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DOE OSTI2020

Three-beam rotational coherent anti-Stokes Raman spectroscopy thermometry in scattering environments

Three-beam rotational coherent anti-Stokes Raman scattering (CARS) measurements performed in highly scattering environments are susceptible to contamination by two-beam CARS signals generated by the pump–probe and Stokes–probe interactions at the measurement volume. If this occurs, differences in the Raman excitation bandwidth between the two-beam and three-beam CARS signals can add significant errors to the spectral analysis. This interference to the best of our knowledge has not been acknowledged in previous three-beam rotational CARS experiments, but may introduce measurement errors up to 25% depending on the temperature, amount of scattering, and differences between the two-beam and three-beam Raman excitation bandwidths. Here, the presence of two-beam CARS signal contamination was experimentally verified using a femtosecond–picosecond rotational CARS instrument in two scattering environments: (1) a fireball generated by a laboratory-scale explosion that contained particulate matter, metal fragments, and soot, and (2) a flow of air and small liquid droplets. A polarization scheme is presented to overcome this interference. By rotating the pump and Stokes polarizations +55° and –55° from the probe, respectively, the two-beam and three-beam CARS signals are orthogonally polarized and can be separated using a polarization analyzer. Using this polarization arrangement, the Raman-resonant three-beam CARS signal amplitude is reduced by a factor of 2.3 compared to the case where all polarizations are parallel. This method is successfully demonstrated in both scattering environments. A theoretical model is presented, and the temperature measurement error is studied for different experimental conditions. The criteria for when this interference may be present are discussed.

42 ENGINEERING↗

DOE OSTI2022

Hybrid time–frequency domain dual-probe coherent anti-Stokes Raman scattering for simultaneous temperature and pressure measurements in compressible flows via spectral fitting

We demonstrate a hybrid time–frequency spectroscopic method for simultaneous temperature/pressure measurements in nonreacting compressible flows with known gas composition. Hybrid femtosecond–picosecond, pure-rotational coherent anti-Stokes Raman scattering (CARS), with two independent, time-delayed probe pulses, is deployed for single-laser-shot measurements of temperature and pressure profiles along an ∼ <#comment/> 5 -mm line. The theory of dual-probe CARS is presented, along with a discussion of the iterative fitting of experimental spectra. Temperature is obtained from spectra acquired with an early, near-collision-free probe time delay ( τ <#comment/> 1 = 0 p s ) and pressure from spectra obtained at probe delays of τ <#comment/> 2 = 150 − <#comment/> 1000 p s , where collisions significantly impact the spectral profile. Unique solutions for temperature and pressure are obtained by iteratively fitting the two spectra to account for small collisional effects observed for the near zero probe delay spectrum. A dual-probe pure-rotational CARS system, in a 1D line-imaging configuration, is developed to demonstrate effectively the simultaneous temperature and pressure profiles recorded along the axial centerline of a highly underexpanded jet. The underexpanded air jet permits evaluation of this hybrid time–frequency domain approach for temperature and pressure measurements across a wide range of low-temperature–low-pressure conditions of interest in supersonic ground-test facilities. Single-laser-shot measurement precisions in both quantities and pressure measurement accuracy are systematically evaluated in the quiet zone upstream of the Mach disk. Precise thermometry approaching 1%−2% is observed in regions of high CARS signal-to-noise ratios. Pressure measurements are optimized at probe time delays where the ratio of the late probe delay to the Raman lifetime exceeds four ( τ <#comment/> 2 / τ <#comment/> R > <#comment/> 4 ). The impact of low-temperature Raman linewidths on CARS pressure measurements is evaluated, and comparisons of CARS pressures obtained with our recent low-temperature pure-rotational Raman linewidth data and extrapolated high-temperature Q -branch linewidths are presented. Considering all measurements with τ <#comment/> 2 / τ <#comment/> R ≥ <#comment/> 4.0 , measured pressures were on average 7.9% of the computed isentropic values with average shot-to-shot deviations representing a combination of instrument noise and fluid fluctuations of 5.0%.

Retter, Jonathan E.↗

DOE OSTI2023

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)↗

DOE OSTI2024

Coherent homodyne detection for amplified cross-beam electric-field induced second harmonic

The electric-field induced second harmonic (E-FISH) signal sensing is commonly used as a nonlinear optical technique to probe electric fields inside a plasma region. Cross-beam E-FISH is being investigated to improve spatial resolution by defining the interaction volume via a controlled geometry of two overlapping noncolinear optical beams. This drastic reduction in interaction length of the electric field and laser region results in a significant signal reduction. Here, to overcome this signal reduction, we introduce coherent amplification of the cross-beam E-FISH signal by mixing the low E-FISH signal with a phase-locked bright local oscillator. We demonstrate enhancement of the signal. By introducing a local oscillator we can now derive the polarity of the measured electric field through the phase of the homodyne signal. To illustrate the technique, we, for the first time, to the best of our knowledge, measure the magnitude and the direction of the electric field in a cold atmospheric pressure plasma jet, which dynamically follows the profile of the applied bias current.

