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At least 19 records

Simultaneous observation of rotational coherent Stokes Raman scattering and coherent anti-Stokes Raman scattering in air and nitrogen

Rotational coherent Stokes Raman scattering (CSRS) and coherent anti-Stokes Raman scattering (CARS) in air and in nitrogen were observed simultaneously by using broadband generation and detection. In the broadband technique used, the entire CARS and CSRS spectrum was generated in a single laser pulse; the CSRS and CARS signals were dispersed by a spectrograph and detected simultaneously by an optical multichannel analyzer. A three-dimensional phase-matching geometry was used to achieve spatial resolution of the CSRS and CARS beams from the input beams. Under resonant conditions, similar experiments may provide a means of investigating the possible interaction between the CSRS and CARS processes in driving the rotational levels.

Snow, J. B.↗

Detection of atomic oxygen and its electronic coherence decays using time-resolved ultrafast coherent Raman scattering

We report the detection of atomic oxygen and quantitative measurements of its electronic Raman coherence decays in flames and low-temperature plasmas using time-resolved hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (CARS). Atomic oxygen was detected using the Raman transitions between the spin–orbit coupled triplet ground states. Atomic oxygen was generated in an H 2 /O 2 /Ar diffusion flame and an O 2 /Ar pulsed plasma discharge. Single exponential decays were observed for the O( 3 P 2 )–O( 3 P 1 ) Raman transition at 158.3 cm −1 and the O( 3 P 2 )–O( 3 P 0 ) Raman transition at 227 cm −1 . From the decay measurements, the atomic O Raman linewidths were obtained from 25 to 150 Torr in non-equilibrium plasma and at 760 Torr in a flame. Enhanced signal-to-noise ratios (SNRs) of atomic oxygen and atomic to molecular oxygen signal contrasts were obtained by taking advantage of electronic triplet coherence beating. Enhancement of up to seven times in the atomic O SNR was observed. Furthermore, we also found that the dephasing rates of O 2 (v = 0–3, N = 37) were similar, which provides evidence for the assumption that vibrational excitation does not influence the dephasing of diatomic molecular rotational CARS transitions.

Atomic and molecular spectroscopy↗

High-throughput single-cell sorting by stimulated Raman-activated cell ejection

Raman-activated cell sorting isolates single cells in a nondestructive and label-free manner, but its throughput is limited by small spontaneous Raman scattering cross section. Coherent Raman scattering integrated with microfluidics enables high-throughput cell analysis, but faces challenges with small cells (<3 μm) and tissue sections. Here, we report stimulated Raman-activated cell ejection (S-RACE) that enables high-throughput single-cell sorting by integrating stimulated Raman imaging, in situ image decomposition, and laser-induced cell ejection. S-RACE allows ejection of live bacteria or fungi guided by their Raman signatures. Furthermore, S-RACE successfully sorted lipid-richRhodotorula glutiniscells from a cell mixture with a throughput of ~13 cells per second, and the sorting results were confirmed by downstream quantitative polymerase chain reaction. Beyond single cells, S-RACE shows high compatibility with tissue sections. Incorporating a closed-loop feedback control circuit further enables real-time SRS imaging-identification-ejection. In summary, S-RACE opens exciting opportunities for diverse single-cell sorting applications.

Science & Technology - Other Topics↗

Temperature Measurements in Hypersonic Wind Tunnels via Femtosecond Coherent Anti-Stokes Raman Scattering

A femtosecond coherent anti-Stokes Raman scattering (fs CARS) instrument is developed to perform gas-phase thermometry in cold-flow hypersonic wind tunnels. Measurements are reported for Mach 8 and 14 pure-nitrogen flows. The fs CARS instrument includes a 100 fs pump/Stokes pulse and a spectrally narrow probe pulse from a second harmonic bandwidth compressor. Important experimental considerations such as limits on the pump/Stokes pulse energy are discussed. The fs CARS focusing and collimating optics are mounted on a two-axis translation stage system to scan the measurement location during a 30 second wind tunnel run. Single-laser-shot rotational CARS spectra are recorded at the laser repetition rate of 1 kHz in the wind tunnel freestream and near simple cone models. Spectral fitting is used to determine quantitative gas temperatures. Freestream temperatures at Mach 8 and 14 spanned ranges of 40–75 and 35–50 K, respectively, depending on tunnel operating conditions. Temperature variations across the central 100 mm span of the wind tunnel were quantified. Measured temperature jumps across conical bow shocks from various models varied by less than 1% from predicted values. Hypersonic boundary layer measurements were demonstrated. In conclusion, these measurements illustrate the utility and robustness of this instrument for the study of complex fluid flow phenomena in challenging ground test facilities.

