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NASA NTRS2006

Simultaneous CARS and Interferometric Rayleigh Scattering

This paper reports for the first time the combination of a dual-pump coherent anti-Stokes Raman scattering system with an interferometric Rayleigh scattering system (CARS - IRS) to provide time-resolved simultaneous measurement of multiple properties in combustion flows. The system uses spectrally narrow green (seeded Nd:YAG at 532 nm) and yellow (552.9 nm) pump beams and a spectrally-broad red (607 nm) beam as the Stokes beam. A spectrometer and a planar Fabry-Perot interferometer used in the imaging mode are used to record the spectrally broad CARS spectra and the spontaneous Rayleigh scattering spectra, respectively. Time-resolved simultaneous measurement of temperature, absolute mole fractions of N2, O2, and H2, and two components of velocity in a Hencken burner flame were performed to demonstrate the technique.

Bivolaru, Daniel↗

NASA NTRS1981

Laser remote sensing of marine sediment load and algal pigments: Laboratory experiments

The fluorescence emission spectra for estuarine water samples excited by an argon laser at 514.5 nm were analyzed. The features of interest were: (1) scattering at the laser wavelength by particulates (Mie); (2) fluorescence from the pigments chlorophyl a and phycoerythrin; (3) Raman scattering by water; and (4) fluorescence by dissolved organic matter. It is shown that these intensities increase with the concentration of the corresponding material and decrease with attenuation. Since the concentration of water is constant the Raman intensity provides a direct measure of attenuation.

Exton, R. J.↗

NASA NTRS1984

Lyman-Alpha Aurora

The existence of intense and variable H Ly a emission from Uranus is demonstrated utilizing the monochromatic imaging capabilities of the International Ultraviolet Explorer satellite. A series of 14 observations, using the IUE short wavelength spectrograph in low dispersion and covering the period from 3 March 1982 through 2 September 1983, shows the disk averaged Ly a brightness of Uranus to vary between 690 and 2230 Rayleighs. Model calculations indicates that 400 R of this emission can be attributed to resonant scattering of solar Ly a radiation. An upper limit of 100 R is obtained for the Raman scattering of solar Ly a by H2 (1280 A). This implies that 300 R is contributed to the planetary Ly a emission by Rayleigh scattering. In addition to being unexpectedly strong, the Uranian Ly a emission has been observed to vary by a factor of two in one 24 hr period and by about 50% in one 5 hr period.

Durrance, S. T.↗

NASA NTRS1987

The temperature dependence of inelastic light scattering from small particles for use in combustion diagnostic instrumentation

A computer calculation of the expected angular distribution of coherent anti-Stokes Raman scattering (CARS) from micrometer size polystyrene spheres based on a Mie-type model, and a pilot experiment to test the feasibility of measuring CARS angular distributions from micrometer size polystyrene spheres by simply suspending them in water are discussed. The computer calculations predict a very interesting structure in the angular distributions that depends strongly on the size and relative refractive index of the spheres.

Cloud, Stanley D.↗

NASA NTRS2018

Optical Characterization of Fuel Injection in a Flame Tube Combustor Using a GE TAPS Injector Configuration

This paper presents results in which we compare fuel staging and its effect on fuel spray pattern, velocity and speciation during combustion for several inlet conditions using a GE TAPS injector configuration. Planar laser-induced fluorescence (PLIF), particle image velocimetry (PIV) and phase Doppler interferometry (PDI) were used to investigate spray patterns and velocity. The 2D PIV provides slices in the flow of axial-vertical or axial horizontal velocity components. With 3D PDI, we obtained 3 components of velocity, and fuel drop sizes. Chemiluminescence imaging and spontaneous Raman scattering (SRS) were used to investigate flame structure, species location and relative species concentration. Phase Doppler and PIV data were acquired using scatter from fuel droplets; therefore, those data were obtained only at the pilot-only test points. Raman measurements were acquired only at 10/90 split points to avoid droplets.

optical diagnostics↗

NASA NTRS2018

Flame Tube Testing of a GEA TAPS Injector: Effects of Fuel Staging on Combustor Fuel Spray Patterns, Flow Structure, and Speciation

GE TAPS↗

DOE OSTI2025

Ultra-high Information-content Chemical Imaging with Broadband Coherent Anti-Stokes Raman and Two-photon Fluorescence Lifetime Microscopy

