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DOE OSTI2025

Origin of Large Effective Phonon Magnetic Moments in Monolayer MoS 2

Recent helicity-resolved magneto-Raman spectroscopy measurement demonstrates large effective phonon magnetic moments of ~2.5 μ B in monolayer MoS 2 , highlighting resonant excitation of bright excitons as a feasible route to activate Γ-point circularly polarized phonons in transition metal dichalcogenides. However, a microscopic picture of this intriguing phenomenon remains lacking. In this work, we show that an orbital transition between the split conduction bands (Δ 0 = 4 meV) of MoS 2 couples to the doubly degenerate E" phonon mode (Ω 0 = 33 meV), forming two hybridized states. Our phononic and electronic Raman scattering measurements capture these two states: (i) one with predominantly phonon contribution in the helicity-switched channels and (ii) one with primarily orbital contribution in the helicity-conserved channels. An orbital-phonon coupling model successfully reproduces the large effective magnetic moments of the circularly polarized phonons and explains their thermodynamic properties. Strikingly, the Raman mode from the orbital transition is superimposed on a strong quasi-elastic scattering background, indicating the presence of spin fluctuations. As a result, the electrons excited to the conduction bands through the exciton exhibit paramagnetic behavior although MoS 2 is generally considered as a nonmagnetic material. By depositing nanometer-thickness nickel thin films on monolayer MoS 2 , we tune the electronic structure so that the A exciton perfectly overlaps with the 633 nm laser. The optimization of resonance excitation leads to pronounced tunability of the orbital-phonon hybridized states. Our results generalize the orbital-phonon coupling model of effective phonon magnetic moments to material systems beyond the paramagnets and magnets.

2D transition metal dichalcogenide↗

NASA NTRS1989

Progress of research on water vapor lidar

Research is summarized on applications of stimulated Raman scattering (SRS) of laser light into near infrared wavelengths suitable for atmospheric monitoring. Issues addressed are conversion efficiency, spectral purity, optimization of operating conditions, and amplification techniques. A Raman cell was developed and built for the laboratory program, and is now available to NASA-Langley, either as a design or as a completed cell for laboratory or flight applications. The Raman cell has been approved for flight in NASA's DC-8 aircraft. The self-seeding SRS technique developed here is suggested as an essential improvement for tunable near-IR DIAL applications at wavelengths of order 1 micrometer or greater.

Wilkerson, Thomas D.↗

NASA NTRS2021

Perseverance’s Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) Investigation

The Scanning Habitable Environments with Raman and Luminescence for Organics and Chemicals (SHERLOC) is a robotic arm-mounted instrument on NASA’s Perseverance rover. SHERLOC has two primary boresights. The Spectroscopy boresight generates spatially resolved chemical maps using fluorescence and Raman spectroscopy coupled to microscopic images (10.1 μm/pixel). The second boresight is a Wide Angle Topographic Sensor for Operations and eNgineering (WATSON); a copy of the Mars Science Laboratory (MSL) Mars Hand Lens Imager (MAHLI) that obtains color images from microscopic scales (∼13 μm/pixel) to infinity. SHERLOC Spectroscopy focuses a 40 μs pulsed deep UV neon-copper laser (248.6 nm), to a ∼100 μm spot on a target at a working distance of ∼48 mm. Fluorescence emissions from organics, and Raman scattered photons from organics and minerals, are spectrally resolved with a single diffractive grating spectrograph with a spectral range of 250 to ∼370 nm. Because the fluorescence and Raman regions are naturally separated with deep UV excitation (<250 nm), the Raman region ∼ 800 – 4000 cm−1 (250 to 273 nm) and the fluorescence region (274 to ∼370 nm) are acquired simultaneously without time gating or additional mechanisms. SHERLOC science begins by using an Autofocus Context Imager (ACI) to obtain target focus and acquire 10.1 μm/pixel greyscale images. Chemical maps of organic and mineral signatures are acquired by the orchestration of an internal scanning mirror that moves the focused laser spot across discrete points on the target surface where spectra are captured on the spectrometer detector. ACI images and chemical maps (< 100 μm/mapping pixel) will enable the first Mars in situ view of the spatial distribution and interaction between organics, minerals, and chemicals important to the assessment of potential biogenicity (containing CHNOPS). Single robotic arm placement chemical maps can cover areas up to 7x7 mm in area and, with the < 10 min acquisition time per map, larger mosaics are possible with arm movements. This microscopic view of the organic geochemistry of a target at the Perseverance field site, when combined with the other instruments, such as Mastcam-Z, PIXL, and SuperCam, will enable unprecedented analysis of geological materials for both scientific research and determination of which samples to collect and cache for Mars sample return.