Aerodynamics↗

High-energy, low-jitter, narrowband ps probe laser for kHz-rate fs/ps coherent anti-Stokes Raman scattering

Hybrid fs/ps coherent anti-Stokes Raman scattering (CARS) thermometry often utilizes ps probe pulses derived from pulse shaping or spectrally filtering the primary laser source or by synchronization with a low repetition rate external laser. This results in limited energy, spectral resolution, and/or repetition rate of the ps probe. In this work, a master-oscillator power-amplifier (MOPA) laser was synchronized to the oscillator of a Ti:sapphire regenerative amplifier to achieve high-energy (600 µJ), narrowband (58 ps) probe pulses at kHz repetition rates. Furthermore, temporal filtering allows the pulse characteristics to be adjusted for each application. At 25 Torr, relevant to high-speed flows, the kHz-rate MOPA system generated signal-to-noise ratios 3× higher in nitrogen and had improved precision relative to a 10 ps probe derived from spectral filtering and the power-amplifier. The MOPA system also enabled single-shot ro-vibrational hybrid fs/ps CARS thermometry in 650 K heated air.

47 OTHER INSTRUMENTATION↗

The effects of focusing on the efficiency of coherent anti-Stokes Raman scattering

The efficiency of coherent anti-Stokes Raman scattering (CARS) is calculated as a function of the input beam sizes of the Stokes and pump laser beams. A Green's function formalism is used to show that maximum efficiency occurs when the confocal parameters of the two input beams are unequal and when the phase mismatch between the anti-Stokes field and the nonlinear polarization is nonzero.

Guha, S.↗

Molecular-Based Optical Measurement Techniques for Transition and Turbulence in High-Speed Flow

High-speed laminar-to-turbulent transition and turbulence affect the control of flight vehicles, the heat transfer rate to a flight vehicle's surface, the material selected to protect such vehicles from high heating loads, the ultimate weight of a flight vehicle due to the presence of thermal protection systems, the efficiency of fuel-air mixing processes in high-speed combustion applications, etc. Gaining a fundamental understanding of the physical mechanisms involved in the transition process will lead to the development of predictive capabilities that can identify transition location and its impact on parameters like surface heating. Currently, there is no general theory that can completely describe the transition-to-turbulence process. However, transition research has led to the identification of the predominant pathways by which this process occurs. For a truly physics-based model of transition to be developed, the individual stages in the paths leading to the onset of fully turbulent flow must be well understood. This requires that each pathway be computationally modeled and experimentally characterized and validated. This may also lead to the discovery of new physical pathways. This document is intended to describe molecular based measurement techniques that have been developed, addressing the needs of the high-speed transition-to-turbulence and high-speed turbulence research fields. In particular, we focus on techniques that have either been used to study high speed transition and turbulence or techniques that show promise for studying these flows. This review is not exhaustive. In addition to the probe-based techniques described in the previous paragraph, several other classes of measurement techniques that are, or could be, used to study high speed transition and turbulence are excluded from this manuscript. For example, surface measurement techniques such as pressure and temperature paint, phosphor thermography, skin friction measurements and photogrammetry (for model attitude and deformation measurement) are excluded to limit the scope of this report. Other physical probes such as heat flux gauges, total temperature probes are also excluded. We further exclude measurement techniques that require particle seeding though particle based methods may still be useful in many high speed flow applications. This manuscript details some of the more widely used molecular-based measurement techniques for studying transition and turbulence: laser-induced fluorescence (LIF), Rayleigh and Raman Scattering and coherent anti-Stokes Raman scattering (CARS). These techniques are emphasized, in part, because of the prior experience of the authors. Additional molecular based techniques are described, albeit in less detail. Where possible, an effort is made to compare the relative advantages and disadvantages of the various measurement techniques, although these comparisons can be subjective views of the authors. Finally, the manuscript concludes by evaluating the different measurement techniques in view of the precision requirements described in this chapter. Additional requirements and considerations are discussed to assist with choosing an optical measurement technique for a given application.

