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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 OSTI2024

Multidimensional coherent spectroscopy of light-driven states and their collective modes in multiband superconductors

We present a comprehensive theory of light-controlled multiband superconductivity, and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multidimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multiband BCS superconductors with spatial fluctuations. We consider driving electromagnetic fields determined self-consistently by Maxwell's equations. By calculating the THz-MDCS spectra measured experimentally in the clean SC limit, we identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. They are controlled by a pair of THz laser pulses with well-defined relative phase (pulse pair). The pseudospin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order-parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state. For negligible interband interaction, the spectra show a transition with increasing field, from traditional pump-probe, four-wave-mixing, and third-harmonic generation peaks determined by the laser frequency to sidebands determined by the excitations of the driven system. These sidebands emerge from difference-frequency Raman processes in the nonequilibrium SC state. For interband couplings weaker than the intraband pairing, we show that the Leggett phase collective mode leads to harmonic sidebands around the traditional pump-probe peaks. Additional Higgs collective mode peaks result from light-induced inversion-symmetry breaking in a thin-film geometry. For strong interband coupling, we find a transition from a nonequilibrium finite Cooper-pair momentum state characterized by hybrid-Higgs amplitude mode peaks in THz-MDCS spectra to a driven state identified experimentally by the emergence of Floquet-type sidebands at bi-Higgs frequencies. Those dominant bi-Higgs-frequency satellites are manifestations of a new order parameter relative phase collective mode that characterizes the nonequilibrium SC state. The predicted interaction- and field-dependent transitions in the spectral profile allow us to propose THz-MDCS experiments for quantum tomography of light-driven superconductivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Two-Dimensional Palladium Diselenide with Strong In-Plane Optical Anisotropy and High Mobility Grown by Chemical Vapor Deposition

Two-dimensional (2D) palladium diselenide (PdSe 2 ) has strong interlayer coupling and a puckered pentagonal structure, leading to remarkable layer-dependent electronic structures and highly anisotropic in-plane optical and electronic properties. However, the lack of high-quality, 2D PdSe 2 crystals grown by bottom-up approaches limits the study of their exotic properties and practical applications. In this work, chemical vapor deposition growth of highly crystalline few-layer (≥2 layers) PdSe 2 crystals on various substrates is reported. The high quality of the PdSe 2 crystals is confirmed by low-frequency Raman spectroscopy, scanning transmission electron microscopy, and electrical characterization. In addition, strong in-plane optical anisotropy is demonstrated via polarized Raman spectroscopy and second-harmonic generation maps of the PdSe 2 flakes. A theoretical model based on kinetic Wulff construction theory and density functional theory calculations is developed and described the observed evolution of “square=like” shaped PdSe 2 crystals into rhombus due to the higher nucleation barriers for stable attachment on the (1,1) and (1,-1) edges, which results in their slower growth rates. Finally, few-layer PdSe 2 field-effect transistors reveal tunable ambipolar charge carrier conduction with an electron mobility up to ≈294 cm 2 V -1 s -1 , which is comparable to that of exfoliated PdSe 2 , indicating the promise of this anisotropic 2D material for electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Unraveling the Correlation between Raman and Photoluminescence in Monolayer MoS 2 through Machine‐Learning Models

Abstract 2D transition metal dichalcogenides (TMDCs) with intense and tunable photoluminescence (PL) have opened up new opportunities for optoelectronic and photonic applications such as light‐emitting diodes, photodetectors, and single‐photon emitters. Among the standard characterization tools for 2D materials, Raman spectroscopy stands out as a fast and non‐destructive technique capable of probing material's crystallinity and perturbations such as doping and strain. However, a comprehensive understanding of the correlation between photoluminescence and Raman spectra in monolayer MoS 2 remains elusive due to its highly nonlinear nature. Here, the connections between PL signatures and Raman modes are systematically explored, providing comprehensive insights into the physical mechanisms correlating PL and Raman features. This study's analysis further disentangles the strain and doping contributions from the Raman spectra through machine‐learning models. First, a dense convolutional network (DenseNet) to predict PL maps by spatial Raman maps is deployed. Moreover, a gradient boosted trees model (XGBoost) with Shapley additive explanation (SHAP) to bridge the impact of individual Raman features in PL features is applied. Last, a support vector machine (SVM) to project PL features on Raman frequencies is adopted. This work may serve as a methodology for applying machine learning to characterizations of 2D materials.