Raman fingerprint spectroscopy and fluorescence lifetime imaging are emerging tools for studying metabolic profiles of biological specimens. While Raman fingerprint spectroscopy detects intrinsic molecular vibrations that reflect the molecular composition and chemical environment of a sample, fluorescence lifetime imaging measures changes in the excited-state lifetime of fluorophores that are sensitive to their microenvironments. Here, we present a multimodal imaging platform combining broadband coherent anti-Stokes Raman scattering (BCARS) and two-photon fluorescence lifetime imaging (2p-FLIM) microscopy that can acquire biologically relevant Raman fingerprint spectra and fluorescence lifetime signals in vivo and simultaneously. The tremendous chemical information obtained from spatially co-registered BCARS and 2p-FLIM images allows us to characterize the subtle differences between sub-cellular compartments and verify the potential false-positive results generated by fluorescence imaging alone. This is demonstrated by directly comparing the BCARS, 2p-FLIM, and two-photon excitation fluorescence(TPEF) signals simultaneously obtained from the same dye-stained organelle in the live, intact C. elegans expressing a green fluorescent protein (GFP) marker. In this work, we introduce the BCARS/2p-FLIM/TPEF setup scheme, the image acquisition steps, data processing, and representative results showing that the cross-modality imaging method enables rigorous characterization and in vivo detection at sub-cellular resolution. Furthermore, this protocol provides a framework for simultaneous chemical and fluorescence lifetime imaging to improve the accuracy of biological interpretation in complex living systems.

Xu, Haoyu [Georgia Institute of Technology, Atlant↗

NASA NTRS1973

Remote Measurement of Atmospheric Temperatures By Raman Lidar

The Raman shifted return of a lidar, or optical radar, system has been utilized to make atmospheric temperature measurements. These measurements were made along a horizontal path at temperatures between -20 C and +30 C and at ranges of about 100 meters. The temperature data were acquired by recording the intensity ratio of two portions of the Raman spectrum which were simultaneously sampled from a preset range. The lidar unit employed in this testing consisted of a 4 joule-10ppm laser operating at 694.3 nm, a 10-inch Schmidt-Cassegrain telescope, and a system of time-gated detection and signal processing electronics. The detection system processed three return signal wavelength intervals - two intervals along the rotational Raman scattered spectrum and one interval centered at the Rayleigh-Mie scattered wavelength. The wavelength intervals were resolved by using a pellicle beam splitter and three optical interference filters. Raman return samples were taken from one discrete range segment during each test shot and the signal intensities were displayed in digital format. The Rayleigh-Mie techniques. The test site utilized to evaluate this measurement technique encompassed a total path length of 200 meters. Major components of the test site included a trailer-van housing the lidar unit, a controlled environment test zone, and a beam terminator. The control zone which was located about 100 meters from the trailer was 12 meters in length, 2.4 meters in diameter, and was equipped with hinged doors at each end. The temperature of the air inside the zone could be either raised or lowered with respect to ambient air through the use of infrared heaters or a liquid-nitrogen cooling system. Conditions inside the zone were continuously monitored with a thermocouple rake assembly. The test path length was terminated by a 1.2 meter square array of energy absorbing cones and a flat black screen. Tests were initially conducted at strictly ambient conditions utilizing the normal outside air temperatures as a test parameter. These tests provided a calibration of the Raman intensity ratio as a function of' temperature for the particular optical-filter arrangement used in this system while also providing a test of' the theoretical prediction formulated in the design of the system. Later tests utilized zone temperatures above and below ambient to provide temperature gradient data. These tests indicate that ten shots, or one minute of' data acquisition, from a 100 meter range can provide absolute temperature measurements with an accuracy of + 30 C and a range resolution of about 5 meters. Because this measurement accuracy compares well with that predicted for this particular unit, it is suggested that a field-application system could be built with signif'icant improvements in both absolute accuracy and range.

Salzman, Jack A.↗

DOE OSTI2021

Enhanced superconductivity and ferroelectric quantum criticality in plastically deformed strontium titanate

The properties of quantum materials are commonly tuned using experimental variables such as pressure, magnetic field and doping. Here we explore a different approach using irreversible, plastic deformation of single crystals. We show that compressive plastic deformation induces low-dimensional superconductivity well above the superconducting transition temperature (Tc) of undeformed SrTiO3, with evidence of possible superconducting correlations at temperatures two orders of magnitude above the bulk Tc. The enhanced superconductivity is correlated with the appearance of self-organized dislocation structures, as revealed by diffuse neutron and X-ray scattering. We also observe deformation-induced signatures of quantum-critical ferroelectric fluctuations and inhomogeneous ferroelectric order using Raman scattering. Our results suggest that strain surrounding the self-organized dislocation structures induces local ferroelectricity and quantum-critical dynamics that strongly influence Tc, consistent with a theory of superconductivity enhanced by soft polar fluctuations. Our results demonstrate the potential of plastic deformation and dislocation engineering for the manipulation of electronic properties of quantum materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1998

