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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Non-Kasha fluorescence of pyrene emerges from a dynamic equilibrium between excited states

Pyrene fluorescence after a high-energy electronic excitation exhibits a prominent band shoulder not present after excitation at low energies. The standard assignment of this shoulder as a non-Kasha emission from the second-excited state (S 2 ) has been recently questioned. To elucidate this issue, we simulated the fluorescence of pyrene using two different theoretical approaches based on vertical convolution and nonadiabatic dynamics with nuclear ensembles. To conduct the necessary nonadiabatic dynamics simulations with high-lying electronic states and deal with fluorescence timescales of about 100 ns of this large molecule, we developed new computational protocols. The results from both approaches confirm that the band shoulder is, in fact, due to S 2 emission. We show that the non-Kasha behavior is a dynamic-equilibrium effect not caused by a metastable S 2 minimum. However, it requires considerable vibrational energy, which can only be achieved in collisionless regimes after transitions into highly excited states. This strict condition explains why the S 2 emission was not observed in some experiments.

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

Analytical and numerical studies of dark current in radiofrequency structures for short-pulse high-gradient acceleration

High-gradient acceleration is a key research area that could enable compact linear accelerators for future colliders, light sources, and other applications. In the pursuit of high-gradient operation, rf breakdown limits the attainable accelerating gradient in normal-conducting rf structures. Recent experiments at the Argonne Wakefield Accelerator suggest a promising approach: using short rf pulses with durations of a few nanoseconds. Experimental studies show that these 𝒪⁡(1⁢ ⁢ns) rf pulses can mitigate breakdown limitations, resulting in higher gradients. For example, an electric field of nearly 400 MV/m was achieved in an 𝑋-band photoemission gun driven by 6-ns-long rf pulses, with rapid rf conditioning and low dark current observed. Despite these promising results, the short-pulse regime remains an underexplored parameter space, and rf breakdown physics under nanosecond-long pulses requires further investigation. In this paper, we present analytical and numerical simulations of dark current dynamics in accelerating cavities operating in the short-pulse regime. We study breakdown-associated processes spanning different time scales, including field emission, multipacting, and plasma formation, using simulations of the 𝑋-band photogun cavities. The results reveal the advantages of using short rf pulses to reduce dark current and mitigate rf breakdown, offering a path toward a new class of compact accelerators with enhanced performance and reduced susceptibility to breakdown.

Linear accelerators↗
DOE OSTI2024

Energy Level Gradients from Surface to Bulk in Hybrid Metal-Halide Perovskite Thin Films

Variations in local strain, defect densities, and composition of hybrid metal-halide perovskites have been reported to create heterogeneous energy landscapes in thin films, which impact charge-carrier diffusion and recombination dynamics. Here, we employ one- and two-photon transient absorption spectroscopy to selectively probe the dynamics of charge carriers from surface and bulk regions of methylammonium lead bromide thin films. Differences in the transient absorption spectra indicate that an energy gradient of approximately 100 meV is formed between the higher band-gap surface and lower band-gap bulk regions. Thus, during their lifetime, photoexcited carriers move away from the surface to recombine in the bulk, where our experiments detect long-lived charge populations despite the significant band splitting that has conventionally been assumed to inhibit efficient radiative recombination. Supported by first-principles calculations, we demonstrate that bright emission can still arise from the bulk with states that occupy a wide range of momenta in the vicinity of the band extrema, which show strong dipole transitions. Our results report that photoexcitations in the hybrid perovskites avoid defect-rich surface regions, and that particularly strong emission is generated from accumulated excitation populations in the bulk. Published by the American Physical Society 2024

Bourelle, Sean A.↗
DOE OSTI2021

Distinguishing Models for Mixed Halide Lead Perovskite Photosegregation via Terminal Halide Stoichiometry

Photoinduced halide segregation in mixed halide hybrid perovskites [i.e., APb(I 1–x Br x ) 3 ] represents an intrinsic instability that impedes their commercialization. Resolving this issue requires developing a microscopic understanding of the phenomenon. Key to this is distinguishing existing models of halide photosegregation by comparing their corresponding predictions to experiment. In this work, we test the temperature dependency of predicted perovskite terminal stoichiometries (x terminal ), following photosegregation, in single and double cation mixed halide perovskites. Our results show a general temperature invariance of x terminal . This largely supports the idea that band gap difference between parent and halide-segregated perovskite phases drives photosegregation. Beyond this, careful examination of temperature- and halide composition-dependent emission energies suggests an alternative explanation for the enhanced photostability of mixed cation/mixed halide perovskites, linked to band gap energy differences between parent and phase-segregated perovskite phases. Together, our results make inroads in clarifying the microscopic origin of mixed halide perovskite photosegregation and pave the way toward approaches that stabilize their use in applications.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Amplified Spontaneous Emission from Electron–Hole Quantum Droplets in Colloidal CdSe Nanoplatelets