Rohit Bhartia↗

NASA NTRS1990

Progress of research on water vapor lidar

Research is described on several aspects of stimulated Raman scattering (SRS) of 532 nm laser light in H2, D2, and CH4. The goals of this work are to develop a more thorough understanding of nonlinear processes involving the Raman effect and four-wave mixing, and to find the best way to generate radiation at several wavelengths simultaneously, for lidar applications. Issues addressed are conversion efficiency, optimization of operating conditions (gas pressure, confocal parameter, etc.) and the distribution of output pulse energy over three Stokes components, the first anti-Stokes component, and the zeroth order (pump) wavelength. The described research and results constitute another step in the development of SRS applications for NASA's atmospheric lidar program.

Wilkerson, T. D.↗

DOE OSTI2024

Resonant Raman in armchair graphene nanoribbons from first-principles

Resonant Raman spectra of armchair graphene nanoribbons (AGNRs) are computed using Density Functional Theory (DFT) and third-order perturbation theory. Results are benchmarked against available experimental data and compared to previously used theoretical approaches based on the Placzek approximation. Comparable agreement with experiments is found for both previously and presently used methods. In addition, a numerical analysis is carried out to provide a justification for the resonant modeling method based on the use of the frequency-dependent dielectric tensor in the Placzek approximation. Finally, this work also provides additional predictions and references for wide AGNRs that might be investigated with Raman scattering experiments in the future.

42 ENGINEERING↗

NASA NTRS1980

Remote sensing of subsurface water temperature by laser Raman spectroscopy

This paper describes experimental remote sensing of subsurface water temperature using the Raman spectroscopic technique. By the use of a pulsed laser and range gating detection techniques, Raman scattering is analyzed as a function of depth in a radar-like echo mode, and thus subsurface profiles of temperature and transmission are obtained. Experiments are described in which Raman data using polarization spectroscopy has been obtained from a ship as a function of depth in ocean water near Grand Bahama Island. A spectral temperature accuracy of + or - 1 C has been obtained from this data in the first two optical attenuation lengths. Raman data obtained from ocean water using the NASA airborne oceanographic lidar is also presented.

Leonard, D. A.↗

NASA NTRS1981

Remote Raman measurement techniques

The use of laser Raman measurement techniques in remote sensing applications is surveyed. A feasibility index is defined as a means to characterize the practicality of a given remote Raman measurement application. Specific applications of Raman scattering to the measurement of atmospheric water vapor profiles, methane plumes from liquid natural gas spills, and subsurface ocean temperature profiles are described. This paper will survey the use of laser Raman measurement techniques in remote sensing applications using as examples specific systems that the Computer Genetics Corporation (CGC) group has developed and engineered.