Bathel, Brett F.↗

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy for rapid, label-free biological imaging

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy is a label-free imaging approach that provides detailed chemical information at high spatial resolution in a sample through nonlinear, coherent excitation of molecular vibrations and detection of Raman spectra. While its utility for biological imaging has been demonstrated, many aspects of this technique must mature before it can be widely adopted. One of the areas of required improvement is imaging speed—most BCARS implementations involve sample rastering, which limits imaging speed. Beam scanning can provide faster BCARS imaging but presents some unique challenges. Here, we describe a beam-scanning BCARS microscopy system that improves spatial resolution twofold and imaging speed by fivefold over a previous beam-scanning implementation. These enhancements were enabled by an improvement in supercontinuum power and the use of a sCMOS camera for its high data transfer rate and low read noise. Implementation of the sCMOS camera required correction for the significant pixel-to-pixel background and photon response nonuniformity. Here, we report on the method that we implemented for calibrating and correcting the pixel-to-pixel differences in sCMOS camera noise.

Dixon, Jessica Z. [Georgia Institute of Technology↗

Evaluation of turbulence induced noise in coherent anti-Stokes Raman scattering

The effect of turbulence in a transonic wind tunnel on coherent anti-Stokes Raman scattering is considered. The driving pump and Stokes waves are taken to be coaxially propagating Gaussian beam waves which are focused on the Raman active medium through the turbulent boundary layer of the flow tube. The random index of refraction variations in the layer are modeled as phase perturbations of the driving waves which cause a reduction of the mean on-axis field and an increase in the mean diameter of the beams. Effective Gaussian beam parameters are developed and the radiated anti-Stokes power calculated as a function of the phase screen parameters. A significant reduction in signal strength occurs for realistic estimates of the phase screen parameter appropriate to a confined transonic flow. A method for estimating the signal degradation which could be applied to other experimental situations is presented.

Elliott, R. A.↗

Spatially and spectrally resolved multipoint coherent anti-Stokes Raman scattering from N2 and O2 flows

Single-shot spectrally resolved broadband rotational coherent anti-Stokes Raman scattering (CARS) from multiple points along a line intersecting a flow has been observed for N2 and O2. A large-angle phase-matching configuration was used to achieve spatial resolution of 0.1 mm x 0.1 mm x 0.1 mm for each of 20 points in the interaction volume. Single-shot multipoint CARS of N2 at different temperatures and of several species in a coflowing jet was observed.

Snow, J. B.↗

Dual-Pump Coherent Anti-Stokes Raman Scattering Temperature and CO2 Concentration Measurements

Measurements of temperature and CO2 concentration using dual-pump coherent anti-Stokes Raman scattering, (CARS) are described. The measurements were performed in laboratory flames,in a room-temperature gas cell, and on an engine test stand at the U.S. Air Force Research Laboratory, Wright-Patterson Air Force Base. A modeless dye laser, a single-mode Nd:YAG laser, and an unintensified back-illuminated charge-coupled device digital camera were used for these measurements. The CARS measurements were performed on a single-laser-shot basis. The standard deviations of the temperatures and CO2 mole fractions determined from single-shot dual-pump CARS spectra in steady laminar propane/air flames were approximately 2 and 10% of the mean values of approximately 2000 K and 0.10, respectively. The precision and accuracy of single-shot temperature measurements obtained from the nitrogen part of the dual-pump CARS system were investigated in detail in near-adiabatic hydrogen/air/CO2 flames. The precision of the CARS temperature measurements was found to be comparable to the best results reported in the literature for conventional two-laser, single-pump CARS. The application of dual-pump CARS for single-shot measurements in a swirl-stabilized combustor fueled with JP-8 was also demonstrated.