Towards quantifying mesoscale flows in the troposphere using Raman lidar and Sondes

Water vapor plays an important role in the energetics of the boundary layer processes which in turn play a key role in regulating regional and global climate. It plays a primary role in Earth's hydrological cycle, in radiation balance as a direct absorber of infrared radiation, and in atmospheric circulation as a latent heat energy source, as well as in determining cloud development and atmospheric stability. Water vapor concentration, expressed as a mass mixing ratio (g kg(exp -l)), is conserved in all meteorological processes except condensation and evaporation. This property makes it an ideal choice for studying many of the atmosphere's dynamic features. Raman scattering measurements from lidar also allow retrieval of water vapor mixing ratio profiles at high temporal and vertical resolution. Raman lidars sense water vapor to altitudes not achievable with towers and surface systems, sample the atmosphere at much higher temporal resolution than radiosondes or satellites, and do not require strong vertical gradients or turbulent fluctuations in temperature that is required by acoustic sounders and radars. Analysis of highly-resolved water vapor profiles are used here to characterize two important mesoscale flows: thunderstorm outflows and a cold front passage. The data were obtained at the Atmospheric Radiation Measurement Site (CART) by the groundbased Department of Energy/Sandia National Laboratories lidar (CART Raman lidar or CARL) and Goddard Space Flight Center Scanning Raman Lidar (SRL). A detailed discussion of the SRL and CARL performance during the IOPs is given by others in this meeting.

Demoz, B.↗

NASA NTRS1986

Investigation of breadboard temperature profiling system for SSME fuel preburner diagnostics

The feasibility of measuring temperatures in the space shuttle main engine (SSME) fuel preburner using spontaneous Raman scattering from molecular hydrogen was studied. Laser radiation is transmitted to the preburner through a multimode optical fiber. Backscattered Raman-shifted light is collected and focused into a second fiber which connects to a remote-located spectrograph and a mutlichannel optical detector. Optics collimate and focus laser light from the transmitter fiber defining the probe volume. The high pressure, high temperature preburner environment was simulated by a heated pressure cell. Temperatures determined by the distribution of Q-branch co-vibrational transitions demonstrate precision and accuracy of 3%. It is indicated heat preburner temperatures can be determined with 5% accuracy with spatial resolution less than 1 cm and temporal resolution of 10 millisec at the nominal preburner operation conditions.

Shirley, J. A.↗

NASA NTRS1990

Some optical and electron microscope comparative studies of excimer laser-assisted and nonassisted molecular-beam epitaxically grown thin GaAs films on Si

The quality of GaAs thin films grown via MBE under pulsed excimer laser irradiation on Si substrates is examined in both laser-irradiated and nonirradiated areas using Raman scattering, Rayleigh scattering, and by photoluminescence (PL), as a function of temperature, and by TEM. The temperature dependence of the PL and Raman peak positions indicates the presence of compressive stress in the thin GaAs films in both laser-irradiated and nonirradiated areas. This indicates incomplete homogeneous strain relaxation by dislocations at the growth temperature. The residual compressive strain at the growth temperature is large enough such that even with the introduction of tensile strain arising from the difference in thermal expansion coefficients of GaAs and Si, a compressive strain is still present at room temperature for these thin GaAs/Si films.

Lao, Pudong↗

DOE OSTI2023

Raman Spectroscopy

Raman spectroscopy is one of the mostly utilized optical spectroscopic tools for revealing both the catalyst structure and surface chemistry in heterogeneous catalysis. It has recently seen increasing role in catalysis research, thanks to the development of new Raman instrumentations, reactors, and combination with other techniques, leading to in situ and operando studies with significant temporal and spatial resolutions. This chapter aimed to provide a general overview of the applications of Raman spectroscopy in heterogeneous catalysis. It starts with an introduction to the fundamentals of Raman scattering including theory and pros and cons for catalysis research; followed by a description of the typical setup of a Raman system and recent advances in Raman instrumentations; then a chronology of the applications of Raman spectroscopy for ex situ, in situ, and operando studies of catalysis; elucidations of the advances in improving the temporal and spatial resolution of Raman spectroscopy of catalysis; Raman application case studies related to catalyst synthesis, treatments, and function under reaction conditions; illustrations of the power of multimodal approach including Raman spectroscopy in catalysis research; and ended with a brief summary and a future outlook.

