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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Anharmonic Exciton‐Phonon Coupling in Metal‐Organic Chalcogenides Hybrid Quantum Wells

Abstract In contrast to inorganic quantum wells, hybrid quantum wells (HQWs) based on metal‐organic semiconductors are characterized by relatively soft lattices, in which excitonic states can strongly couple to lattice phonons. Therefore, understanding the lattice's impact on exciton dynamics is essential for harnessing the optoelectronic potential of HQWs. Beyond 2D metal halide perovskites, layered metal‐organic chalcogenides (MOCs), which are an air‐stable, underexplored material class hosting room‐temperature excitons, can be exploited as photodetectors, light emitting devices, and ultrafast photoswitches. Here, the role of phonons in the optical transitions of the prototypical MOC [AgSePh] ∞ is elucidated. Impulsive stimulated Raman scattering (ISRS) allows the detection of coherent exciton oscillations driven by Fröhlich interaction with low‐energy optical phonons. Steady state absorption and Raman spectroscopies reveal a strong exciton‐phonon coupling (Huang‐Rhys parameter ≈1.7) and its anharmonicity, manifested as a nontrivial temperature‐dependent Stokes shift. The ab initio calculations support these observations, hinting at an anharmonic behavior of the low‐energy phonons <200 cm −1 . These results untangle complex exciton‐phonon interactions in MOCs, establishing an ideal testbed for room‐temperature many‐body phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Validation of magnetized gas-jet experiments to investigate the effects of an external magnetic field on laser-plasma instabilities

Laser-plasma instabilities (LPI) play a detrimental role in energy coupling to the target in inertial confinement fusion (ICF). The recent development of applied strong magnetic fields for use in ICF and laboratory astrophysics experiments has opened opportunities to investigate the role of external magnetic fields on LPIs. Recent numerical studies have shown that stimulated Raman scattering (SRS) can be mitigated by external magnetic fields in the kinetic regime of the instability and warrant systematic experimental studies to validate modelling. To this end, we design experiments at the OMEGA-EP laser facility to investigate the effect of an external perpendicular B-field of 5–30 T on the backscattered light spectrum from a gas-jet target. We present measurements from a proof-of-principle experiment, where the backward-SRS (BSRS) is in the kinetic regime, for which the magnetization is expected to produce the greatest effects on instability growth. New simulations motivated by this experiment are used to inform the proposal of an upgraded experimental design. Our simulation predictions show that the new design is suited to experimentally demonstrating BSRS mitigation by an external magnetic field, despite the magnetization effects on the hydrodynamics, as well as the inherent temporal and spatial variations in plasma conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Attosecond Probing of Coherent Vibrational Dynamics in CBr 4

A coherent vibrational wavepacket is launched and manipulated in the symmetric stretch (a1) mode of CBr 4 , by impulsive stimulated Raman scattering (ISRS) from nonresonant 400 nm laser pump pulses with various peak intensities on the order of tens of 10 12 W/cm 2 . Extreme ultraviolet (XUV) attosecond transient absorption spectroscopy (ATAS) records the wavepacket dynamics as temporal oscillations in XUV absorption energy at the bromine M 4,5 3d 3/2,5/2 edges around 70 eV. The results are augmented by nuclear timedependent Schrödinger equation simulations. Slopes of the (Br 3d 3/2,5/2 ) –1 10a 1 * core-excited state potential energy surface (PES) along the a 1 mode are calculated to be –9.4 eV/Å from restricted open-shell Kohn–Sham calculations. Using analytical relations derived for the small-displacement limit and the calculated slopes of the core-excited state PES, a deeper insight into the vibrational dynamics is obtained by retrieving the experimental excursion amplitude of the vibrational wavepacket and the amount of population transferred to the vibrational first-excited state as a function of pump-pulse peak intensity. Experimentally, the results show that XUV ATAS is capable of resolving oscillations in the XUV absorption energy on the order of a few to tens of meV with tens of femtosecond time precision. This corresponds to change in C–Br bond length on the order of 10 –4 to 10 –3 Å. The results and the analytic relationships offer a clear physical picture, on multiple levels of understanding, of how the pump-pulse peak intensity controls the vibrational dynamics launched by nonresonant ISRS in the small-displacement limit.

