Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Coherent spectroscopy”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Cavity-Assisted Coherent Phonon Generation and Control in a WSe 2 /Au Structure

Coherent phonons in the Terahertz (THz) regime have gained attention as potential candidates for next-generation high-speed, low-energy information carriers in atomically thin phononic or phonon-integrated on-chip devices. Nevertheless, achieving efficient control over THz coherent phonons continues to pose a considerable challenge. In this work, we explore THz coherent phonon generation in exfoliated van der Waals (vdW) flakes of WSe 2 on Au (WSe 2 /Au) and Si (WSe 2 /Si) using time-resolved pump-probe spectroscopy. The generation of THz coherent phonons was studied as a function of WSe 2 layer thickness and laser wavelength. Notably, a significant enhancement in THz coherent phonon generation was observed in the WSe 2 /Au structure, but only within specific ranges of WSe 2 thickness and laser wavelength. Further, the results from numerical simulations, which consider a self-hybridized optical cavity depending on WSe 2 thickness, along with optical reflectance and Raman spectroscopy measurements, aligned well with the time-domain observations of THz coherent phonon generation. We propose that the observed enhancement in THz coherent phonon generation is strongly influenced by light-matter interaction in the WSe 2 cavity, a mechanism that may be applicable to a broader range of vdW materials. These findings offer promising insights for the development of THz phononic or phonon-integrated devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2004

Reflectance and Thermal Infrared Spectroscopy of Mars: Relationship Between ISM and TES for Compositional Determinations

Reflectance spectroscopy has demonstrated that high albedo surfaces on Mars contain heavily altered materials with some component of hematite, poorly crystalline ferric oxides, and an undefined silicate matrix. The spectral properties of many low albedo regions indicate crystalline basalts containing both low and high calcium pyroxene, a mineralogy consistent with the basaltic SNC meteorites. The Thermal Emission Spectrometer (TES) experiment on the Mars Geochemical Surveyor has acquired critical new data relevant to surface composition and mineralogy, but in a wavelength region that is complementary to reflectance spectroscopy. The essence of the completed research was to analyze TES data in the context of reflectance data obtained by the French ISM imaging spectrometer experiment in 1989. This approach increased our understanding of the complementary nature of these wavelength regions for mineralogic determinations using actual observations of the martian surface. The research effort focused on three regions of scientific importance: Syrtis Major-Isidis Basin, Oxia Palus-Arabia, and Valles Marineris. In each region distinct spatial variations related to reflectance, and in derived mineralogic information and interpreted compositional units were analyzed. In addition, specific science questions related to the composition of volcanics and crustal evolution, soil compositions and pedogenic processes, and the relationship between pristine lithologies and weathering provided an overall science-driven framework for the work. The detailed work plan involved colocation of TES and ISM data, extraction of reflectance and emissivity spectra from areas of known reflectance variability, and quantitative analysis using factor analysis and statistical techniques to determine the degree of correspondence between these different wavelength regions. Identified coherent variations in TES spectroscopy were assessed against known atmospheric effects to validate that the variations are due to surface properties. With this new understanding of reflectance and emission spectroscopy, mineralogic interpretations were derived and applied to the science objectives of the three regions.

Boyce, Joseph↗
DOE OSTI2021

Role of peracetic acid on the disruption of lignin packing structure and its consequence on lignin depolymerisation

