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At least 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

Interference-free optical detection for Raman spectroscopy

An architecture for spontaneous Raman scattering (SRS) that utilizes a frame-transfer charge-coupled device (CCD) sensor operating in a subframe burst gating mode to realize time-resolved combustion diagnostics is disclosed. The technique permits all-electronic optical gating with microsecond shutter speeds (<5 .mu.s), without compromising optical throughput or image fidelity. When used in conjunction with a pair of orthogonally-polarized excitation lasers, the technique measures time-resolved vibrational Raman scattering that is minimally contaminated by problematic optical background noise.

Nguyen, Quang-Viet↗
DOE OSTI2023

Suppressing parametric instabilities in direct-drive inertial-confinement-fusion plasmas using broadband laser light

It has long been recognized that broadband laser light has the potential to control parametric instabilities in inertial-confinement-fusion (ICF) plasmas. Here, we use results from laser-plasma-interaction simulations to estimate the bandwidth requirements for mitigating the three predominant classes of instabilities in direct-drive ICF implosions: cross-beam energy transfer (CBET), two-plasmon decay (TPD), and stimulated Raman scattering (SRS). We find that for frequency-tripled, Nd:glass laser light, a bandwidth of 8.5 THz can significantly increase laser absorption by suppressing CBET, while ∼13 THz is needed to mitigate absolute TPD and SRS on an ignition-scale platform. None of the glass lasers used in contemporary ICF experiments, however, possess a bandwidth greater than 1 THz and reaching larger values requires the use of an auxiliary broadening technique such as optical parametric amplification or stimulated-rotational-Raman scattering. An arguably superior approach is the adoption of an argon-fluoride (ArF) laser as an ICF driver. Besides having a broad bandwidth of ∼10 THz, the ArF laser also possesses the shortest wavelength (193 nm) that can scale to the high energy/power required for ICF—a feature that helps to mitigate parametric instabilities even further. We show that these native properties of ArF laser light are sufficient to eliminate nearly all CBET scattering in a direct-drive target and also raise absolute TPD and SRS thresholds well above those for broadband glass lasers. The effective control of parametric instabilities with broad bandwidth is potentially a “game changer” in ICF because it would enable higher laser intensities and ablation pressures in future target designs.

Bates, J. W. (ORCID:0000000188087240)↗
NASA NTRS2002

Simultaneous Laser Raman-rayleigh-lif Measurements and Numerical Modeling Results of a Lifted Turbulent H2/N2 Jet Flame in a Vitiated Coflow

An experiment and numerical investigation is presented of a lifted turbulent H2/N2 jet flame in a coflow of hot, vitiated gases. The vitiated coflow burner emulates the coupling of turbulent mixing and chemical kinetics exemplary of the reacting flow in the recirculation region of advanced combustors. It also simplifies numerical investigation of this coupled problem by removing the complexity of recirculating flow. Scalar measurements are reported for a lifted turbulent jet flame of H2/N2 (Re = 23,600, H/d = 10) in a coflow of hot combustion products from a lean H2/Air flame ((empty set) = 0.25, T = 1,045 K). The combination of Rayleigh scattering, Raman scattering, and laser-induced fluorescence is used to obtain simultaneous measurements of temperature and concentrations of the major species, OH, and NO. The data attest to the success of the experimental design in providing a uniform vitiated coflow throughout the entire test region. Two combustion models (PDF: joint scalar Probability Density Function and EDC: Eddy Dissipation Concept) are used in conjunction with various turbulence models to predict the lift-off height (H(sub PDF)/d = 7,H(sub EDC)/d = 8.5). Kalghatgi's classic phenomenological theory, which is based on scaling arguments, yields a reasonably accurate prediction (H(sub K)/d = 11.4) of the lift-off height for the present flame. The vitiated coflow admits the possibility of auto-ignition of mixed fluid, and the success of the present parabolic implementation of the PDF model in predicting a stable lifted flame is attributable to such ignition. The measurements indicate a thickened turbulent reaction zone at the flame base. Experimental results and numerical investigations support the plausibility of turbulent premixed flame propagation by small scale (on the order of the flame thickness) recirculation and mixing of hot products into reactants and subsequent rapid ignition of the mixture.