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

Microsecond fingerprint stimulated Raman spectroscopic imaging by ultrafast tuning and spatial-spectral learning

Label-free vibrational imaging by stimulated Raman scattering (SRS) provides unprecedented insight into real-time chemical distributions. Specifically, SRS in the fingerprint region (400–1800 cm -1 ) can resolve multiple chemicals in a complex bio-environment. However, due to the intrinsic weak Raman cross-sections and the lack of ultrafast spectral acquisition schemes with high spectral fidelity, SRS in the fingerprint region is not viable for studying living cells or large-scale tissue samples. Here, we report a fingerprint spectroscopic SRS platform that acquires a distortion-free SRS spectrum at 10 cm -1 spectral resolution within 20 µs using a polygon scanner. Meanwhile, we significantly improve the signal-to-noise ratio by employing a spatial-spectral residual learning network, reaching a level comparable to that with 100 times integration. Collectively, our system enables high-speed vibrational spectroscopic imaging of multiple biomolecules in samples ranging from a single live microbe to a tissue slice.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Element- and enantiomer-selective visualization of molecular motion in real-time

Ultrafast optical-domain spectroscopies allow to monitor in real time the motion of nuclei in molecules. Achieving element-selectivity had to await the advent of time resolved X-ray spectroscopy, which is now commonly carried at X-ray free electron lasers. However, detecting light element that are commonly encountered in organic molecules, remained elusive due to the need to work under vacuum. Here, we present an impulsive stimulated Raman scattering (ISRS) pump/carbon K-edge absorption probe investigation, which allowed observation of the low-frequency vibrational modes involving specific selected carbon atoms in the Ibuprofen RS dimer. Remarkably, by controlling the probe light polarization we can preferentially access the enantiomer of the dimer to which the carbon atoms belong.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Mapping wave packet bifurcation at a conical intersection in CH 3 I by attosecond XUV transient absorption spectroscopy

Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH 3 I). Gaseous CH 3 I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH 3 I ground state along the C-I stretch mode (538 ± 7 cm -1 ) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH 3 I are also detected.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Conical intersection and coherent vibrational dynamics in alkyl iodides captured by attosecond transient absorption spectroscopy

The photodissociation dynamics of alkyl iodides along the C–I bond are captured by attosecond extreme-ultraviolet (XUV) transient absorption spectroscopy employing resonant ∼20 fs UV pump pulses. The methodology of previous experiments on CH3I [Chang et al., J. Chem. Phys. 154, 234301 (2021)] is extended to the investigation of a C–I bond-breaking reaction in the dissociative A-band of C2H5I, i-C3H7I, and t-C4H9I. Probing iodine 4d core-to-valence transitions in the XUV enables one to map wave packet bifurcation at a conical intersection in the A-band as well as coherent vibrations in the ground state of the parent molecules. Analysis of spectroscopic bifurcation signatures yields conical intersection crossing times of 15 ± 4 fs for CH3I, 14 ± 5 fs for C2H5I, and 24 ± 4 fs for i-C3H7I and t-C4H9I, respectively. Observations of coherent vibrations, resulting from a projection of A-band structural dynamics onto the ground state by resonant impulsive stimulated Raman scattering, indirectly reveal multimode C–I stretch and CCI bend vibrations in the A-bands of C2H5I, i-C3H7I, and t-C4H9I.

Chang, Kristina F. (ORCID:000000022315039X)↗
DOE OSTI2023

Effect of overlapping laser beams and density scale length in laser-plasma instability experiments on OMEGA EP

Experiments have been conducted on the OMEGA EP laser facility to study the effect of density scale length and overlapping beam geometry on laser-plasma instabilities near and below the quarter-critical density. Experiments were conducted in both planar geometry (density scale length L n ~ 190 to 300 μm) and spherical geometry (L n ~ 150 μm) with up to four overlapping beams and were designed to have overlapped intensities and density scale lengths comparable to OMEGA spherical experiments, but with many fewer beams. In comparison with previous experiments on OMEGA and National Ignition Facility, it is confirmed that shorter density scale lengths favor the two-plasmon decay (TPD) instability, while longer density scale lengths favor stimulated Raman scattering (SRS). In addition, for experiments at the same scale length and overlapped laser intensity, higher single-beam intensities favor SRS, while a larger number of overlapping beams favor TPD.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Hot electron preheat in hydrodynamically scaled direct-drive inertial confinement fusion implosions on the NIF and OMEGA