Peracetic acid (PAA) is an effective oxidant capable of solubilising lignin and efficiently depolymerising it to selective phenolic compounds; however, the specific role by which PAA initiates the depolymerisation is still elusive. Herein, interaction between PAA and the lignin macromolecule and the consequent structural changes of the latter were studied by characterising the lignin packing structure and its associated changes during the oxidation process. While the lignin packing structure and its changes associated with the PAA-mediated oxidation were probed by X-ray diffraction, the impact of the PAA on different chemical functionalities present in the lignin structure was established by 13 C and 1 H– 13 C heteronuclear single-quantum coherence nuclear magnetic resonance (NMR) spectroscopy. Further, combining the NMR spectroscopy results, and the product distribution, we conclude that the predominant reaction pathway for the oxidative depolymerisation of lignin with PAA is the Baeyer–Villiger oxidation of the ketone formed by the oxidation of the benzylic hydroxyl group adjacent to the β-O-4 linkage. The experimental evidence provided herein corroborated that PAA instigates oxygen insertion to the lignin macromolecule resulting in disruption of its packing structures and facilitates depolymerisation. We also investigated various metal oxide and mixed metal oxide catalysts to identify effective catalysts that further enhance the efficiency of PAA-mediated depolymerisation of lignin and produce selective monomeric phenolic compounds. Techno-economic analysis was also conducted to identify the key parameters associated with this oxidative process that need to be considered for possible commercial application.

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

Plasma Assisted Combustion and Chemical Processing: Chapter 9 - Plasma Diagnostics

Plasma dynamics and chemistry have a broad range of timescales from picoseconds to milliseconds. In addition, it involves nonequilibrium energy transfer between electrons, ions, electronically and vibrationally excited states, radicals, intermediate species, and reactants and products as well as surface charges and chemistry. To understand plasma physics and chemistry, it is essential to conduct time and space resolved, quantitative detection of nonequilibrium temperature distributions, electron energy and number density, electric field, and species concentrations. There are enormous publications and review articles on this subject. The focus of this chapter is to be placed on the most recent progress in gas phase plasma properties and chemistry, especially on optical emission spectroscopy, laser absorption spectroscopy, Faraday rotational spectroscopy, Raman and Thompson scattering, femtosecond and picosecond (fs/ps) coherent anti-Stokes Raman scattering (CARS) spectroscopy, and electric field-induced second harmonic generation methods.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Diffraction enhanced imaging utilizing a laser produced x-ray source

Image formation by Fresnel diffraction utilizes both absorption and phase-contrast to measure electron density profiles. The low spatial and spectral coherence requirements allow the technique to be performed with a laser-produced x-ray source coupled with a narrow slit. This makes it an excellent candidate for probing interfaces between materials at extreme conditions, which can only be generated at large-scale laser or pulsed power facilities. Here, we present the results from a proof-of-principle experiment demonstrating an effective ~2 μm laser-generated source at the OMEGA Laser Facility. This was achieved using slits of 1 × 30 μm 2 and 2 × 40 μm 2 geometry, which were milled into 30 μm thick Ta plates. Combining these slits with a vanadium He-like 5.2 keV source created a 1D imaging system capable of micrometer-scale resolution. The principal obstacles to achieving an effective 1 μm source are the slit tilt and taper—where the use of a tapered slit is necessary to increase the alignment tolerance. We demonstrate an effective source size by imaging a 2 ± 0.2 μm radius tungsten wire.

3D printing↗
DOE OSTI2025

Probing the impact of oxygen negative ions on the self-organized pattern in 1 atm DC glow with liquid anode

In an atmospheric DC glow discharge with a liquid anode, the plasma anode glow attached to the grounded liquid surface under certain conditions self-organizes into coherent patterns. Optical emission spectroscopy revealed that the emission consists primarily of the second positive system of nitrogen, N 2 (C-B), whose excitation energy is low and sensitive to changes in the electron energy distribution. In addition to electrons, negative ions can accumulate in the anode sheath and affect the local space charge. It has been speculated that these negative ions play a role in pattern formation at the anode surface. In this work, the role of oxygen negative ions was explored. It was found that the formation of anode patterns requires at least a 7% volume fraction of oxygen in the ambient gas. Results showed that O 2 - is the dominant negative ion species in atmospheric DC glow discharge, with a density of ~10 12 cm -3 . While the presence of oxygen appears to be crucial for pattern formation, this study indicated that patterns still formed without geometric changes even when 62% of negative ions in the plasma were detached by a laser. This suggests that negative ions do not support the patterns, while oxygen's heating effect may induce instability at the anode.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe 2 van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Screening of Polar Electron-Phonon Interactions near the Surface of the Rashba Semiconductor BiTeCl