Cabra, R.↗
DOE OSTI2025

Spontaneously formed phonon frequency combs in van der Waals solid CrGeTe 3 and CrSiTe 3

Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. Here we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe 3 (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest A g mode in CrGeTe 3 splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 200K. These modes correspond to localized oscillations of Ge 2 Te 6 clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe 3 , demonstrating the generalizability of this phenomenon. Our findings demonstrate that Raman scattering effectively probes high-frequency nonlinear phonon modes, offering insight into the generation of long-lived, tunable phonon frequency combs with potential applications in ultrafast material control and phonon-based technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Picosecond Synchronization System for the Distribution of Photon Pairs Through a Fiber Link Between Fermilab and Argonne National Laboratories

Here we demonstrate a three-node quantum network for C-band photon pairs using 2 pairs of 59 km of deployed fiber between Fermi and Argonne National Laboratories. The C-band pairs are directed to nodes using a standard telecommunication switch and the detection system is synchronized to picosecond scale timing resolution using a coexisting O-or L-band optical clock distribution system. We measure a reduction of coincidence to-accidental ratio (CAR) of the C-band pairs from 51 ± 2 to 5.3 ± 0.4 due to Raman scattering of the O-band clock pulses. Despite this reduction, the CAR is nevertheless suitable for quantum networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Raman Microscopy Investigation of GLP-1 Peptide Association with Supported Phospholipid Bilayers

A wide range of important biological processes occur at phospholipid membranes including cell signaling, where a peptide or small molecule targets a membrane-localized receptor protein. In this work, we report the adaptation of confocal-Raman microscopy to quantify populations of unlabeled glucagon-like peptide-1 (GLP-1), a membrane-active 30-residue incretin peptide, in supported phospholipid bilayers deposited on the interior surfaces of wide-pore porous silica particles. Quantification of lipid bilayer-associated peptide is achieved by measuring the Raman scattering intensity of the peptide relative to that of the supported-lipid bilayer, which serves as an internal standard. The dependence of the bilayer-associated GLP-1 population on the solution-concentration of GLP-1 produces an isotherm used to determine the equilibrium constant for peptide-bilayer association and the maximum peptide surface coverage. The maximum coverage of GLP-1 in the lipid bilayer was found to be only 1/5th of a full monolayer based on its hydrodynamic radius. The saturation coverage, therefore, is not limited by the size of GLP-1 but by the ability of the bilayer to accommodate the peptide at high concentrations within the bilayer. Raman spectra show that GLP-1 association with the supported bilayer is accompanied by structural changes consistent with the intercalation of the peptide into bilayer, where the observed increase in acyl-chain order would increase the lipid density and provide free volume needed to accommodate the peptide. Furthermore, these results were compared with previous measurements of the association of fluorescently-labeled GLP-1 with a planar-supported bilayer; the unlabeled peptide exhibits a 3-fold greater affinity for the lipid-bilayer on the porous-silica support suggesting that the fluorescent label alters GLP-1 lipid-bilayer association.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1987

Raman spectroscopic investigations of Hg-Cd-Te melts

Raman scattering measurements are reported for a series of Hg sub1-xCd subxTe (with x less than or =0.2) materials from 295 K (room temperature) to 1126K (up to and above their liquidus temperatures), and for Hg sub1-xCd subxTe (x=0.3) at 285K. The samples were contained in high-temperature optically-flat fused silica cell. Variable temperature measurements were effected in a three-zone, high-temperature furnace equipped with optical windows, and monitored externally by three independently programmable temperature controllers. All studies were made in the backscattering geometry using the 5145 A line of an Ar+ ion laser, with incident power less than 250 mW, as the excitiation source. An intensity enhancement is observed for a mode in each of the compositions studied. The frequency of this mode varies with composition, 142/cm for HgTe, and 128/cm for both the Hg sub1-xCd subxTe (x=0.053 and 0.204) samples. In addition, a shift to lower frequency as a function of temperature is observed in all samples. This shift is most prominent for the x=0.053 sample. The temperature dependence of these modes as the liquidus temperatures are achieved and surpassed for these samples is presented as being associated with a structural transition in the Hg-rich compositions of the Hg sub1-xCd subxTe series. To our knowledge, this is the first reported study of Raman scattering by phonons in the melts of these materials.