Braatz, Jisue↗

DOE OSTI2023

Raman Spectroscopy

Braatz, Jisue↗

DOE OSTI2020

Comparable Enhancement of TERS Signals from WSe 2 on Chromium and Gold

Plasmonic tip-sample junctions, at which the incident and scattered optical fields are localized and optimally enhanced, are often exploited to achieve ultrasensitive and highly spatially localized tip-enhanced Raman scattering (TERS). Recent work has demonstrated that the sensitivity and spatial resolution that are required to probe single molecules are attainable in such platforms. In this work, we observe and rationalize comparable TERS from few-layer WSe 2 single crystals exfoliated onto Au- and Cr-coated Si substrates, using a plasmonic TERS probe excited with a 638-nm laser. Our experimental observations are supported by finite-difference time-domain simulations that illustrate that the attainable field enhancement factors at the Au-Au and Au-Cr tip-sample nanojunctions are comparable in magnitude. Furthermore, through a combined experimental and theoretical analysis, we propose that besides Au/Ag, several metallic substrates may be used to record bright TERS spectral images.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Layered topological semimetal GaGeTe: New polytype with non-centrosymmetric structure

GaGeTe is a layered van der Waals material composed of germanene and GaTe sublayers that has been recently predicted to be a basic Z 2 topological semimetal. To date, only one polytype of GaGeTe is known with trigonal centrosymmetric structure (α phase, space group R-3m, No. 166). Here we show that as-grown samples of GaGeTe show traces of at least another polytype with hexagonal non-centrosymmetric structure (β phase, space group P6 3 mc, No. 186). Moreover, we suggest that another bulk hexagonal polytype (γ phase, space group P-3m1, No. 164) could also be found near room conditions. Both α and β polytypes have been identified and characterized by means of X-ray diffraction and Raman scattering measurements with the support of ab initio calculations. We provide the vibrational properties of both polytypes and show that the Raman spectrum reported for GaGeTe almost forty years ago and attributed to the α phase, was, in fact, that of the secondary β phase. Additionally, we show that a Fermi resonance occurs in α-GaGeTe under non-resonant excitation conditions, but not under resonant excitation conditions. Theoretical calculations show that bulk β-GaGeTe is a non-centrosymmetric weak topological semimetal with even smaller lattice thermal conductivity than centrosymmetric bulk α-GaGeTe. In perspective, our work paves the way for the control and engineering of GaGeTe polytypes to design and implement complex van der Waals heterostructures formed by a combination of centrosymmetric and non-centrosymmetric layers of up to three different polytypes in a single material, suitable for a number of fundamental studies and technological applications.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Accurate in vivo tumor detection using plasmonic-enhanced shifted-excitation Raman difference spectroscopy (SERDS)

For the majority of cancer patients, surgery is the primary method of treatment. In these cases, accurately removing the entire tumor without harming surrounding tissue is critical; however, due to the lack of intraoperative imaging techniques, surgeons rely on visual and physical inspection to identify tumors. Surface-enhanced Raman scattering (SERS) is emerging as a non-invasive optical alternative for intraoperative tumor identification, with high accuracy and stability. However, Raman detection requires dark rooms to work, which is not consistent with surgical settings. Methods: Herein, we used SERS nanoprobes combined with shifted-excitation Raman difference spectroscopy (SERDS) detection, to accurately detect tumors in xenograft murine model. Results: We demonstrate for the first time the use of SERDS for in vivo tumor detection in a murine model under ambient light conditions. We compare traditional Raman detection with SERDS, showing that our method can improve sensitivity and accuracy for this task. Conclusion: Our results show that this method can be used to improve the accuracy and robustness of in vivo Raman/SERS biomedical application, aiding the process of clinical translation of these technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1973

A new effect in the depolarization of resonant light scattering from molecules in the vapor phase: I2

Theoretical discussions of the depolarization ratios in two types of resonance processes are given. These processes are discrete state resonance fluorescence, and Raman scattering when the resonance is between a bound state and evanescent-dissociative states. Theory predicts a dramatic difference for these two cases due to a quantum mechanical phase cancellation in the case of virtual dissociative states. The predictions have been verified experimentally.

Silverstein, S. D.↗