Hot electron preheat has been quantified in warm, directly driven inertial confinement fusion implosions on OMEGA and the National Ignition Facility (NIF), to support hydrodynamic scaling studies. These CH-shell experiments were designed to be hydrodynamically equivalent, spanning a factor of 40 in laser energy and a factor of 3.4 in spatial and temporal scales, while preserving the incident laser intensity of 10 15 W/cm 2 . Experiments with similarly low levels of beam smoothing on OMEGA and NIF show a similar fraction (~0.2%) of laser energy deposited as hot electron preheat in the unablated shell on both OMEGA and NIF and similar preheat per mass (~2 kJ/mg), despite the NIF experiments generating a factor of three more hot electrons (~1.5% of laser energy) than on OMEGA (~0.5% of laser energy). This is plausibly explained by more absorption of hot electron energy in the ablated CH plasma on NIF due to larger areal density, as well as a smaller solid angle of the imploding shell as viewed from the hot electron generating region due to the hot electrons being produced at a larger standoff distance in lower-density regions by stimulated Raman scattering, in contrast to in higher-density regions by two-plasmon decay on OMEGA. Finally, the results indicate that for warm implosions at intensities of around 10 15 W/cm 2 , hydrodynamic equivalence is not violated by hot electron preheat, though for cryogenic implosions, the reduced attenuation of hot electrons in deuterium–tritium plasma will have to be considered.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Evolution and hot electron generation of laser–plasma instabilities in direct-drive inertial confinement fusion

A series of 2D in-plane plane wave particle-in-cell simulations find distinctive paths of laser-plasma instability evolution in OMEGA-scale implosions, depending on the initial electron temperature. At low temperatures, two-plasmon decay (TPD) dominates in both initial growth and the steady state. At high temperatures, the initial dominant modes switch to stimulated Raman scattering, but TPD still dominates a steady state characterized by cavitation and Langmuir turbulence. A hot electron scaling is also obtained from the simulations that, when combined with laser/plasma conditions from hydro simulations, can predict hot electron generation in implosions that do not employ smoothing-by-spectral-dispersion (SSD). It also shows that under the same laser/plasma conditions, SSD can reduce hot electron generation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

The anisotropic nature of singlet fission in single crystalline organic semiconductors

The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.

Chemistry↗
DOE OSTI2024

Time-resolved magneto-optical effects in the altermagnet candidate MnTe

α -MnTe is an antiferromagnetic semiconductor with above room temperature T N = 310 K, which is promising for spintronic applications. Recently, it was reported to be an altermagnet, containing bands with momentum-dependent spin splitting; time-resolved experimental probes of MnTe are, therefore, important both for understanding novel magnetic properties and potential device applications. Here, we investigate ultrafast spin dynamics in epitaxial MnTe(001)/InP(111) thin films using pump-probe magneto-optical measurements in the Kerr configuration. At room temperature, we observe an oscillation mode at 55 GHz that does not appear at zero magnetic field. Combining field and polarization dependence, we identify this mode as a magnon, likely originating from inverse stimulated Raman scattering. Magnetic field-dependent oscillations persist up to at least 335 K, which could reflect coupling to known short-range magnetic order in MnTe above T N . Additionally, we observe two optical phonons at 3.6 and 4.2 THz, which broaden and redshift with increasing temperature.

Gray, Isaiah↗
DOE OSTI2020

Generation of gamma radiation by a subterawatt ultrashort laser pulse: optimisation of preplasma and pulse duration