Morrobel-Sosa, Anny↗
DOE OSTI2025

Hong-Ou-Mandel interference with a coexisting clock using transceivers for synchronization over deployed fiber

Interference between independently generated photons is a key step towards distributing entanglement over long distances, but it requires synchronization between the distantly-located photon sources. Synchronizing the clocks of such photon sources using coexisting two-way classical optical communications over the same fiber that transports the quantum photonic signals is a promising approach for achieving photon-photon interference over long distances, enabling entanglement distribution for quantum networking using the deployed fiber infrastructure. Here, we demonstrate photon-photon interference by observing the Hong-Ou-Mandel dip between two distantly-located sources: a weak coherent-state source obtained by attenuating the output of a laser and a heralded single-photon source. We achieve a maximum dip visibility of 0.58 +/- 0.04 when the two sources are connected via 4.3 km of deployed fiber. Dip visibilities > 0.5 are nonclassical and a first step towards achieving teleportation over the deployed fiber infrastructure. In our experiment, the classical optical communication is achieved with - 21 dBm of optical signal launch power, which is used to synchronize the clocks in the two independent, distantly-located photon sources. The impact of spontaneous Raman scattering from the classical optical signals is mitigated by appropriate choice of the quantum- and classical-channel wavelengths. All equipment used in our experiment (the photon sources and the synchronization setup) is commercially available. Finally, our experiment represents a scalable approach to enabling practical quantum networking with commercial equipment and coexistence with classical communications in optical fiber.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Magnetosynthesis effect on magnetic order, phonons, and magnons in single-crystal Sr 2 ⁢ IrO 4

It was shown earlier that applying a magnetic field during the growth of Sr 2 IrO 4 , also known as “field-alteration”, induces significant changes to its structural, magnetic, and transport properties. However, the microscopic nature of these changes is enigmatic. Here, in this study, we employed resonant elastic and inelastic x-ray scattering, as well as Raman scattering, to investigate samples from two batches of Sr 2 IrO 4 grown in magnetic fields of different strengths. Our findings reveal that samples grown in a weaker magnetic field have similar magnetic order to non-altered samples, whereas those grown in a stronger field show a different stacking of weak in-plane ferromagnetic moments. Additionally, we observed significant softening and broadening of select Raman-active phonons in the field altered samples, with a stronger effect in the samples grown in the stronger field. We discuss insights that our results provide into the microscopic nature of field-alteration in Sr 2 IrO 4 .

36 MATERIALS SCIENCE↗
NASA NTRS1988

Mobile lidar system for measurement of water vapor mixing ratio and ozone number density

The Water Vapor Lidar was modified and extended to make differential absorption measurements of ozone. Water vapor measurements make use of a weak molecular scattering process known as Raman scattering. It is characterized by a shift in wavelength of the scattered beam of light relative to the incident one. Some of the energy of the incident photon is converted to vibrational or rotational energy within the molecule leaving the scattered photon shifted to a slightly longer wavelength. When performing water vapor measurements, profiles are acquired of water vapor mixing ratio from near the ground to beyond 7 km every 2 minutes. By forming a color composite image of the individual profiles, the spatial and temporal evolution of water vapor is visible with vertical resolution of 75 to 150m and temporal resolution of 2 minutes. The ozone lidar is intended for use as a cross calibration facility for other stationary ozone lidar systems. The ozone measurement employs the technique known as differential absorption. The backscattered laser radiation from two different wavelengths is measured. Successful measurements of 308 nm returns were made from 80 km with an averaging period of 6 hours. Using these data and a standard atmosphere density curve, an ozone number density profile was made which agrees very well with the standard ozone curve between 20 and 40 km.