Lucht, Robert P.↗

Coherent anti-Stokes Raman scattering with squeezed light: CARS for quantum-enhanced spectroscopy and imaging

We theoretically investigate quantum-enhanced coherent anti-Stokes Raman scattering (CARS) using squeezed light to amplify vibrational transition rates at low photon flux. Quantum sensing approaches are needed for nondestructive nanometrology such as in bioimaging where reduced photodamage is desired while retaining resolution and sensitivity. We analyze both single-mode squeezing applied to the pump field and two-mode squeezing between the pump and Stokes fields. We also show that the ordering of displacement and squeezing operations—whether displacement precedes squeezing or squeezing precedes displacement—has an impact on the resulting CARS transition amplitudes due to a difference in the photon number and the quantum-enhancement coefficients, with the latter offering a stronger enhancement in the case of two modes squeezing of the pump and Stokes under experimentally accessible conditions. Furthermore, our calculations capture these quantum enhancements through the intrinsic photon-number correlations of squeezed light, eliminating the need for interferometric detection or higher pump powers that are otherwise required to reach comparable sensitivities in classical CARS. Finally, we outline a quantum plasmonic extension of our model in which local field enhancements caused by surface plasmon excitation in metallic nanoparticles can be incorporated via mode-selective field amplification factors, offering a pathway toward combining squeezed-light quantum optics with surface-enhanced nanoscale spectroscopy and imaging.

Atomic & molecular structure↗

Three-beam hybrid fs/ps coherent anti-Stokes Raman scattering of rotation–vibration non-equilibrium

In this work, we demonstrate time-resolved rotational and vibrational temperature measurements to probe plasma non-equilibrium through a simple three-beam hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) system. A single pump/Stokes pair is employed to generate both the pure-rotational and ro-vibrational Raman coherence. A novel phase-matching scheme, to our knowledge, is employed to spatially overlap the two CARS signals, simplifying the optical design and allowing signal selection by tuning a single spectrometer grating. Measurements were performed near the electrodes in a N 2 DC glow discharge. Both the rotational temperature and the vibrational populations up to $v$ = 8 were calculated from the separately measured single-shot pure-rotational and ro-vibrational CARS spectra. Strong rotation–vibration non-equilibrium was observed at both electrodes, with the cathode showing higher vibrational and rotational temperatures. In addition, non-Boltzmann behaviors were observed at both electrodes. This simplified approach enables measurements of rotational and vibrational temperatures with high spatial resolution in non-equilibrium flows.

42 ENGINEERING↗

Coherent Anti-Stokes Raman Scattering (CARS) as a Probe for Supersonic Hydrogen-Fuel/Air Mixing

The dual-pump coherent anti-Stokes Raman spectroscopy (CARS) method was used to measure temperature and the absolute mole fractions of N2, O2 and H2 in a supersonic non-reacting fuel-air mixing experiment. Experiments were conducted in NASA Langley Research Center s Direct Connect Supersonic Combustion Test Facility. Under normal operation of this facility, hydrogen and air burn to increase the enthalpy of the test gas and O2 is added to simulate air. This gas is expanded through a Mach 2 nozzle and into a combustor model where fuel is then injected, mixes and burns. In the present experiment the O2 of the test gas is replaced by N2. The lack of oxidizer inhibited combustion of the injected H2 fuel jet allowing the fuel/air mixing process to be studied. CARS measurements were performed 427 mm downstream of the nozzle exit and 260 mm downstream of the fuel injector. Maps were obtained of the mean temperature, as well as the N2, O2 and H2 mean mole fraction fields. A map of mean H2O vapor mole fraction was also inferred from these measurements. Correlations between different measured parameters and their fluctuations are presented. The CARS measurements are compared with a preliminary computational prediction of the flow.

