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At least 469 records · Page 26

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↗

Video-rate Raman-based metabolic imaging by Airy light-sheet illumination and photon-sparse detection

Despite its massive potential, Raman imaging represents just a modest fraction of all research and clinical microscopy to date. This is due to the ultralow Raman scattering cross-sections of most biomolecules that impose low-light or photon-sparse conditions. Bioimaging under such conditions is suboptimal, as it either results in ultralow frame rates or requires increased levels of irradiance. Here, we overcome this tradeoff by introducing Raman imaging that operates at both video rates and 1,000-fold lower irradiance than state-of-the-art methods. To accomplish this, we deployed a judicially designed Airy light-sheet microscope to efficiently image large specimen regions. Further, we implemented subphoton per pixel image acquisition and reconstruction to confront issues arising from photon sparsity at just millisecond integrations. We demonstrate the versatility of our approach by imaging a variety of samples, including the three-dimensional (3D) metabolic activity of single microbial cells and the underlying cell-to-cell variability. To image such small-scale targets, we again harnessed photon sparsity to increase magnification without a field-of-view penalty, thus, overcoming another key limitation in modern light-sheet microscopy.

60 APPLIED LIFE SCIENCES↗

Vibrational modes and crystallographic structure of Cd 3 As 2 and (Cd 1-x Zn x ) 3 As 2 epilayers

Low-temperature Raman scattering is used to study the crystal structure of molecular-beam epitaxially grown layers of the Dirac semimetal Cd 3 As 2 and its related alloy (Cd 1-x Zn x ) 3 As 2 . The combination of narrow-linewidth spectra, multiple growth directions and full polarization analysis allows improved accuracy in identifying the irreducible representation of over 57 Raman-active vibrations. Several disagreements with previous identifications are found. Structurally, the results agree with the centrosymmetric I41/acd space group of bulk-grown Cd 3 As 2 and are clearly distinct from the Raman spectra of nanoscale platelets and wires. Three-fold twinning is seen in (112) Cd 3 As 2 grown on (111) zincblende substrates corresponding to the three possible tetragonal orientations. In dilute (Cd 1-x Zn x ) 3 As 2 , phonons have a frequency and scattering amplitude dependence on Zn concentration that is continuous with Cd 3 As 2 but at least one frequency is absent at the alloy endpoint, preventing a simple one-mode description of the alloy phonon.

36 MATERIALS SCIENCE↗

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.↗

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.↗

Significantly increased Raman enhancement on defect-rich O-incorporated 1T-MoS 2 nanosheets

Improving charge transfer is the key to the performance of non-noble metal semiconductor-based surface enhanced Raman scattering (SERS) substrates. In this work, the O-incorporated 1T-MoS 2 nanosheets with rich sulfur defects (ID-MoS 2 ) are obtained by simple calcination of 1T-MoS 2 nanosheets in air atmosphere. Using rhodamine 6G (R6G) as typical probe molecules, ID-MoS 2 nanosheets show ultrahigh Raman enhancement effects with an enhancement factor of 1.24 × 10 7 due to sulfur defects and O incorporation in the 1T-MoS 2 lattice. First-principle density functional theory calculations suggest that the existence of sulfur defects and O incorporation significantly increase the Fermi energy level (E f ) and electronic density of states of ID-MoS 2 . Furthermore, O incorporation can enhance the interactions between the substrate and the adsorbed molecules through electrostatic and hydrogen bonding. All these improve the charge transfer resonance and result in the remarkable SERS activity of ID-MoS 2 nanosheets. This is the first study on the increasing SERS performance of semiconductor substrates by simultaneously employing defect and dopant incorporation. This study provides an approach to optimize the performance of semiconductor-based SERS substrates.

36 MATERIALS SCIENCE↗

Detection of chiral spin fluctuations driven by frustration in Mott insulators

Topologically ordered states, such as chiral spin liquids, have been proposed as candidates that host fraction alized excitations. However, detecting chiral character or proximity to these nontrivial states remains a challenge. Resonant Raman scattering can be a powerful tool for detecting chiral fluctuations, as the 𝐴 2⁢𝑔 channel probes excitations with broken time-reversal symmetry and local chiral order. Here, we use exact diagonalization to characterize the resonant 𝐴 2⁢𝑔 channel, alongside two-magnon scattering in 𝐵 1⁢𝑔 and 𝐸 𝑔 channels, for the Hubbard model on lattices with increasing levels of geometric spin frustration, where tuning the incident energy near the Mott gap reveals strong chiral spin excitation intensity. In conclusion, increased spin frustration in the Mott insulator results in an overall softening of the Raman 𝐴 2⁢𝑔 response, indicating a tendency toward low energy chiral-chiral fluctuations in Mott insulators with magnetic frustration and proximity to chiral spin liquid states that can potentially be tuned by external perturbations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Compact Raman Spectrometers Would Detect Hydrogen