Whiteman, D.↗
NASA NTRS1999

Pressure Measurements Using an Airborne Differential Absorption Lidar: Analysis of the Systematic Error Sources - Part 1

Remote airborne measurements of the vertical and horizontal structure of the atmospheric pressure field in the lower troposphere are made with an oxygen differential absorption lidar (DIAL). A detailed analysis of this measurement technique is provided which includes corrections for imprecise knowledge of the detector background level, the oxygen absorption fine parameters, and variations in the laser output energy. In addition, we analyze other possible sources of systematic errors including spectral effects related to aerosol and molecular scattering interference by rotational Raman scattering and interference by isotopic oxygen fines.

Flamant, Cyrille N.↗
DOE OSTI2021

Pulse-burst spontaneous Raman thermometry of unsteady wave phenomena in a shock tube

A high-speed temperature diagnostic based on spontaneous Raman scattering (SRS) was demonstrated using a pulse-burst laser. The technique was first benchmarked in near-adiabatic H 2 -air flames at a data-acquisition rate of 5 kHz using an integrated pulse energy of 1.0 J per realization. Both the measurement precision and accuracy in the flame were within 3% of adiabatic predictions. Furthermore, this technique was then evaluated in a challenging free-piston shock tube environment operated at a shock Mach number of 3.5. SRS thermometry resolved the temperature in post-incident and post-reflected shock flows at a repetition rate of 3 kHz and clearly showed cooling associated with driver expansion waves. Collectively, this Letter represents a major advancement for SRS in impulsive facilities, which had previously been limited to steady state regions or single-shot acquisition.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Raster Thomson scattering in large-scale laser plasmas produced at high repetition rate

We present optical Thomson scattering measurements of electron density and temperature in a large-scale (~2 cm) exploding laser plasma produced by irradiating a solid target with a high energy (5-10 J) laser pulse at high repetition rate (1 Hz). The Thomson scattering diagnostic matches this high repetition rate. Unlike previous work performed in single shots at much higher energies, the instrument allows point measurements anywhere inside the plasma by automatically translating the scattering volume using motorized stages as the experiment is repeated at 1 Hz. Measured densities around 4×10 16 cm -3 and temperatures around 7 eV result in a scattering parameter near unity, depending on the distance from the target. The measured spectra show the transition from collective scattering close to the target to non-collective scattering at larger distances. Densities obtained by fitting the weakly collective spectra agree to within 10% with an irradiance calibration performed via Raman scattering in nitrogen.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Time-domain self-broadened and air-broadened nitrogen S-branch Raman linewidths at 80–200 K recorded in an underexpanded jet

We report pure-rotational N 2 –N 2 , N 2 –air, and O 2 –air S-branch linewidths for temperatures of 80–200 K by measuring the time-dependent decay of rotational Raman coherences in an isentropic free-jet expansion from a sonic nozzle. We recorded pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) spectra along the axial centerline of the underexpanded jet, within the barrel shock region upstream of the Mach disk. The dephasing of the pure-rotational Raman coherence was monitored using probe-time-delay scans at different axial positions in the jet, corresponding to varying local temperatures and pressures. The local temperature was obtained by fitting CARS spectra acquired at zero probe time delay, where the impact of collisions was minimal. The measured decay of each available Raman transition was fit to a dephasing constant and corrected for the local pressure, which was obtained from the CARS-measured static temperature and thermodynamic relationships for isentropic expansion from the known stagnation state. Nitrogen self-broadened transitions decayed more rapidly than those broadened in air for all temperatures, corresponding to higher Raman linewidths. In general, the measured S-branch linewidths deviated significantly in absolute and relative magnitudes from those predicted by extrapolating the modified exponential gap model to low temperatures. The temperature dependence of the Raman linewidth for each measured rotational state of nitrogen (J ≤ 10) and oxygen (N ≤ 11) was fit to a temperature-dependent power law over the measurable temperature domain (80–200 K) and extrapolated to both higher rotational states and room temperature. Furthermore, the measured and modeled low-temperature linewidth data provided here will aid low temperature gas-phase pressure measurements with fs/ps CARS.

