to PL. Yet, Au 21 (S-Adm) 15 maintains some emissive properties due to a nearby symmetry-allowed excited state. Furthermore, our results show that suppression of non-radiative decay due to the surface “lock rings” which encircle the Au kernel and the surface “lock atoms” which bridge the fundamental Au-kernel units (e.g., tetrahedra, icosahedra, etc.) is the key to obtain high QYs in gold nanoclusters. Here, the complicated excited-state processes and the small absorption coefficient of the band-edge transition lead to the large Stokes shifts and the long PL lifetimes that are widely observed in gold nanoclusters.

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

Control of Photoswitching Kinetics with Strong Light–Matter Coupling in a Cavity

Most photochemistry occurs in the regime of weak light–matter coupling, in which a molecule absorbs a photon and then performs photochemistry from its excited state. In the strong coupling regime, enhanced light–matter interactions between an optical field and multiple molecules lead to collective hybrid light–matter states called polaritons. This strong coupling leads to fundamental changes in the nature of the excited states including multi-molecule delocalized excitations, modified potential energy surfaces, and dramatically altered energy levels relative to non-coupled molecules. Here, the effect of strong light–matter coupling on covalent photochemistry has not been well explored. Photoswitches undergo reversible intramolecular photoreactions that can be readily monitored spectroscopically. In this work, we study the effect of strong light–matter coupling on the kinetics of photoswitching within optical cavities. Reproducing prior experiments, photoswitching of spiropyran/merocyanine photoswitches is decelerated in a cavity. Fulgide photoswitches, however, show the opposite effect, with strong coupling accelerating photoswitching. While modified merocyanine switching can be explained by changes in radiative decay rates or the amount of light in the cavity, modified fulgide switching kinetics suggest direct changes to excited-state reaction kinetics.

Cavities↗
DOE OSTI2021

Signatures of moiré trions in WSe 2 /MoSe 2 heterobilayers

Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators superconductors and generalized Wigner crystals2. When excitons are confined by a moiré superlattice, a new class of exciton emerges, which holds promise for realizing artificial excitonic crystals and quantum optical effects. When such moiré excitons are coupled to charge carriers, correlated states may arise. However, no experimental evidence exists for charge-coupled moiré exciton states, nor have their properties been predicted by theory. In this work, we report the optical signatures of trions coupled to the moiré potential in tungsten diselenide/molybdenum diselenide heterobilayers. The moiré trions show multiple sharp emission lines with a complex charge-density dependence, in stark contrast to the behaviour of conventional trions. We infer distinct contributions to the trion emission from radiative decay in which the remaining carrier resides in different moiré minibands. Variation of the trion features is observed in different devices and sample areas, indicating high sensitivity to sample inhomogeneity and variability. The observation of these trion features motivates further theoretical and experimental studies of higher-order electron correlation effects in moiré superlattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Application of saturation absorption spectroscopy to study the hyperfine structure of 235U and accurate 235U/238U isotope ratio determinations at 861.031 nm

The uranium transition 5f 3 6d7s 2 ( 5 L 6 ) → 5f 3 7s 2 7p ( 5 K 5 ) at 861.031 nm was studied using saturation absorption spectroscopy. The hyperfine structure of the 235 U isotope was determined by measuring the Doppler-suppressed absorption spectrum, and the hyperfine structure constants were obtained by employing transition-specific line strength theory and spectral fitting. The magnetic-dipole and electric-quadrupole constants were determined to be A = -3.2887 ± 0.1957 mK and B = 31.8712 ± 8.0789 mK for the upper state 5f 3 7s 2 7p ( 5 K 5 ). A theoretical calculation for the hyperfine structure constants of the 235 U isotope was also carried out by the relativistic configuration-interaction (RCI) method, and the obtained values were found to be in agreement with the measured values. In addition, the line profile of 238 U was experimentally investigated for different excitation intensities and modeled using the RCI method for estimating the transition probability and oscillator strength, with various residual broadening mechanisms considered beyond the radiative decay. Finally, we show that these results allow us to make improvements on the precision of spectral measurements using our previously developed technique for isotope ratio determinations in atomic beams.