Understanding electron-phonon coupling in noncentrosymmetric materials is critical for controlling the internal fields which give rise to Rashba interactions. We apply time- and angle-resolved photoemission spectroscopy (trARPES) to study coherent phonons in the surface and bulk regions of the polar semiconductor BiTeCl. Aided by \textit{ab initio} calculations, our measurements reveal the coupling of out-of-plane $A_1$ modes and an in-plane $E_2$ mode. By considering how these modes modulate the electric dipole moment in each unit cell, we show that the polar $A_1$ modes are more effectively screened in the metallic surface region, while the non-polar $E_2$ mode couples in both regions. Finally, in addition to informing strategies to optically manipulate Rashba interactions, this work has broader implications for the behavior of electron-phonon coupling in systems characterized by inhomogeneous dielectric environments.

36 MATERIALS SCIENCE↗
NASA NTRS1999

Acoustic Pyrometry Applied to Gas Turbines and Jet Engines

Internal gas temperature is one of the most fundamental parameters related to engine efficiency and emissions production. The most common methods for measuring gas temperature are physical probes, such as thermocouples and thermistors, and optical methods, such as Coherent Anti Stokes Raman Spectroscopy (CARS) or Rayleigh scattering. Probes are relatively easy to use, but they are intrusive, their output must be corrected for errors due to radiation and conduction, and their upper use temperature is limited. Optical methods are nonintrusive, and they measure some intrinsic property of the gas that is directly related to its temperature (e.g., lifetime or the ratio of line strengths). However, optical methods are usually difficult to use, and optical access is not always available. Lately, acoustic techniques have been receiving some interest as a way to overcome these limitations.

Fralick, Gustave C.↗
NASA NTRS2007

Development of Supersonic Combustion Experiments for CFD Modeling

This paper describes the development of an experiment to acquire data for developing and validating computational fluid dynamics (CFD) models for turbulence in supersonic combusting flows. The intent is that the flow field would be simple yet relevant to flows within hypersonic air-breathing engine combustors undergoing testing in vitiated-air ground-testing facilities. Specifically, it describes development of laboratory-scale hardware to produce a supersonic combusting coaxial jet, discusses design calculations, operability and types of flames observed. These flames are studied using the dual-pump coherent anti- Stokes Raman spectroscopy (CARS) - interferometric Rayleigh scattering (IRS) technique. This technique simultaneously and instantaneously measures temperature, composition, and velocity in the flow, from which many of the important turbulence statistics can be found. Some preliminary CARS data are presented.

Baurle, Robert↗
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 OSTI2025

Experimental study of high-energy single-pulse nanosecond discharges in pin-to-pin configuration

Single-pulse pin-to-pin nanosecond pulsed discharges in ambient air (gap distances of 3–7 mm) were investigated at high pulse energies (∼20–30 mJ deposited energy per 11 ns full width at half maximum pulse). A Michelson interferometry setup (532 nm continuous-wave laser) was employed to record time-resolved interferograms of the discharge, enabling spatially resolved calculation of the electron number density. An intensified charge-coupled device camera was used to capture the spatiotemporal evolution of the discharge (streamer formation and spark channel development), and Coherent Anti-Stokes Raman Spectroscopy (CARS) was used to measure post-discharge N 2 vibrational temperatures. Discharge current and voltage were monitored with a back-current shunt. The discharge was initiated with simultaneous cathode-directed and anode-directed streamers that bridge the gap within ∼1 ns and form a luminous, filamentary plasma channel immediately after breakdown. Laser interferometry measurements showed peak electron number densities of the order of 10 1 7–10 18 cm −3 , occurring about 15–20 ns after pulse arrival at the discharge gap. Shorter gap discharges yielded higher peak electron densities, consistent with the higher energy density in the smaller gaps. Spatially, the electron density was highest near the electrodes and decreased toward the midgap region, with 5 and 7 mm gaps exhibiting a pronounced drop in the central channel. CARS indicated initial vibrational temperatures of approximately 4000–6000 K in the spark core of ∼50 ns after the discharge onset, decaying on a ∼500 ns timescale as the plasma cooled and recombined.