Leonard, D. A.↗

NASA NTRS1986

Observation of atmospheric ozone by dial with Raman lasers pumped by a KrF laser

Since the XeCl excimer laser (308 nm) was first used in Differential Absorption Lidar (DIAL) for stratospheric ozone detection, the XeCl ozone lidar became a useful tool for the monitoring of the stratospheric ozone concentration. Shorter wavelength lasers are needed for the observation of ozone in the troposphere where the ozone concentration is about one order of magnitude smaller than in the stratosphere. In 1983, tropospheric ozone was observed with the combination of the second Stokes line (290.4 nm) of stimulated Raman scattering from methane pumped by a KrF laser and the XeCl laser line. The measurement of the ozone distribution from ground to 30 km was reported, using three Stokes lines of Raman lasers pumped by a KrF laser. At wavelengths shorter than 295 nm, the background solar radiation is effectively suppressed by atmospheric ozone. Such a solar-blind effect can be expected when two wavelengths 277 and 290.4 nm are used for DIAL ozone detection. A preliminary measurement of the day time ozone distribution in the troposphere is presented using these wavelengths generated by a KrF laser with a Raman shifter. Analysis using the lidar equation predicts the maximum detectable range is 7 km.

Maeda, M.↗

NASA NTRS2017

Rotational Raman-Based Temperature Measurements in a High-Velocity Turbulent Jet

Spontaneous rotational Raman scattering spectroscopy is used to acquire the first ever high quality, spatially-resolved measurements of the mean and root mean square (rms) temperature fluctuations in turbulent, high-velocity heated jets. Raman spectra in air were obtained across a matrix of radial and axial locations downstream from a 50 mm diameter nozzle operating from subsonic to supersonic conditions over a wide range of temperatures and Mach numbers, in accordance with the Tanna matrix frequently used in jet noise studies. These data were acquired in the hostile, high noise (115 dB) environment of a large scale open air test facility at NASA Glenn Research Center (GRC). Temperature estimates were determined by performing nonlinear least squares fitting of the single shot spectra to the theoretical rotational Stokes spectra of N2 and O2, using a custom in-house code developed specifically for this investigation. The laser employed in this study was a high energy, long-pulsed, frequency doubled Nd:YAG laser. One thousand single-shot spectra were acquired at each spatial coordinate. Mean temperature and rms temperature variations were calculated at each measurement location. Excellent agreement between the averaged and single-shot temperatures was observed with an accuracy better than 2.5 percent for temperature, and rms variations in temperature between +/-2.2 percent at 296 K and +/-4.5 percent at 850 K. The results of this and planned follow-on studies will support NASA GRC's development of physics-based jet noise prediction, turbulence modeling and aeroacoustic source modeling codes.

Randy J Locke↗

NASA NTRS2017

Rotational Raman-Based Temperature Measurements in a High-Velocity Turbulent Jet

Randy J Locke↗

NASA NTRS1981

Absolute tracer dye concentration using airborne laser-induced water Raman backscatter

The use of simultaneous airborne-laser-induced dye fluorescence and water Raman backscatter to measure the absolute concentration of an ocean-dispersed tracer dye is discussed. Theoretical considerations of the calculation of dye concentration by the numerical comparison of airborne laser-induced fluorescence spectra with laboratory spectra for known dye concentrations using the 3400/cm OH-stretch water Raman scatter as a calibration signal are presented which show that minimum errors are obtained and no data concerning water mass transmission properties are required when the laser wavelength is chosen to yield a Raman signal near the dye emission band. Results of field experiments conducted with an airborne conical scan lidar over a site in New York Bight into which rhodamine dye had been injected in a study of oil spill dispersion are then indicated which resulted in a contour map of dye concentrations, with a minimum detectable dye concentration of approximately 2 ppb by weight.

Hoge, F. E.↗

DOE OSTI2025

Large Propagation-Direction-Dependent Circularly Polarized Emission and Scattering Anisotropies of a Chiral Organic-Inorganic Semiconductor

Chiral materials are important tools for transducing circularly polarized light within many emerging opto-electronic and spin-based technologies. Here, we demonstrate that thin films of a bismuth iodide-based 0D chiral hybrid organic-inorganic semiconductor (HOIS) exhibit large anisotropy values in circularly polarized light emission (CPLE) that approach 50%, with mirror-image responses from front- and back-side measurements. A comprehensive analysis of light-wave propagation, absorption, emission, and scattering is constructed on the basis of a symmetry-derived exciton fine structure model, which accurately describes the direction and polarization dependence of the observed excitonic circular dichroism and CPLE, including contributions from both photoluminescence and resonant Raman scattering. Our analysis indicates that molecular chirality drives preferential film alignment with respect to the out-of-plane lattice vector direction, producing the observed anisotropies. This first demonstration in an HOIS system provides a unique route for enhancing polarization-dependent emission, and circularly polarized light transduction more broadly, in self-assembled HOIS.