Lu, Ang‐Yu↗
DOE OSTI2020

High yield production of ultrathin fibroid semiconducting nanowire of Ta 2 Pd 3 Se 8

Immediately after the demonstration of the high-quality electronic properties in various two dimensional (2D) van der Waals (vdW) crystals fabricated with mechanical exfoliation, many methods have been reported to explore and control large scale fabrications. Comparing with recent advancements in fabricating 2D atomic layered crystals, large scale production of one dimensional (1D) nanowires with thickness approaching molecular or atomic level still remains stagnant. Here, we demonstrate the high yield production of a 1D vdW material, semiconducting Ta 2 Pd 3 Se 8 nanowires, by means of liquid-phase exfoliation. The thinnest nanowire we have readily achieved is around 1 nm, corresponding to a bundle of one or two molecular ribbons. Transmission electron microscopy (TEM) and transport measurements reveal the as-fabricated Ta 2 Pd 3 Se 8 nanowires exhibit unexpected high crystallinity and chemical stability. Our low-frequency Raman spectroscopy reveals clear evidence of the existing of weak inter-ribbon bindings. The fabricated nanowire transistors exhibit high switching performance and promising applications for photodetectors.

1D semiconductor↗
DOE OSTI2020

Enhancement of van der Waals Interlayer Coupling through Polar Janus MoSSe

Interlayer coupling plays essential roles in the quantum transport, polaritonic, and electrochemical properties of stacked van der Waals (vdW) materials. In this work, we report the unconventional interlayer coupling in vdW heterostructures (HSs) by utilizing an emerging 2D material, Janus transition metal dichalcogenides (TMDs). In contrast to conventional TMDs, monolayer Janus TMDs have two different chalcogen layers sandwiching the transition metal and thus exhibit broken mirror symmetry and an intrinsic vertical dipole moment. Such a broken symmetry is found to strongly enhance the vdW interlayer coupling by as much as 13.2% when forming MoSSe/MoS 2 HS as compared to the pristine MoS 2 counterparts. Our noncontact ultralow-frequency Raman probe, linear chain model, and density functional theory calculations confirm the enhancement and reveal the origins as charge redistribution in Janus MoSSe and reduced interlayer distance. Furthermore, our results uncover the potential of tuning interlayer coupling strength through Janus heterostacking.

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

Ab Initio Molecular Dynamics Spectra for Characterization of Hydrated Al 2 O 3 Supported MoO x

The structure of supported MoO x /Al 2 O 3 catalysts is investigated using ab initio molecular dynamics (AIMD) and density-functional theory (DFT). Phase diagrams were computed to understand the hydroxylation coverage as a function of the temperature, H 2 O partial pressure, and MoO x loading. We relate the shifts in experimental Raman vibrational frequencies under hydrated conditions to hydrogen bonding interactions and the MoO x anchoring location. We showcase that the use of AIMD as a benchmark for DFT can provide insight into how, under certain hydrated conditions, DFT excels as an inexpensive method for computing vibrational frequencies, while, under dehydrated conditions, it is susceptible to the largest errors. Additionally, to facilitate the analysis of the hydroxyl region of experimental infrared spectra, we compute the power spectra of individual hydroxyls and see a strong relationship between OH stretching frequencies and the surrounding coordination environment, which are also impacted by anchored MoO x . Here, we compare computational and experimental IR and Raman spectra of catalysts synthesized herein under the same conditions.