Compact Raman spectrometers developed to measure concentrations of hydrogen as low as hundreds of parts per million in air, nitrogen, or other carrier gases. Advantages include speed, dynamic range, and ease of calibration. Design concept incorporates Raman-scattering apparatus into compact instrument of hydrogen leaking into stream of gas or into gas enclosed in small space. Should hydrogen-fueled cars and trucks come into widespread use, instruments used to detect leaks from vehicles and supply equipment, to help prevent explosions. Similar spectrometers developed to detect other gases emitting characteristic Raman spectra.

Helms, William R.↗

PIV and Rotational Raman-Based Temperature Measurements for CFD Validation in a Single Injector Cooling Flow

Film cooling is used in a wide variety of engineering applications for protection of surfaces from hot or combusting gases. The design of more efficient thin film cooling geometries/configurations could be facilitated by an ability to accurately model and predict the effectiveness of current designs using computational fluid dynamics (CFD) code predictions. Hence, a benchmark set of flow field property data were obtained for use in assessing current CFD capabilities and for development of better turbulence models. Both Particle Image Velocimetry (PIV) and spontaneous rotational Raman scattering (SRS) spectroscopy were used to acquire high quality, spatially-resolved measurements of the mean velocity, turbulence intensity and also the mean temperature and normalized root mean square (rms) temperatures in a single injector cooling flow arrangement. In addition to flowfield measurements, thermocouple measurements on the plate surface enabled estimates of the film effectiveness. Raman spectra in air were obtained across a matrix of radial and axial locations downstream from a 68.07 mm square nozzle blowing heated air over a range of temperatures and Mach numbers, across a 30.48cm long plate equipped with a single injector cooling hole. In addition, both centerline streamwise 2-component PIV and cross-stream 3-component Stereo PIV data at 15 axial stations were collected in the same flows. The velocity and temperature data were then compared against Wind-US CFD code predictions for the same flow conditions. The results of this and planned follow-on studies will support NASA's development and assessment of turbulence models for heated flows.

Wernet, Mark P.↗

PIV and Rotational Raman-Based Temperature Measurements for CFD Validation in a Single Injector Cooling Flow

Film cooling is used in a wide variety of engineering applications for protection of surfaces from hot or combusting gases. The design of more efficient thin film cooling geometries/configurations could be facilitated by an ability to accurately model and predict the effectiveness of current designs using computational fluid dynamics (CFD) code predictions. Hence, a benchmark set of flow field property data were obtained for use in assessing current CFD capabilities and for development of better turbulence models. Both Particle Image Velocimetry (PIV) and spontaneous rotational Raman scattering (SRS) spectroscopy were used to acquire high quality, spatially-resolved measurements of the mean velocity, turbulence intensity and also the mean temperature and normalized root mean square (rms) temperatures in a single injector cooling flow arrangement. In addition to flowfield measurements, thermocouple measurements on the plate surface enabled estimates of the film effectiveness. Raman spectra in air were obtained across a matrix of radial and axial locations downstream from a 68.07 mm square nozzle blowing heated air over a range of temperatures and Mach numbers, across a 30.48cm long plate equipped with a single injector cooling hole. In addition, both centerline streamwise 2-component PIV and cross-stream 3-component Stereo PIV data at 15 axial stations were collected in the same flows. The velocity and temperature data were then compared against Wind-US CFD code predictions for the same flow conditions. The results of this and planned follow-on studies will support NASA's development and assessment of turbulence models for heated flows.

Turbulence Modeling↗

Near-octave lithium niobate soliton microcomb

Thin film lithium niobate (LN) is bringing renewed potential to the realm of integrated photonics. Its strong quadratic and cubic nonlinearities as well as wide transparency window are ideal for realizing on-chip self-referenced soliton microcombs. However, broadband Kerr cavity soliton generation in LN thin films remains challenging due to limited dispersion control and competition from strong stimulated Raman scattering (SRS). Here, we demonstrate the generation of soliton microcombs in LN thin films featuring broad spectral spans up to 4/5 octaves with the emission of dual dispersion waves (2/3 octaves apart) and sub-terahertz repetition rates (down to 335 GHz) by suppressing strong SRS. Numerical simulations based on coupled-mode equations that incorporate Raman effects further elucidate the soliton dynamics in this highly Raman-active material system.