14 SOLAR ENERGY↗

NASA NTRS2009

Enhancing SERS by Means of Supramolecular Charge Transfer

In a proposed method of sensing small quantities of molecules of interest, surface enhanced Raman scattering (SERS) spectroscopy would be further enhanced by means of intermolecular or supramolecular charge transfer. There is a very large potential market for sensors based on this method for rapid detection of chemical and biological hazards. In SERS, the Raman signals (vibrational spectra) of target molecules become enhanced by factors of the order of 108 when those molecules are in the vicinities of nanostructured substrate surfaces that have been engineered to have plasmon resonances that enhance local electric fields. SERS, as reported in several prior NASA Tech Briefs articles and elsewhere, has remained a research tool and has not yet been developed into a practical technique for sensing of target molecules: this is because the short range (5 to 20 nm) of the field enhancement necessitates engineering of receptor molecules to attract target molecules to the nanostructured substrate surfaces and to enable reliable identification of the target molecules in the presence of interferants. Intermolecular charge-transfer complexes have been used in fluorescence-, photoluminescence-, and electrochemistry-based techniques for sensing target molecules, but, until now, have not been considered for use in SERS-based sensing. The basic idea of the proposed method is to engineer receptor molecules that would be attached to nanostructured SERS substrates and that would interact with the target molecules to form receptor-target supramolecular charge-transfer complexes wherein the charge transfer could be photoexcited.

Wong, Eric↗

NASA NTRS1990

Flow diagnostics in unseeded air

Several approaches are presented for the quantitative measurement of flowfield parameters in high-speed flows. The techniques are developed for the study of air flows in the Mach 2 to Mach 3 regime and can be extended to the hypersonic and subsonic regimes in a straightforward manner. Instantaneous two-dimensional cross-sectional images of the density using UV Rayleigh scattering and the measurement of velocity profiles using the RELIEF technique are shown. The RELIEF technique employs two high-powered lasers separated in frequency by the vibrational frequency of oxygen molecules to write lines across the flowfield by stimulated Raman scattering. The preliminary results indicate that the UV Rayleigh scattering may also be extended to the measurement of velocity and temperature fields by using an atomic or molecular absorption filter window, and that the RELIEF technique can be extended to marking shaped volumetric points or arrays of points in the flowfield for velocity and vorticity measurements.

Miles, R.↗

DOE OSTI2025

Real-Time Detection of Hydrogen and Ammonia Isotopologues for Impurity Removal and Recovery of Tritium

To accommodate gas measurements for impurity removal and recovery of tritium, a silver-coated optical or waveguide is employed for collecting Raman scattered signals to determine relative hydrogen and ammonia isotopologue populations in real time. The data and results presented here demonstrate an analytical methodology for the analysis of four ammonia and three hydrogen isotopologues in a hydrogen–deuterium exchange reaction by gas phase Raman spectroscopy. Standard chemometric modeling techniques effectively unravel the signatures of the isotopologues involved observed here; however, a sophisticated quantum chemical approach supports the spectral assignments. An interpretation of the data presented here can emphasize the practicality and reliability of the gaseous monitoring system in complex chemical environments for the hydrogen fuel economy as well as the more distant energy source from a facility that handles tritium. There are still considerable concerns about the measurement of tritium in isotope separation and radiological impurities from gas processing. A common impurity in gas processing is ammonia, which can form readily in the presence of nitrogen and tritium. Substituted ammonia (NQ 3 ), where Q = H, D, or T, is traditionally removed through getters or diffusers along with other non-hydrogen contaminants. A preferable analytical approach is noninvasive and can be deployed for real-time process evaluation in radiological environments.