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

Selective Detection in Impulsive Low-Frequency Raman Imaging Using Shaped Probe Pulses

Impulsive stimulated Raman scattering (ISRS) using a single short femtosecond pump pulse to excite molecular vibrations offers an elegant pump-probe approach to perform vibrational imaging below 200 cm –1 . One shortcoming of ISRS is its inability to offer vibrational selectivity as all the vibrational bonds whose frequencies lie within the short pump-pulse bandwidth are excited. To date, several coherent control techniques have been explored to address this issue and selectively excite a specific molecular vibration by shaping the pump pulse. There has not been any systematic work that reports an analogous shaping of the probe pulse to implement preferential detection. In this work, we focus on vibrational imaging and report vibrational selective detection by shaping the probe pulse in time. Here, we demonstrate numerically and experimentally two pulse-shaping strategies with one functioning as a vibrational notch filter and the other functioning as a vibrational low-pass filter. This enables fast (25 μs/pixel) and selective hyperspectral imaging in the low-frequency regime (< 200 cm –1 ).

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1981

Rayleigh scattering

The physical phenomena of molecular scattering are examined with the objective of redefining the confusing terminology currently used. The following definitions are proposed: molecular scattering consists of Rayleigh and vibrational Raman scattering; the Rayleigh scattering consists of rotational Raman lines and the central Cabannes line; the Cabannes line is composed of the Brillouin doublet and the central Gross or Landau-Placzek line. The term 'Rayleigh line' should never be used.

Young, A. T.↗
DOE OSTI2023

Calibration of the sub-aperture backscatter system on OMEGA EP

The sub-aperture backscatter (SABS) diagnostic on the OMEGA EP Laser System is a diagnostic that is used to measure the backscattered and sidescattered light during laser–plasma interaction experiments that are relevant to high-energy-density physics and inertial confinement fusion. The diagnostic collects stimulated Brillouin scattering (SBS) UV light at around 351 nm and stimulated Raman scattering (SRS) in the visible-light regime in the 420–720-nm-wavelength range and provides spectrally and temporally resolved information. Five 1-in. light collectors, composed of a lens, ground glass diffuser, and coupling into a 300-μm fiber, are positioned behind the last steering mirror on one of the four beamlines to catch a portion of the beam cross section (~1.5%) of the emission that is scattered into the beamline. The SRS light is collected in two light collectors, combined, and transported via graded index fibers to a streaked spectrometer. The SABS-SRS streak spectrometer has a temporal and spectral resolution of 100 ps and 1 nm, respectively. Three other light collectors collect, combine, and transport the SBS signal to a Hamamatsu high-voltage photodiode, where an oscilloscope digitizes the data, providing a time resolution of better than 1 ns. To obtain an absolute energy calibration of SRS measurements, light signals of known energy and wavelength were injected into the light collectors one at a time. The resulting counts on the streak camera charge-coupled device for SRS are then correlated with the incident fluence of scattered light at the light collector in order to allow a quantitative assessment of streak camera sensitivity to determine the energy of the scattered light during experiments. The measurements were performed in situ from the light collectors to the detectors. Other offline measurements provided the transmission of the optics between the target chamber center and the light collectors.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Polarization-separated double-imaging spectroscopy for weakly-ionized plasma diagnostics

Laser Thomson scattering, which provides thermal properties of electrons, has been extensively utilized in plasma diagnostics. However, being a non-resonant linear light scattering technique, it often encounters several challenges in weakly-ionized plasma diagnostics due to spectral overlap with different scatterings induced from other existing species, including Mie, Rayleigh, and rotational Raman scatterings. To address this challenge, we propose an imaging spectroscopy technique, polarization-separated double-imaging spectroscopy (PoDIS), which selectively separates specific scatterings based on their polarization characteristics. Using an atmospheric plasma jet as a plasma source for demonstration, we show that PoDIS can effectively separate rotational Raman and Thomson scatterings from a superimposed spectrum without prior knowledge or assumptions about the thermal properties of neutrals or electrons. This separation enables independent fitting of the rotational Raman and Thomson scattering spectra, allowing for precise determination of the thermal properties of neutral particles and electrons separately.

Bak, Junhwi [Texas A&M University, College Station↗