Two-dimensional cadmium selenide nanoplatelets (NPLs) exhibit large absorption cross sections and homogeneously broadened band-edge transitions that offer utility in wide-ranging optoelectronic applications. Here, we examine the temperature-dependence of amplified spontaneous emission (ASE) in 4- and 5-monolayer thick NPLs and show that the threshold for close-packed (neat) films decreases with decreasing temperature by a factor of 2-10 relative to ambient temperature owing to extrinsic (trapping) and intrinsic (phonon-derived line width) factors. Interestingly, for pump intensities that exceed the ASE threshold, we find development of intense emission to lower energy in particular provided that the film temperature is <= 200 K. For NPLs diluted in an inert polymer, both biexcitonic ASE and low-energy emission are suppressed, suggesting that described neat-film observables rely upon high chromophore density and rapid, collective processes. Transient emission spectra reveal ultrafast red-shifting with the time of the lower energy emission. Taken together, these findings indicate a previously unreported process of amplified stimulated emission from polyexciton states that is consistent with quantum droplets and constitutes a form of exciton condensate. For studied samples, quantum droplets form provided that roughly 17 meV or less of thermal energy is available, which we hypothesize relates to polyexciton binding energy. Polyexciton ASE can produce pump-fluence-tunable red-shifted ASE even 120 meV lower in energy than biexciton ASE. Finally, our findings convey the importance of biexciton and polyexciton populations in nanoplatelets and show that quantum droplets can exhibit light amplification at significantly lower photon energies than biexcitonic ASE.

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

Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

Abstract Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2 H MoS 2 for 18 th order harmonic generation; > 20 times higher than 2 H MoS 2 for terahertz emission). We link this giant nonlinear optical response to topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and heralds the applications of topological materials in optoelectronics down to the monolayer limit.

42 ENGINEERING↗
DOE OSTI2023

Multiwavelength analysis of Fermi -LAT blazars with high-significance periodicity: detection of a long-term rising emission in PG 1553+113

ABSTRACT Blazars display variable emission across the entire electromagnetic spectrum, with time-scales that can range from a few minutes to several years. Our recent work has shown that a sample of five blazars exhibit hints of periodicity with a global significance ${\gtrsim}2\, \sigma$ at γ-ray energies, in the range of 0.1 GeV < E < 800 GeV. In this work, we study their multiwavelength emission, covering the X-ray, ultraviolet, optical, and radio bands. We show that three of these blazars present similar periodic patterns in the optical and radio bands. Additionally, fluxes in the different bands of the five blazars are correlated, suggesting a co-spatial origin. Moreover, we detect a long-term (≈10 yr) rising trend in the light curves of PG 1553+113, and we use it to infer possible constraints on the binary black hole hypothesis.

Astronomy & Astrophysics↗
DOE OSTI2024

Synchrotron self-Compton in a radiative-adiabatic fireball scenario: modelling the multiwavelength observations in some Fermi /LAT bursts

Energetic GeV photons expected from the closest and the most energetic Gamma-ray bursts (GRBs) provide a unique opportunity to study the very-high-energy emission as well as the possible correlations with lower energy bands in realistic GRB afterglow models. In the standard GRB afterglow model, the relativistic homogeneous shock is usually considered to be fully adiabatic, however, it could be partially radiative. Based on the external forward-shock scenario in both stellar wind and constant-density medium, we present a radiative-adiabatic analytical model of the synchrotron self-Compton (SSC) and synchrotron processes considering an electron energy distribution with a power-law index of $1\lt p\lt 2$ and $2\le p$. We show that the SSC scenario plays a relevant role in the radiative parameter $\epsilon$, leading to a prolonged evolution during the slow cooling regime. In a particular case, we derive the Fermi/LAT light curves together with the photons with energies $\ge 100$ MeV in a sample of nine bursts from the second Fermi/LAT GRB catalogue that exhibited temporal and spectral indices with $\gtrsim 1.5$ and $\approx 2$, respectively. These events can hardly be described with closure relations of the standard synchrotron afterglow model, and also exhibit energetic photons above the synchrotron limit. We have modelled the multiwavelength observations of our sample to constrain the microphysical parameters, the circumburst density, the bulk Lorentz factor, and the mechanism responsible for explaining the energetic GeV photons.