Ammonia↗

NASA NTRS1993

Intense backward Raman lasers in CH4 and H2

The conversion efficiency of the first Stokes radiation generated by backward stimulated Raman scattering is measured in CH4 and H2 that are pumped by a third harmonic of a Nd:YAG laser in the 12-55-mJ energy range and in the 0.86-6.00-MPa pressure range. Our experimental results show that CH4 is a better Raman medium than H2 at moderate pressures (a few megapascals) to efficiently generate backward Raman lines.

Sentrayan, Karuppasamy↗

NASA NTRS2001

One-Dimensional Spontaneous Raman Measurements Made in a Gas Turbine Combustor

The NASA Glenn Research Center and the aerospace industry are designing and testing low-emission combustor concepts to build the next generation of cleaner, more fuel efficient aircraft powerplants. These combustors will operate at much higher inlet temperatures and at pressures that are up to 3 to 5 times greater than combustors in the current fleet. From a test and analysis viewpoint, there is an increasing need for measurements from these combustors that are nonintrusive, simultaneous, multipoint, and more quantitative. Glenn researchers have developed several unique test facilities (refs. 1 and 2) that allow, for the first time, optical interrogation of combustor flow fields, including subcomponent performance, at pressures ranging from 1 to 60 bar (1 to 60 atm). Experiments conducted at Glenn are the first application of a visible laser-pumped, one-dimensional, spontaneous Raman-scattering technique to analyze the flow in a high-pressure, advanced-concept fuel injector at pressures thus far reaching 12 bar (12 atm). This technique offers a complementary method to the existing two- and three-dimensional imaging methods used, such as planar laser-induced fluorescence. Raman measurements benefit from the fact that the signal from each species is a linear function of its density, and the relative densities of all major species can be acquired simultaneously with good precision. The Raman method has the added potential to calibrate multidimensional measurements by providing an independent measurement of species number-densities at known points within the planar laser-induced fluorescence images. The visible Raman method is similar to an ultraviolet-Raman technique first tried in the same test facility (ref. 3). However, the visible method did not suffer from the ultraviolet technique's fuel-born polycyclic aromatic hydrocarbon fluorescence interferences.

DeGroot, Wilhelmus A.↗

NASA NTRS2002

One-Dimensional Spontaneous Raman Measurements of Temperature Made in a Gas Turbine Combustor

The NASA Glenn Research Center is working with the aeronautics industry to develop highly fuel-efficient and environmentally friendly gas turbine combustor technology. This effort includes testing new hardware designs at conditions that simulate the high-temperature, high-pressure environment expected in the next-generation of high-performance engines. Glenn has the only facilities in which such tests can be performed. One aspect of these tests is the use of nonintrusive optical and laser diagnostics to measure combustion species concentration, fuel/air ratio, fuel drop size, and velocity, and to visualize the fuel injector spray pattern and some combustion species distributions. These data not only help designers to determine the efficacy of specific designs, but provide a database for computer modelers and enhance our understanding of the many processes that take place within a combustor. Until recently, we lacked one critical capability, the ability to measure temperature. This article summarizes our latest developments in that area. Recently, we demonstrated the first-ever use of spontaneous Raman scattering to measure combustion temperatures within the Advanced Subsonics Combustion Rig (ASCR) sector rig. We also established the highest rig pressure ever achieved for a continuous-flow combustor facility, 54.4 bar. The ASCR facility can provide operating pressures from 1 to 60 bar (60 atm). This photograph shows the Raman system setup next to the ASCR rig. The test was performed using a NASA-concept fuel injector and Jet-A fuel over a range of air inlet temperatures, pressures, and fuel/air ratios.

Hicks, Yolanda R.↗