We report an experimental and numerical study of the acceleration of electrons in a plasma interacting with a subterawatt laser pulse (intensity of ∼3 × 10{sup 18} W cm{sup −2} at a pulse duration of 50 fs). A preplasma layer on the surface of a molybdenum target is formed by an additional laser pulse with a duration of 8 ns and an intensity of ∼2 × 10{sup 12} W cm{sup −2}. It is shown that an increase in the laser pulse duration to 1700 fs at a constant energy (and a proportional decrease in intensity) leads to an increase in the yield of bremsstrahlung γ-radiation by more than an order of magnitude when the nanosecond pulse is ahead of the femtosecond one by 15 − 25 ns. Interferometry data and results of diagnostics of optical and γ-radiation of a plasma demonstrate that the collisional ionisation of atoms by electrons oscillating in the field of such a laser pulse plays an essential role in the formation of electron density profile. The sensitivity of the described effect to the level of amplified spontaneous emission is determined, despite the nanosecond pulse impact. Numerical simulations show that at a large pulse duration, the acceleration of electrons is stipulated by the beaking of plasma waves excited during stimulated Raman scattering of laser radiation. (paper)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Decreasing the amplitude of macroscopic quantum fluctuations in the case of transient SRS

It is shown experimentally that, under the conditions of transient stimulated Raman scattering, pumping by two successive orthogonally polarised laser pulses makes it possible to reduce the amplitude of macroscopic quantum energy fluctuations of a Stokes pulse by a factor of 4 in comparison with single-shot pumping. An energy dispersion of 0.9 % for the first Stokes component is obtained in hydrogen at a relative energy dispersion of ytterbium laser pulses of 0.4 %. (nonlinear optical phenomena)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Spectrally selective fundamental core mode suppression in optical fibre containing absorbing rods

The feasibility of making a wavelength-selective fibre filter using fibre with absorbing rods in its silica cladding has been demonstrated theoretically for the first time. The technique described in this paper is of great practical interest for designing fibre lasers and amplifiers emitting at wavelengths where lasing is impeded by the presence of more energetically favourable radiative transitions in the active medium. In addition, the approach proposed here can be used for stimulated Raman scattering suppression. The unique feature of the fundamental core mode suppression mechanism examined is that there is a (bending) controlled spectral width of a region where excess losses are produced. (selection of papers presented at the international workshop on fibre lasers (20 – 24 September 2020, Novosibirsk))

36 MATERIALS SCIENCE↗
DOE OSTI2023

Core-excited states of SF 6 probed with soft-x-ray femtosecond transient absorption of vibrational wave packets

A vibrational wavepacket in SF 6 is created by impulsive stimulated Raman scattering with a few-cycle infrared pulse and mapped simultaneously onto five sulfur core-excited states using table-top soft x-ray transient absorption spectroscopy between 170 to 200 eV. The femtosecond vibrations induce real-time energy shifts of the x-ray absorption, whose amplitude depend strongly on the nature of the core-excited state. The pump laser intensity is used to control the number of vibrational states in the superposition, thereby accessing core-excited levels for various extensions of the S-F stretching motion. This enables the determination of the relative core-level potential energy gradients for the symmetric stretching mode, in good agreement with TDDFT calculations. This experiment demonstrates a new means of characterizing core-excited potential energy curves.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Cogeneration of hot electrons from multiple laser-plasma instabilities

Interactions of two plasmon decay (TPD) and side stimulated Raman scattering (SSRS) were studied using 3-D particle-in-cell simulations under ICF-relevant conditions for linearly and circularly polarized lasers. In the linear stage, SSRS took place under n e = 0.235n c and TPD dominated near the quarter-critical density surface and their growth rates agreed with theory. In the nonlinear stage, SSRS reduced TPD through pump depletion. Hot electrons were found to be first accelerated by the SSRS plasma waves and then by TPD plasma waves through a co-generation mechanism. Compared to the linearly polarized case with the same laser intensity, both SSRS and TPD were reduced due to the lower laser amplitude in the circularly-polarized case. As a result, a 30 percent decrease in hot electron flux was observed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Nonlinear transmission of laser light through coronal plasma due to self-induced incoherence

The success of direct laser-driven inertial con nement fusion (ICF) relies critically on the efficient coupling of laser light to plasma. At ignition scale, the absolute stimulated Raman scattering (SRS) instability can severely inhibit this coupling by redirecting and strongly depleting laser light. This article describes a new dynamic saturation regime of the absolute SRS instability near one quarter of the critical density. The saturation occurs when spatiotemporal ion-acoustic fluctuations in the plasma density detune the instability resonance. Here, the dynamic saturation mitigates the strong depletion of laser light and enhances its transmission through the instability region, explaining the coupling of laser light to ICF targets at higher plasma densities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