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

Evaluation of a frequency-dependent phase shift in chirped Raman lasers for atom gravimeters

Light-pulse atom gravimetry has emerged as a powerful technique for precisely measuring absolute gravitational acceleration. Raman lasers are commonly used in this technique to coherently manipulate the atomic wave packet, of which the effective frequency is chirped continuously to compensate for the Doppler shift. In this study we investigate an additional phase shift in the Raman lasers that arises due to the frequency chirp. Here, we directly measure this phase shift by recording the beat signal of the Raman lasers with a high-speed oscilloscope, providing an independent evaluation of the resultant error in atom gravimeters caused by this phase shift. Concurrently, we detect the influence of the additional phase shift on gravity measurements using our atom gravimeter, and the results are in good agreement with the independent evaluation. Notably, there may still be a residual error at the microgal level when performing differential measurements by reversing the direction of the effective wave vector of the Raman lasers. We propose that this residual error can in principle be eliminated by selecting the same chirp frequency range for both directions in the differential measurement.

Xu, Yaoyao [Huazhong Univ. of Science and Technolo↗
DOE OSTI2021

Thickness and Spin Dependence of Raman Modes in Magnetic Layered Fe 3 GeTe 2

2D layered Fe 3 GeTe 2 has attracted increasing attention due to its high magnetic ordering temperature and novel physical properties. Lattice dynamics is a fundamental property of Fe 3 GeTe 2 , and its relationships with the number of layers and interlayer spin ordering have not yet been explored in depth. Here, by first-principles density functional theory calculations, the phonon vibrations and Raman intensities of Fe 3 GeTe 2 are systematically studied from the bulk to monolayer structures. Furthermore, the spin-phonon coupling effect is investigated by considering different interlayer magnetic orderings: ferromagnetic and antiferromagnetic. It is found that the frequencies of Raman modes in Fe 3 GeTe 2 exhibit considerable dependence on the layer number and spin ordering. In this work, the results not only reveal the notable spin-phonon interactions in Fe 3 GeTe 2 , but also demonstrate that Raman modes can be utilized for characterizing the sample thickness and interlayer spin ordering in this 2D magnet.

2D magnets↗
DOE OSTI2025

Van der Waals Sandwich Structures for Surface-Enhanced Raman Scattering

Surface-enhanced Raman scattering (SERS) intensity of two-dimensional (2D) materials critically depends on the resonant conditions and factors such as the substrate interferences and molecule adsorption fluctuations, making comprehensive investigation, understanding, and optimization of 2D materials-assisted SERS challenging. Here, in this work, the wavelength-dependent SERS of van der Waals structures of 2D materials is systematically investigated, focusing on the intrinsic frequency-dependent Raman tensors by first-principles method while ruling out other extrinsic factors in experiments. Distinct enhancement profiles are found for different 2D materials, among which MoS2 and graphene exhibit remarkably strong and broadband enhancement effects. For stacked multilayers and heterostructures of 2D materials, the calculated SERS addresses the significance of the first contact monolayer effect. Based on the above theory, the van der Waals sandwich structures are proposed and investigated as the SERS substrates, verifying a further significantly enhanced SERS performance. This resonant first-principles study demonstrates a comprehensive and analytical way to explore and promote the SERS of van der Waals structures.

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

Beyond the Charge Transfer Mechanism for 2D Materials-Assisted Surface Enhanced Raman Scattering

Two-dimensional (2D) materials have been extensively implemented as surface-enhanced Raman scattering (SERS) substrates, enabling trace-molecule detection for broad applications. However, the accurate understanding of the mechanism remains elusive because most theoretical explanations are still phenomenological or qualitative based on simplified models and rough assumptions. To advance the development of 2D material-assisted SERS, it is vital to attain a comprehensive understanding of the enhancement mechanism and a quantitative assessment of the enhancement performance. Here, the microscopic chemical mechanism of 2D material-assisted SERS is quantitatively investigated. The frequency-dependent Raman scattering cross sections suggest that the 2D materials’ SERS performance is strongly dependent on the excitation wavelengths and the molecule types. By analysis of the microscopic Raman scattering processes, the comprehensive contributions of SERS can be revealed. Beyond the widely postulated charge transfer mechanisms, the quantitative results conclusively demonstrate that the resonant transitions within 2D materials alone are also capable of enhancing the molecular Raman scattering through the diffusive scattering of phonons. Furthermore, all of these scattering routines will interfere with each other and determine the final SERS performance. Our results not only provide a complete picture of the SERS mechanisms but also demonstrate a systematic and quantitative approach to theoretically understand, predict, and promote the 2D materials SERS toward analytical applications.