Danehy, P. M.↗

Dual-pump Coherent anti-Stokes Raman scattering measurements in H 2 /CH 4 Counterflow Flames

Temperature and major species concentration measurements are reported in a Williams Seshadri counterflow burner using dual-pump coherent anti-Stokes Raman scattering (DPCARS). Hencken burner H2/Air flames with equivalence ratio of 0.8-1.4 were used to characterize the accuracy of the system. The mean errors for temperature, XH2/XN2 mole fraction ratio, and XO2/XN2 mole fraction ratio are 1.0%, 14.7%, and 5.5%, respectively. The counterflow burner uses a CH4, H2, and N2 mixture as fuel and synthetic air as oxidizer. Measurements were performed along the counterflow burner central axis for two different fuel compositions: 4% H2/86% CH4/10% N2 and 87%H2/3% CH4/10% N2. The measured temperature and species mole fractions agree well with the 1-D opposed-flow diffusion flame simulation. One observation is that the fuel inlet temperature is higher than 300 K, which suggests the possibility of the stagnation plane residing closer to the fuel side. Lastly, these measurements provide valuable data for testing and validation of advanced 2-D flame models.

Murdock, Benjamin K.↗

Nitrogen thermometry in an inductively coupled plasma torch using broadband nanosecond coherent anti-Stokes Raman scattering

The development of atmospheric hypersonic flight and re-entry capabilities requires the characterization of the thermo-chemical state of representative test environments. This study demonstrates the usage of multiplex nanosecond N 2 coherent anti-Stokes Raman scattering (CARS) to measure temperatures in an atmospheric, high-temperature (>6000K), air plasma plume, generated by an inductively coupled plasma torch. These are some of the highest temperatures ever accessed via gas-phase CARS, to our knowledge. Temperatures of N 2 in the equilibrium plasma plume are determined via theoretical fits to measured CARS spectra. We discuss the practical implementation of CARS at very high temperatures, including the scaling of the N 2 CARS signal strength from 300 to 6700 K, where the expected peak signal from the high-temperature plasma torch gases is two orders of magnitude less than commonly encountered in combustion environments. An intensified CCD camera enables single-laser-shot detection at temperatures as high as 6200 K, by increasing sensitivity and providing a time gate against intense background luminosity. We also discuss the impacts of unwanted two-beam CARS contributions from outside the nominal three-beam measurement volume. We present mean axial and radial temperature profiles, as well as time-series data derived from both single-laser-shot and accumulated CARS spectra. The single-laser-shot precision is 1.7%–2.6% at temperatures of 3500 to 6200 K. The presented results pave the way for the use of CARS at very high temperatures and the measurement of spatially resolved interface processes in high-enthalpy flows.

Fries, Dan (ORCID:0000000229513294)↗

Plasma-assisted deflagration to detonation transition in a microchannel with fast-frame imaging and hybrid fs/ps coherent anti-Stokes Raman scattering measurements

Our study examines kinetic enhancement by nanosecond dielectric barrier discharge (ns-DBD) plasma on fuellean dimethyl ether (DME), oxygen (O 2 ), and argon (Ar) premixtures during deflagration to detonation transition (DDT) experiments in a microchannel. Non-equilibrium plasma produces active species and radicals and creates fast and slow heating of a mixture to promote ignition due to electronic and vibrational excitation. Experiments have been conducted to examine the influence of the plasma discharge on the premixture and on the resultant deflagration to detonation transition (DDT) onset time and distance through the use of high speed imaging and one-dimensional, two-beam, femtosecond/picosecond, coherent anti-Stokes Raman scattering (CARS). A highspeed camera is used to trace the time histories of flame front position and velocity and to identify the dynamics and onset of DDT. The results show that plasma discharge can nonlinearly affect the onset time and distance of DDT. It is shown that a small number of plasma discharge pulses prior to ignition result in reduced DDT onset time and distance by 60% and 40%, respectively, when compared to the results without pre-excitation by ns discharges. The results also show that an increase of plasma discharge pulses results in an extended DDT onset time and distance of 224% and 94%, respectively. Time history of the deflagration wave speed of DME and the analysis of ignition timescale under the choking condition of the deflagration front suggest low temperature ignition may play a role for DME near the isobaric choking condition of the burned gas and the DDT. Plasmainduced conversion of the reactive mixture was assessed via the O 2 to CO 2 ratio as measured through fs/ps CARS during the DBD discharges. The present experiments demonstrate the ability of non-equilibrium plasma to alter the chemistry of DME/O 2 /Ar premixtures in order to control DDT for applications in advanced propulsion engines.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