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

Generation of bright monomeric red fluorescent proteins via computational design of enhanced chromophore packing

Red fluorescent proteins (RFPs) have found widespread application in chemical and biological research due to their longer emission wavelengths. Here, we use computational protein design to increase the quantum yield and thereby brightness of a dim monomeric RFP (mRojoA, quantum yield = 0.02) by optimizing chromophore packing with aliphatic residues, which we hypothesized would reduce torsional motions causing non-radiative decay. Experimental characterization of the top 10 designed sequences yielded mSandy1 (λ em = 609 nm, quantum yield = 0.26), a variant with equivalent brightness to mCherry, a widely used RFP. We next used directed evolution to further increase brightness, resulting in mSandy2 (λ em = 606 nm, quantum yield = 0.35), the brightest Discosoma sp. derived monomeric RFP with an emission maximum above 600 nm reported to date. Crystallographic analysis of mSandy2 showed that the chromophore p-hydroxybenzylidene moiety is sandwiched between the side chains of Leu63 and Ile197, a structural motif that has not previously been observed in RFPs, and confirms that aliphatic packing leads to chromophore rigidification. Our results demonstrate that computational protein design can be used to generate bright monomeric RFPs, which can serve as templates for the evolution of novel far-red fluorescent proteins.

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

Rigid cationic ligands enable high-efficiency NIR-II photoluminescence in copper( i ) iodide hybrid semiconductors

Near-infrared (NIR) luminescent materials are pivotal for advanced optoelectronic and biomedical applications, yet attaining efficient emission in the NIR-II region (950-1400 nm) remains challenging. Here, we introduce a ligand cationization strategy for designing copper(i) iodide-organic hybrid materials that emit in the NIR-II region (920-1120 nm) with PLQYs up to 8.58%. By incorporating rigid cationic ligands with CuI modules, we synergistically achieve bandgap narrowing (to 1.51 eV) and structural rigidification via ionic-dative bonding, effectively suppressing non-radiative decay while extending emission beyond 1100 nm. Coupled with solution processability-enabled by the successful synthesis of nanometer-sized nanoparticles in various shapes-and excellent thermal stability (≥210 °C), this work establishes ligand cationization as a universal approach for designing efficient NIR-II emitters.

Chen, Jingwen↗
DOE OSTI2020

Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP

Rydberg states of molecules are intrinsically challenging to study due to the presence of fast non-radiative decay pathways, such as predissociation. However, selectively exciting Rydberg states with values of the orbital angular momentum (ℓ) ℓ ≳ 3 is a productive strategy to minimize this rapid decay and to populate molecular Rydberg states with lifetimes that approach those of atoms. Here, in this proof-of-principle demonstration, we transfer population to an nf Rydberg state of the calcium atom by stimulated Raman adiabatic passage, in which an optical and a millimeter-wave field couple the initial and final states via an intermediate nd Rydberg state. Numerical simulations reproduce the observed time and frequency dependences of the population transfer and suggest the utility of this scheme to populate high-ℓ Rydberg states of molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Experimental validation of a collision-radiation dataset for molecular hydrogen in plasmas

Quantitative spectroscopy of molecular hydrogen has generated substantial demand, leading to the accumulation of diverse elementary process data encompassing radiative transitions, electron-impact transitions, predissociations, and quenching. However, their rates currently available are still sparse, and there are inconsistencies among those proposed by different authors. In this study, we demonstrate an experimental validation of such a molecular dataset by composing a collisional-radiative model (CRM) for molecular hydrogen and comparing experimentally obtained vibronic populations across multiple levels. From the population kinetics of molecular hydrogen, the importance of each elementary process in various parameter space is studied. In low-density plasmas (electron density ne≲1017 m−3) the excitation rates from the ground states and radiative decay rates, both of which have been reported previously, determine the excited state population. The inconsistency in the excitation rates affects the population distribution the most significantly in this parameter space. However, in higher density plasmas (ne≳1018 m−3), the excitation rates from excited states become important, which have never been reported in the literature, and may need to be approximated in some way. In order to validate these molecular datasets and approximated rates, we carried out experimental observations for two different hydrogen plasmas; a low-density radio frequency heated plasma (ne≈1016 m−3) and the Large Helical Device (LHD) divertor plasma (ne≳1018 m−3). The visible emission lines from EF1Σg+, HH¯1Σg+, D1Πu±, GK1Σg+, I1Πg±, J1Δg±, h3Σg+, e3Σu+, d3Πu±,g3Σg+, i3Πg±, and j3Δg± states were observed simultaneously and their population distributions were obtained from their intensities. We compared the observed population distributions with the CRM prediction, in particular the CRM with the rates compiled by Janev et al., Miles et al., and those calculated with the molecular convergent close-coupling (MCCC) method. The MCCC prediction gives the best agreement with the experiment, particularly for the emission from the low-density plasma. However, the population distribution in the LHD divertor shows a worse agreement with the CRM than those from low-density plasma, indicating the necessity of the precise excitation rates from excited states. We also found that the rates for the electron attachment is inconsistent with experimental results. This requires further investigation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Theory of topological exciton insulators and condensates in flat Chern bands