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

Confocal Raman Microscopy Investigation of Phospholipid Monolayers Deposited on Nitrile-Modified Surfaces in Porous Silica Particles

Phospholipid bilayers deposited on a variety of surfaces offer models for investigation of the lipid membrane structure and supports for biocompatible sensors. Hybrid-supported phospholipid bilayers (HSLBs) are stable membrane models for these investigations, typically prepared by self-assembly of a lipid monolayer over an n-alkane-modified surface. HSLBs have been prepared on n-alkyl chain-modified silica and used for lipophilicity-based chromatographic separations. The structure of these hybrid bilayers differs from vesicle membranes where the lipid head group spacing is greater due to interdigitation of the lipid acyl chains with the underlying n-alkyl chains bound to the silica surface. This interdigitated structure exhibits a broader melting transition at a higher temperature due to strong interactions between the lipid acyl chains and the immobile n-alkyl chains bound to silica. In the present work, we seek to reduce the interactions between a lipid monolayer and its supporting substrate by self-assembly of 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC) on porous silica functionalized with nitrile-terminated surface ligands. The frequency of Raman scattering of the surface -C≡N stretching mode at the lipid–nitrile interface is consistent with an n-alkane-like environment and insensitive to lipid head group charge, indicating that the lipid acyl chains are in contact with the surface nitrile groups. The head group area of this lipid monolayer was determined from the within-particle phospholipid concentration and silica specific surface area and found to be 54 ± 2 Å 2 , equivalent to the head group area of a DMPC vesicle bilayer. The structure of these nitrile-supported phospholipid monolayers was characterized below and above their melting transition by confocal Raman microscopy and found to be nearly identical to DMPC vesicle bilayers. Their narrow gel-to-fluid-phase melting transition is equivalent to dispersed DMPC vesicles, indicating that the acyl chain structure on the nitrile support mimics the outer leaflet structure of a vesicle membrane.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Adapting confocal Raman microscopy for in situ studies of redox transformations at electrode-electrolyte interfaces

Confocal Raman microscopy was applied to quantify redox species present within the diffusion layer adjacent to an electrode surface under potentiostatic control. A glass microscope coverslip with a thin indium tin oxide (ITO) coating served as both the working electrode and optical window for a microscope-stage mountable spectroelectrochemical cell. A high numerical aperture objective mounted in an inverted microscope frame just below the stage brought excitation radiation through the coverslip window and to a tight focus a few micrometers above the ITO film surface. Species diffusing into the confocal probe volume defined by the excitation beam focus and the collected light region were detected, identified and quantified based on their Raman scattering frequencies and intensities. Here, in measurements that interrogated the interconversion of ferrocyanide and ferricyanide ions as a function of applied voltage, least-squares regression analysis of spectral datasets predicted the formal potential and relative surface concentrations of the ions in good agreement with the expected Nernstian response. Preliminary studies of methyl viologen reduction at an ITO film/Nafion membrane interface were conducted and show the possibility for estimation of mass transport coefficients of redox species within ionic polymer materials.