Coherent anti-Stokes Raman spectroscopy↗
DOE OSTI2020

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe 2 with Femtosecond Core-Level Spectroscopy

In this study, we employ few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to reveal simultaneously the intra- and interband carrier relaxation and the light-induced structural dynamics in nanoscale thin films of layered 2H-MoTe 2 semiconductor. By interrogating the valence electronic structure via localized Te 4 d (39-46 eV) and Mo 4 p (35-38 eV) core levels, the relaxation of the photoexcited hole distribution is directly observed in real time. We obtain hole thermalization and cooling times of 15 ± 5 fs and 380 ± 90 fs, respectively, and an electron-hole recombination time of 1.5 ± 0.1 ps. Furthermore, excitations of coherent out-of-plane A 1g (5.1 THz) and in-plane E 1g (3.7 THz) lattice vibrations are visualized through oscillations in the XUV absorption spectra. By comparison to Bethe-Salpeter equation simulations, the spectral changes are mapped to real-space excited-state displacements of the lattice along the dominant A 1g coordinate. By directly and simultaneously probing the excited carrier distribution dynamics and accompanying femtosecond lattice displacement in 2H-MoTe 2 within a single experiment, our work provides a benchmark for understanding the interplay between electronic and structural dynamics in photoexcited nanomaterials.

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

Conical intersections shed light on hot carrier cooling in quantum dots

Experimental observations of vibronic coherences in electronically excited colloidal semiconductor nanocrystals offer a window into the ultrafast dynamics of hot carrier cooling. In previous work, we showed that, in amine-passivated quantum dots (QDs), these coherences arise during relaxation through a cascade of conical intersections between electronically excited states. Here, in this work, we demonstrate the generality of this framework by application to QDs with surface-bound carboxylate ligands. A model involving a similar cascade of conical intersections accurately reproduces the frequencies of vibronic coherences observed with broadband multidimensional spectroscopy. The impact of ligands on the relaxation dynamics is attributed to two distinct mechanisms involving either electronic or vibrational coupling between the core and ligands. Compared to the amine-passivated QDs studied previously, the electronic coupling mechanism is less prominent in carboxylate-passivated QDs. Furthermore, comparison of acetate and formate ligands reveals that truncating the ligand alkyl chains alters the relaxation behavior predicted by the model.

14 SOLAR ENERGY↗
DOE OSTI2023

Coherent Phonon-Induced Modulation of Charge Transfer in 2D Hybrid Perovskites

Electron–phonon interactions play an essential role in charge transport and transfer processes in semiconductors. For most structures, tailoring electron–phonon interactions for specific functionality remains elusive. Here, it is shown that, in hybrid perovskites, coherent phonon modes can be used to manipulate charge transfer. In the 2D double perovskite, (AE2T) 2 AgBiI 8 (AE2T: 5,5“-diylbis(amino-ethyl)-(2,2”-(2)thiophene)), the valence band maximum derived from the [Ag 0.5 Bi 0.5 I4] 2– framework lies in close proximity to the AE2T-derived HOMO level, thereby forming a type-II heterostructure. During transient absorption spectroscopy, pulsed excitation creates sustained coherent phonon modes, which periodically modulate the associated electronic levels. Thus, the energy offset at the organic–inorganic interface also oscillates periodically, providing a unique opportunity for modulation of interfacial charge transfer. Density-functional theory corroborates the mechanism and identifies specific phonon modes as likely drivers of the coherent charge transfer. These observations are a striking example of how electron–phonon interactions can be used to manipulate fundamentally important charge and energy transfer processes in hybrid perovskites.