acceleration of particles↗
DOE OSTI2025

Emission properties of a hybrid metallized diamond(001) photocathode

The spectral emission characteristics of a proof-of-concept hybrid metallized diamond(001) photocathode are presented. The quantum efficiency (QE) is shown to be determined by the photoinjection efficiency across the ohmic contact at the back metallized face, whereas the mean transverse energy (MTE) of the photoemitted electrons is consistent with an (optical)phonon-assisted and momentum-resonant Franck-Condon mechanism [Franck-Condon electron emission from polar semiconductor photocathodes, Phys. Rev. Appl. 23, 054065 (2025)] following electron drift transport to the untreated diamond(001) front emission face. Emission is observed from both the lower and upper conduction bands of diamond with positive and negative electron affinity, respectively. A potential route to the realization of a red-visible photocathode based on this concept with a sub-50 meV MTE and a QE greater than 0.1% is discussed.

Density of states↗
DOE OSTI2026

Searching for synchrotron emission from the geminga TeV halo using the planck satellite

Pulsars convert a significant fraction of their total spin-down power into very high-energy electrons, leading to the formation of TeV halos. While these halos are well characterized at TeV energies, it remains unclear whether pulsars also accelerate electrons efficiently at lower energies and how these particles propagate through their surrounding environments. We aim to test whether synchrotron emission from $\sim 50$–$300 \, \textrm{GeV}$ electrons around the Geminga pulsar can be detected in the frequency range observed by the Planck satellite. This would help constrain low-energy particle acceleration and diffusion in the vicinity of pulsars. We model the expected synchrotron emission from Geminga’s TeV halo based on various diffusion and injection spectrum scenarios and compare these predictions to publicly available multi-frequency Planck data. We find no conclusive evidence of spatially extended synchrotron emission associated with Geminga in any of Planck’s frequency bands. Our calculations show that even under favorable diffusion and injection conditions, the predicted synchrotron flux lies well below Planck’s measured background levels.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Quantum Light Emission from Coupled Defect States in DNA-Functionalized Carbon Nanotubes

Solid-state single-photon sources are essential building blocks for quantum photonics and quantum information technologies. This study demonstrates promising single-photon emission from quantum defects generated in single-wall carbon nanotubes (SWCNTs) by covalent reaction with guanine nucleotides in their single-stranded DNA coatings. Low-temperature photoluminescence spectroscopy and photon-correlation measurements on individual guanine-functionalized SWCNTs (GF-SWCNTs) indicate that multiple, closely spaced guanine defect sites within a single ssDNA strand collectively form an exciton trapping potential that supports a localized quantum state capable of room-temperature single-photon emission. In addition, exciton traps from adjacent ssDNA strands are weakly coupled to give cross-correlations between their separate photon emissions. Theoretical modeling identifies coupling mechanism as a capture of band-edge excitons. Finally, because the spatial pattern of nanotube functionalization sites can be readily controlled by selecting ssDNA base sequences, GF-SWCNTs should become a versatile family of quantum light emitters with engineered properties.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnetosphere Evolution and Precursor-driven Electromagnetic Signals in Merging Binary Neutron Stars

We detail new force-free simulations to investigate magnetosphere evolution and precursor electromagnetic (EM) signals from binary neutron stars. Our simulations fully follow a representative inspiral motion, capturing the intricate magnetospheric dynamics and their impact on EM outflows. We explore a range of stellar magnetic moment orientations and relative strengths, finding that the magnetospheres and Poynting flux evolution are strongly configuration dependent. The Poynting flux exhibits pulsations at twice the orbital frequency, 2Ω, and is highly anisotropic, following a power-law dependence on orbital frequency. The index ranges from 1 to 6, shaped by the intricate dynamics of the magnetospheres. Furthermore, we present the first computation of (1) the EM forces acting on the star surfaces, revealing the presence of torques that, for highly magnetized stars, could influence the orbital dynamics or break the crust; (2) the high-energy emission signals from these systems by adopting the established isolated pulsar theory. Assuming curvature radiation in the radiation-reaction limit, we find that photons could reach TeV–PeV energies in the last ∼ms for magnetic field strengths 10 10 –10 15 G. However, our analysis of single photon magnetic pair production suggests that these photons are unlikely to escape, with the MeV band emerging as a promising observational window for precursor high-energy emission. In this framework, we construct high-energy emission skymaps and light curves, exploring observational implications. Finally, we propose potential precursor radio emission and delayed afterglow echoes from magnetized outflows, which may contribute to late-time rebrightening in short gamma-ray bursts or to orphan afterglows.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