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

Preference for a pressure-induced 3D structure after 1T-HfSe 2

Extensive crystal structure prediction searches provide evidence of two 3D structures with orthorhombic (Immm) and monoclinic (C2/m) space groups as reasonable candidates for the first pressure-induced phase of 1T-HfSe 2 . Our candidates are compared with two recent proposals that keep the 2D nature of the ambient conditions phase and display hexagonal (P6 3 /mmc) and monoclinic (C2/m) symmetry, although the latter has a different structure than our proposed C2/m phase. Both of these 2D-like structures are discarded based on simple thermodynamic and kinetic arguments that can be extended to explain the pressure-induced polymorphic sequence of other transition metal dichalcogenides. The computed observables of our orthorhombic phase are fully consistent with the experimental structural and Raman data observed at low and high-pressure.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Strong Surface-Enhanced Coherent Phonon Generation in van der Waals Materials

Terahertz (THz) coherent phonons have emerged as promising candidates for the next generation of high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. However, effectively manipulating THz coherent phonons remains a significant challenge. Here, in this study, we investigated THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of Fe 3 GeTe 2 , Fe 5 GeTe 2 , and FePS 3 . We successfully generated the THz A 1g coherent phonon mode in these vdW flakes. An innovative approach involved partially exfoliating vdW flakes on a gold substrate and partially on a silicon (Si) substrate to compare the THz coherent phonon generation between both sides. Interestingly, we observed a significantly enhanced THz coherent phonon in the vdW/gold area compared with that in the vdW/Si area. Frequency-domain Raman mapping across the vdW flakes corroborated these findings. Numerical simulations further indicated a stronger enhanced surface field in vdW/gold structures than in vdW/Si structures. Consequently, we attribute the observed enhancement in THz coherent phonon generation to the increased surface field on the gold substrate. This enhancement was consistent across the three different vdW materials studied, suggesting the universality of this strategy. Our results hold promise for advancing the design of THz phononic and phonon-integrated devices.

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

Improved isotope-shift-based bounds on bosons beyond the Standard Model through measurements of the $^2$D$_{3/2} - ^2$D$_{5/2}$ interval in Ca$^+$

We perform high-resolution spectroscopy of the $3$d$~^2$D$_{3/2} - 3$d$~^2$D$_{5/2}$ interval in all stable even isotopes of $^A$Ca$^+$ (A = 40, 42, 44, 46 and 48) with an accuracy of $\sim$ 20 Hz using direct frequency-comb Raman spectroscopy. Combining these data with isotope shift measurements of the 4s$~^2$S$_{1/2} \leftrightarrow 3$d$~^2$D$_{5/2}$ transition, we carry out a King plot analysis with unprecedented sensitivity to coupling between electrons and neutrons by bosons beyond the Standard Model. Furthermore, we estimate the sensitivity to such bosons from equivalent spectroscopy in Ba$^+$ and Yb$^+$. Finally, the data yield isotope shifts of the 4s$~^2$S$_{1/2} \leftrightarrow 3$d$~^2$D$_{3/2}$ transition at 10 part-per-billion through combination with recent data of Knollmann et al (2019).

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Suppressing the enhancement of stimulated Raman scattering in inhomogeneous plasmas by tuning the modulation frequency of a broadband laser

The stimulated Raman scattering (SRS) instability can inhibit the performance of laser driven inertial confinement fusion (ICF) implosions by scattering light into unwanted directions or by generating hot electrons that preheat the target fuel. In principle, ICF target designs can avoid parameter regimes conducive to large, linear SRS gains. In practice, kinetic inflation—the nonlinear enhancement of SRS due to electron trapping in the excited plasma wave—makes this difficult. Here we show that laser bandwidth in the form of frequency modulation can either decrease or increase the inflationary SRS (iSRS) threshold in inhomogeneous plasmas depending on the maximum chirp of the laser pulse. The threshold, mapped out by a series of particle-in-cell simulations, exhibits a minimum when the frequency change within the pulse cancels the spatial detuning due to density inhomogeneities along the trajectory of the scattered light. In conclusion, by tuning the pump laser parameters away from this minimum, the iSRS threshold can be larger than at zero bandwidth, providing a path to mitigating kinetic inflation in ignition relevant plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