Excitons are the neutral quasiparticles that form when Coulomb interactions create bound states between electrons and holes. Due to their bosonic nature, excitons are expected to condense and exhibit superfluidity at sufficiently low temperatures. In interacting Chern insulators, excitons may inherit the nontrivial topology and quantum geometry from the underlying electron wavefunctions. We theoretically investigate the excitonic bound states and superfluidity in flat-band insulators pumped with light. We find that the exciton wavefunctions exhibit vortex structures in momentum space, with the total vorticity being equal to the difference of Chern numbers between the conduction and valence bands. Moreover, both the exciton binding energy and the exciton superfluid density are proportional to the Brillouin-zone average of the quantum metric and the Coulomb potential energy per unit cell. Spontaneous emission of circularly polarized light from radiative decay is a detectable signature of the exciton vorticity. We propose that the vorticity can also be experimentally measured via the nonlinear anomalous Hall effect, whereas the exciton superfluidity can be detected by voltage-drop quantization through a combination of quantum geometry and Aharonov–Casher effect. Topological excitons and their superfluid phase could be realized in flat bands of twisted Van der Waals heterostructures.

Science & Technology - Other Topics↗
DOE OSTI2025

Enhanced search for neutral current Δ radiative single-photon production in MicroBooNE

We report results from an updated search for neutral current (NC) resonant Δ⁡(1232) baryon production and subsequent Δ radiative decay (NC Δ → 𝑁⁢𝛾). We consider events with and without final state protons; events with a proton can be compared with the kinematics of a Δ⁡(1232) baryon decay, while events without a visible proton represent a more generic phase space. In order to maximize sensitivity to each topology, we simultaneously make use of two different reconstruction paradigms, Pandora and Wire-Cell, which have complementary strengths, and select mostly orthogonal sets of events. Considering an overall scaling of the NC Δ → 𝑁⁢𝛾 rate as an explanation of the MiniBooNE anomaly, our data exclude this hypothesis at 94.4% CL. When we decouple the expected correlations between NC Δ → 𝑁⁢𝛾 events with and without final state protons, our data exclude an interpretation in which all excess events have associated protons at 2.0⁢𝜎, and are consistent with an interpretation in which all excess events have no associated protons at 0.63⁢𝜎.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Quantum states of cylindrical surface charge density for modeling plasmonic circuit elements: Nanowires, nanorods, cavities, and waveguides

Nanostructures in the form of ellipsoids, prolate spheroids, rings, and cylinders are known to exhibit resonant surface and cavity modes with applications in nanophotonics and plasmonics and, more recently, in novel quantum experiments, in which control of plasmons and their interactions with plasmons, photons, phonons, excitons, and quantum emitters are desired. Nanorods and nanowires are examples of plasmonic structures with spectral properties of potential use as interconnects and circuit components. Additionally, estimates of the surface properties of these components are needed in circuit design and integrated systems. Here, we present a quantum Hamiltonian for the cylindrical surface charge density. We then study the photon excitation of plasmons on the cylindrical surface and calculate their scattering and radiative decay rate. Nonradiative decay of plasmons induces an efficient heating of the nanoparticle and can photoacoustically excite mechanical oscillations. Computational calculations are also presented for the plasmonic modes and the ensuing excitations of nanomechanical eigenmodes of nanoparticles with near-cylindrical symmetries.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