BASS XXXII: Studying the Nuclear Millimeter-wave Continuum Emission of AGNs with ALMA at Scales ≲100–200 pc

To understand the origin of nuclear (≲100 pc) millimeter-wave (mm-wave) continuum emission in active galactic nuclei (AGNs), we systematically analyzed subarcsecond resolution Band-6 (211–275 GHz) Atacama Large Millimeter/submillimeter Array data of 98 nearby AGNs (z < 0.05) from the 70 month Swift/BAT catalog. The sample, almost unbiased for obscured systems, provides the largest number of AGNs to date with high mm-wave spatial resolution sampling (~1–200 pc), and spans broad ranges of 14–150 keV luminosity {$40\lt \mathrm{log}[{L}_{14-150}/(\mathrm{erg}\,{{\rm{s}}}^{-1})]\lt 45$}, black hole mass $[5\lt \mathrm{log}({M}_{\mathrm{BH}}/{M}_{\odot })\lt 10$], and Eddington ratio ($-4\lt \mathrm{log}{\lambda }_{\mathrm{Edd}}\lt 2$). We find a significant correlation between 1.3 mm (230 GHz) and 14–150 keV luminosities. Its scatter is ≈0.36 dex, and the mm-wave emission may serve as a good proxy of the AGN luminosity, free of dust extinction up to N H ~ 10 26 cm –2 . While the mm-wave emission could be self-absorbed synchrotron radiation around the X-ray corona according to past works, we also discuss different possible origins of the mm-wave emission: AGN-related dust emission, outflow-driven shocks, and a small-scale (<200 pc) jet. The dust emission is unlikely to be dominant, as the mm-wave slope is generally flatter than expected. Also, due to no increase in the mm-wave luminosity with the Eddington ratio, a radiation-driven outflow model is possibly not the common mechanism. Furthermore, we find independence of the mm-wave luminosity on indicators of the inclination angle from the polar axis of the nuclear structure, which is inconsistent with a jet model whose luminosity depends only on the angle.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

MeV–GeV Gamma-Ray Emission from SNR G327.1–1.1 Discovered by the Fermi-LAT

Abstract We report the discovery of MeV–GeV γ -ray emission by the Fermi-LAT positionally coincident with the TeV pulsar wind nebula (PWN) HESS J1554–550 within the host supernova remnant (SNR) G327.1–1.1. The γ -ray emission is point-like and faint but significant (>4 σ ) in the 300 MeV–2 TeV energy range. We report here the Fermi-LAT analysis of the observed γ -ray emission followed by a detailed multiwavelength investigation to understand the nature of the emission. The central pulsar powering the PWN within G327.1–1.1 has not been detected in any wave band; however, it is likely embedded within the X-ray nebula, which is displaced from the center of the radio nebula. The γ -ray emission is faint and therefore a pulsation search to determine if the pulsar may be contributing is not feasible. Prior detailed multiwavelength reports revealed an SNR system that is old, τ ∼ 18,000 yr, where the interaction of the reverse shock with the PWN is underway or has recently occurred. We find that the γ -ray emission agrees remarkably well with a detailed broadband model constructed in a prior report based on independent hydrodynamical and semianalytic simulations of an evolved PWN. We further investigate the physical implications of the model for the PWN evolutionary stage incorporating the new Fermi-LAT data and attempt to model the distinct particle components based on a spatial separation analysis of the displaced PWN counterparts.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