Gong, Zheng (ORCID:0000000301704870)↗

Laser Raman diagnostics in subsonic and supersonic turbulent jet diffusion flames

Ultraviolet (UV) spontaneous vibrational Raman scattering combined with laser-induced predissociative fluorescence (LIPF) is developed for temperature and multi-species concentration measurements. Simultaneous measurements of temperature, major species (H2, O2, N2, H2O), and minor species (OH) concentrations are made with a 'single' narrow band KrF excimer laser in subsonic and supersonic lifted turbulent hydrogen-air diffusion flames. The UV Raman system is calibrated with a flat-flame diffusion burner operated at several known equivalence ratios from fuel-lean to fuel-rich. Temperature measurements made by the ratio of Stokes/anti-Stokes signal and by the ideal gas law are compared. The single shot measurement precision for concentration and temperature measurement is 5 to 10 pct. Calibration constants and bandwidth factors are determined from the flat burner measurements and used in a data reduction program to arrive at temperature and species concentration measurements. These simultaneous measurements of temperature and multi-species concentrations allow a better understanding of the complex turbulence-chemistry interactions and provide information for the input and validation of CFD models.

Cheng, T. S.↗

Dynamic fingerprint of fractionalized excitations in single-crystalline Cu3Zn(OH)6FBr

Abstract Beyond the absence of long-range magnetic orders, the most prominent feature of the elusive quantum spin liquid (QSL) state is the existence of fractionalized spin excitations, i.e., spinons. When the system orders, the spin-wave excitation appears as the bound state of the spinon-antispinon pair. Although scarcely reported, a direct comparison between similar compounds illustrates the evolution from spinon to magnon. Here, we perform the Raman scattering on single crystals of two quantum kagome antiferromagnets, of which one is the kagome QSL candidate Cu 3 Zn(OH) 6 FBr, and another is an antiferromagnetically ordered compound EuCu 3 (OH) 6 Cl 3 . In Cu 3 Zn(OH) 6 FBr, we identify a unique one spinon-antispinon pair component in the E 2g magnetic Raman continuum, providing strong evidence for deconfined spinon excitations. In contrast, a sharp magnon peak emerges from the one-pair spinon continuum in the E g magnetic Raman response once EuCu 3 (OH) 6 Cl 3 undergoes the antiferromagnetic order transition. From the comparative Raman studies, we can regard the magnon mode as the spinon-antispinon bound state, and the spinon confinement drives the magnetic ordering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

First Look at the Upper Tropospheric Ozone Mixing Ratio from OMI Estimated using the Cloud Slicing Technique

The Cloud Slicing technique has emerged as a powerful tool for the study of ozone in the upper troposphere. In this technique one looks at the variation with cloud height of the above-cloud column ozone derived from the backscattered ultraviolet instruments, such as TOMS, to determine the ozone mixing ratio. For this technique to work properly one needs an instrument with relatively good horizontal resolution with very good signal to noise in measuring above-cloud column ozone. In addition, one needs the (radiatively) effective cloud pressure rather than the cloud-top pressure, for the ultraviolet photons received by a satellite instrument are scattered from inside the cloud rather than from the top. For this study we use data from the OMI sensor, which was recently launched on the EOS Aura satellite. OMI is a W-Visible backscattering instrument with a nadir pixel size of 13 x 24 km. The effective cloud pressure is derived from a new algorithm based on Rotational Raman Scattering and O2-O2, absorption in the 340-400 nm band of OMI.

Bhartia, Pawan K.↗

Raman Temperature and Density Measurements in Supersonic Jets

Prediction of flow-field properties in supersonic jets using computational fluid dynamics (CFD) code predictions has become routine; however, obtaining accurate solutions becomes more challenging when there is a significant temperature difference between the jet core and the ambient air and/or compressibility effects are significant. Benchmark sets of flow field property data are required in order to assess current CFD capabilities and develop better modeling approaches for these turbulent flow fields where accurate calculation of temperatures and turbulent heat flux is important. Particle Image Velocimetry (PIV), spontaneous rotational Raman scattering (SRS) spectroscopy and Background Oriented Schlieren (BOS) have been previously used to acquire measurements of the mean and root mean square (rms) velocities, the mean and rms gas temperatures and density gradients in subsonic jet flows and film cooling flows. In this work, the ability to measure density is added to the list of measurands available using the acquired Raman spectra. The suite of measurement techniques are now applied to supersonic jet flows. The computation of the local gas pressure in the potential core of an over-expanded jet is demonstrated using the Raman measured gas temperature and density. Additionally, a unique density feature in temperature matched, perfectly expanded jet flow shear layers identified using BOS was verified using the Raman measurement technique. These non-intrusive flow measurements are compared against RANS predictions of the supersonic jet flow properties as a means of assessing their prediction accuracy.