36 MATERIALS SCIENCE↗
NASA NTRS2002

Fundamental Mixing and Combustion Experiments for Propelled Hypersonic Flight

The first experiment is a study of a coaxial jet discharging into stagnant laboratory air, with center jet of a mixture of 5% oxygen and 95% helium by volume and coflow jet of air. The exit flow pressure of both center-jet and coflow nozzles is 1 atmosphere. The presence of oxygen in the center jet is to allow the use of an oxygen flow-tagging technique (RELIEF4) to obtain non-intrusive velocity measurements. Both jets are nominally Mach 1.8, but, because of the greater speed of sound, the center jet velocity is more than twice that of the coflow. The mixing layer which forms between the center jet and the coflow near the nozzle exit is compressible, with a calculated convective Mach number of approximately 0.7. This geometry has several advantages: The streamwise development of the flow is generally dominated by turbulent stresses (rather than pressure forces), and thus calculations are sensitive to turbulence modeling. It includes features present in supersonic combustors, including a compressible mixing layer near the nozzle exit and a light-gas/air plume downstream. Since it is a free jet, it provides easy access for both optical instrumentation and probes. Since it is axisymmetric, it requires fewer experimental measurements to fully characterize, and calculations can be performed with more modest computer resources. However, weak shock waves formed at the nozzle exit strengthen and turn normal as they approach the axis, complicating the flow. Care is thus taken in the design of the facility to provide as near as possible to 1-D flow at the exit of both center and coflow nozzles, and to minimize the strength of waves generated at the nozzle exit. Results from this experiment are compared to CFD solutions obtained by VULCAN, a previously developed code used in engine analysis. The second experiment is a study of a supersonic combustor consisting of a diverging duct with single downstream-angled wall injector. Thus, the geometry is relatively simple and large regions of subsonic recirculating flow are avoided. The nominal entrance Mach number is 2 and the enthalpy of the test gas (hot air "simulant") is nominally that of Mach 7 flight. It was believed, on the basis of calculations performed that this would produce mixing-limited flow, that is to say, one for which chemical reaction to equilibrium proceeds at a much greater rate than mixing. It later proved that this was not the case. The primary experimental technique employed is coherent anti-Stokes Raman spectroscopy, known by its acronym CARS. The species probed is molecular nitrogen and the quantity measured is temperature. Intrusive probes, such as Pitot, total temperature, hot-wire, etc., are not used due to access difficulty and high heat flux in the combustor, and because they may alter the flow. CARS has several advantages over other optical methods. It is a relatively mature and well-understood technique. Signal levels are relatively high and the signal is in the form of a coherent (laser) beam that can be collected through small windows. Incoherent (non-CARS) interferences are rejected by spatial filtering.

Diskin, G. S.↗
DOE OSTI2025

Non-Equilibrium in a Dust-Forming Low-Temperature Plasma: A CARS Study

Dust-forming low-temperature plasmas are versatile systems for the production of nanoparticles with tunable functionalities. While attractive from a materials processing point of view, these systems are inherently complex, with several plasma-induced phenomena determining the properties of the produced materials. Here, we characterize a carbon nanoparticle-forming plasma using coherent anti-Stokes Raman spectroscopy (CARS), with the primary goal of measuring gas temperature. While gas temperature is typically assumed to be at or slightly above room temperature in these reactors, we measure gas temperatures exceeding 1000 K under typical process conditions. We find a correlation between the gas temperature and the nanoparticle yield, suggesting that the particle nucleation and growth process releases energy within the reaction volume, leading to significant gas heating. In addition, we find that the relaxation of vibrationally excited species at the particle surfaces is a major contributor to their heating. In conclusion, these results underscore the complexity of these systems and the need for their more in-depth characterization using advanced techniques such as CARS.

Basic Plasma Phenomena and Gas Discharges↗