New Identifications and Multiwavelength Properties of Extragalactic Fermi Gamma-Ray Sources in the SPT-SZ Survey Field

he fourth Fermi Large Area Telescope catalog (4FGL) contains 5064 $\ γ$-ray sources detected at high significance, but 26% of them still lack associations at other wavelengths. The SPT-SZ survey, conducted between 2008 and 2011 with the South Pole Telescope (SPT), covers 2500 deg 2 of the southern sky in three millimeter-wavelength (mm) bands and was used to construct a catalog of nearly 5000 emissive sources. In this study, we introduce a new cross-matching scheme to search for multiwavelength counterparts of extragalactic $\ γ$-ray sources using a mm catalog. We apply a Poissonian probability to evaluate the rate of spurious false associations and compare the multiwavelength associations from the radio, mm, near-infrared, and X-ray with 4FGL $\ γ$-ray sources. In the SPT-SZ survey field, 85% of 4FGL sources are associated with mm counterparts. These mm sources include 94% of previously associated 4FGL sources and 56% of previously unassociated 4FGL sources. The latter group contains 40 4FGL sources for which SPT has provided the first identified counterparts. Nearly all of the SPT-associated 4FGL sources can be described as flat-spectrum radio quasars or blazars. We find that the mm band is the most efficient wavelength for detecting $\ γ$-ray blazars when considering both completeness and purity. We also demonstrate that the mm band correlates better to the $\ γ$-ray band than the radio or X-ray bands. With the next generation of CMB experiments, this technique can be extended to greater sensitivities and more sky area to further complete the identifications of the remaining unknown $\ γ$-ray blazars.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Receiving flat bands near the Fermi level in 1T-VSe2 by using angle resolved photoemission spectroscopy

Here, we study the surface electronic structure of 1T-VSe 2 by means of angle resolved photoemission spectroscopy and uncover a dispersion-less emission located in the vicinity of the Fermi level. Its crystal momentum dependency reveals that it occupies large portions of the Brillouin zone (BZ), where no bulk band is expected. Upon electron doping (deposition of Rb-atoms), the system evolves in a surprising way. Besides the expected down-shifting of the bands, a splitting of both bulk and dispersion-less emission is observed. This peculiar behavior strongly suggests the intrinsic nature of the dispersion-less emission. Its characterization may therefore be relevant to a deeper understanding of the physics of transition metal dichalcogenides.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

A fully kinetic model for orphan gamma-ray flares in blazars

ABSTRACT Blazars emit a highly variable non-thermal spectrum. It is usually assumed that the same non-thermal electrons are responsible for the IR-optical-UV emission (via synchrotron) and the gamma-ray emission (via inverse Compton). Hence, the light curves in the two bands should be correlated. Orphan gamma-ray flares (i.e. lacking a luminous low-frequency counterpart) challenge our theoretical understanding of blazars. By means of large-scale two-dimensional radiative particle-in-cell simulations, we show that orphan gamma-ray flares may be a self-consistent by-product of particle energization in turbulent magnetically dominated pair plasmas. The energized particles produce the gamma-ray flare by inverse Compton scattering an external radiation field, while the synchrotron luminosity is heavily suppressed since the particles are accelerated nearly along the direction of the local magnetic field. The ratio of inverse Compton to synchrotron luminosity is sensitive to the initial strength of turbulent fluctuations (a larger degree of turbulent fluctuations weakens the anisotropy of the energized particles, thus increasing the synchrotron luminosity). Our results show that the anisotropy of the non-thermal particle population is key to modelling the blazar emission.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

One dimensional temperature measurements by resonantly ionized photoemission thermometry of molecular nitrogen

This paper presents an extensive parameter study of a non-intrusive and non-seeded laser diagnostic method for measuring one dimensional (1D) rotational temperature of molecular nitrogen (N 2 ) at 165 - 450 K. Compared to previous efforts using molecular oxygen, here resonantly ionized and photoelectron induced fluorescence of molecular nitrogen for thermometry (N 2 RIPT) was demonstrated. The RIPT signal is generated by directly probing various rotational levels within the rovibrational absorption band of N 2 , corresponding to the 3-photon transition of N 2 ( X 1 Σ g + , v =0→ b 1 Π u , v ′ =6) near 285 nm, without involving collisional effects of molecular oxygen and nitrogen. The photoionized N 2 produces strong first negative band of N 2 + ( B 2 Σ u + − X 2 Σ g + ) near 390 nm, 420 nm, and 425 nm. Boltzmann analyses of various discrete fluorescence emission lines yield rotational temperatures of molecular nitrogen. By empirically choosing multiple rotational levels within the absorption band, non-scanning thermometry can be accurately achieved for molecular nitrogen. It is demonstrated that the N 2 RIPT technique can measure 1D temperature profile up to ∼5 cm in length within a pure N 2 environment. Multiple wavelengths are thoroughly analyzed and listed that are accurate for RIPT for various temperature ranges.

McCord, Walker (ORCID:0000000179747550)↗