Raman Spectroscopy↗

Theory of stimulated and spontaneous axion scattering.

We present a theory for nonlinear, resonant excitation of dynamical axions by counterpropagating electromagnetic waves in materials that break both 𝒫 and 𝒯 symmetries. We show that dynamical axions can mediate an exponential growth in the amplitude of the lower frequency (Stokes) beam. We also discuss spontaneous generation of a counterpropagating Stokes mode, enabled by resonant amplification of quantum and thermal fluctuations in the presence of a single pump laser. Remarkably, the amplification can be orders of magnitude larger than that obtained via stimulated Brillouin and Raman scattering processes, and can be modulated with the application of external magnetic fields, making stimulated axion scattering promising for optoelectronics applications.

Smith, M.↗

The Influence of Structural Dynamics in Two-Dimensional Hybrid Organic–Inorganic Perovskites on Their Photoluminescence Efficiency — Neutron Scattering Analysis

Two-dimensional hybrid organic–inorganic perovskites (HOIPs) have emerged as promising materials for light-emitting diode applications. In this study, by using time-of-flight neutron spectroscopy we identified and quantitatively separated the lattice vibrational and molecular rotational dynamics of two perovskites, butylammonium lead iodide (BA)2PbI4 and phenethyl-ammonium lead iodide (PEA) 2 PbI 4 . By examining the corresponding temperature dependence, we found that the lattice vibrations, as evidenced by neutron spectra, are consistent with the lattice dynamics obtained from Raman scattering. We revealed that the rotational dynamics of organic molecules in these materials tend to suppress their photoluminescence quantum yield (PLQY) while the vibrational dynamics did not show predominant correlations with the same. Additionally, we observed photoluminescence emission peak splitting for both systems, which becomes prominent above certain critical temperatures where the suppression of PLQY begins. This study suggests that the rotational motions of polarized molecules may lead to a reduction in exciton binding energy or the breaking of degeneracy in exciton binding energy levels, enhancing non-radiative recombination rates, and consequently reducing photoluminescence yield. These findings offer a deeper understanding of fundamental interactions in 2D HOIPs and could guide the design of more efficient light-emitting materials for advanced technological applications.

Rajeev, Haritha Sindhu [Univ. of Virginia, Charlot↗

PIV and Rotational Raman-Based Temperature Measurements for CFD Validation of a Perforated Plate Cooling Flow: Part I

Film cooling is used in a wide variety of engineering applications for protection of surfaces from hot or combusting gases. The design of more efficient film cooling geometries/configurations could be facilitated by an ability to accurately model and predict the effectiveness of current designs using computational fluid dynamics (CFD) code predictions. Hence, a benchmark set of flow field property data was obtained to assess current CFD capabilities and develop better modeling approaches for these turbulent flow fields where accurate calculation of turbulent heat flux is important. Both Particle Image Velocimetry (PIV) and spontaneous rotational Raman scattering (SRS) spectroscopy were used to acquire high quality, spatially-resolved measurements of the mean and root mean square (rms) velocities as well as the mean and rms temperatures in a film cooling flow field. In addition to off-body flow field measurements, infrared thermography (IR) and thermocouple measurements on the plate surface enabled estimates of the film effectiveness. Raman spectra in air were obtained across a matrix of axial locations downstream from a 68.07 mm square nozzle blowing heated air over a range of temperatures (up to TR = 2.7) and Mach numbers (up to Mach 0.9), across a 30.48 cm long plate equipped with three patches of 45 small (~1 mm) diameter cooling holes arranged in a staggered configuration. In addition, both streamwise 2-component PIV (on the plate centerline) and cross-stream 3-component Stereo PIV data at 14 axial stations were collected in the same flows. Only a subset of the data collected in the test program is included in this Part I report. The rest of the data will be published in a future report, Part II, along with planned CFD predictions of the complex cooling film flow. The entire data set of Raman temperature data, PIV velocity data and IR camera data covering the Set Points 23 and 49 in the test matrix in Table 1 is available in an accompanying DVD (available online from www.sti.nasa.gov) for those interested in further analysis.

Nozzle↗