42 ENGINEERING↗

DOE OSTI2021

Deep-learning-aided forward optical coherence tomography endoscope for percutaneous nephrostomy guidance

Percutaneous renal access is the critical initial step in many medical settings. In order to obtain the best surgical outcome with minimum patient morbidity, an improved method for access to the renal calyx is needed. In our study, we built a forward-view optical coherence tomography (OCT) endoscopic system for percutaneous nephrostomy (PCN) guidance. Porcine kidneys were imaged in our experiment to demonstrate the feasibility of the imaging system. Three tissue types of porcine kidneys (renal cortex, medulla, and calyx) can be clearly distinguished due to the morphological and tissue differences from the OCT endoscopic images. To further improve the guidance efficacy and reduce the learning burden of the clinical doctors, a deep-learning-based computer aided diagnosis platform was developed to automatically classify the OCT images by the renal tissue types. Convolutional neural networks (CNN) were developed with labeled OCT images based on the ResNet34, MobileNetv2 and ResNet50 architectures. Nested cross-validation and testing was used to benchmark the classification performance with uncertainty quantification over 10 kidneys, which demonstrated robust performance over substantial biological variability among kidneys. ResNet50-based CNN models achieved an average classification accuracy of 82.6%±3.0%. The classification precisions were 79%±4% for cortex, 85%±6% for medulla, and 91%±5% for calyx and the classification recalls were 68%±11% for cortex, 91%±4% for medulla, and 89%±3% for calyx. Interpretation of the CNN predictions showed the discriminative characteristics in the OCT images of the three renal tissue types. The results validated the technical feasibility of using this novel imaging platform to automatically recognize the images of renal tissue structures ahead of the PCN needle in PCN surgery.

Wang, Chen↗

DOE OSTI2023

Three-dimensional imaging using coherent x rays at grazing incidence geometry

We have developed a three-dimensional coherent diffraction imaging algorithm to retrieve phases of diffraction patterns of samples in grazing incidence small angle x-ray scattering experiments. The algorithm interprets the diffraction patterns using the distorted-wave Born approximation instead of the Born approximation, as in this case, the existence of a reflected beam from the substrate causes the diffraction pattern to deviate significantly from the simple Fourier transform of the object. Detailed computer simulations show that the algorithm works. Verification with real experiments is planned.

Yang, Yi↗

DOE OSTI2020

Optimizing hybrid rotational femtosecond/picosecond coherent anti-Stokes Raman spectroscopy in nitrogen at high pressures and temperatures

We demonstrate the use of hybrid rotational femtosecond/picosecond (fs/ps) coherent anti-Stokes Raman spectroscopy (HR-CARS) as a technique for temperature measurements in nitrogen gas at high pressures and temperatures. A broadband pulse shaper-adjusted 42 fs pulse interacts with a narrow-bandwidth, frequency-upconverted 5.5 ps pulse in a cell containing N 2 at pressures of 1–70 atm and temperatures of 300–1000 K. A computational code is used to model spectra and fit experimental results to obtain best-fit temperatures. We demonstrate good qualitative fits as well as good accuracy and precision between thermocouple measured and best-fit temperatures over the explored pressure and temperature regimes. The overall average percentage temperature difference between thermocouple measurements and best-fit temperatures is − <#comment/> 0 . 3 % <#comment/> with a standard deviation of 7.1%, showing the suitability of HR-CARS for characterizing high-pressure and -temperature environments.

Torge Mecker, Nils (ORCID:0000000238977170)↗

DOE OSTI2020

Machine learning enabled lineshape analysis in optical two-dimensional coherent spectroscopy

Optical two-dimensional (2D) coherent spectroscopy excels in studying coupling and dynamics in complex systems. The dynamical information can be learned from lineshape analysis to extract the corresponding linewidth. However, it is usually challenging to fit a 2D spectrum, especially when the homogeneous and inhomogeneous linewidths are comparable. We implemented a machine learning algorithm to analyze 2D spectra to retrieve homogeneous and inhomogeneous linewidths. The algorithm was trained using simulated 2D spectra with known linewidth values. The trained algorithm can analyze both simulated (not used in training) and experimental spectra to extract the homogeneous and inhomogeneous linewidths. Finally, this approach can be potentially applied to 2D spectra with more sophisticated spectral features.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

X-ray computed tomography using partially coherent Fresnel diffraction with application to an optical fiber

A reconstruction algorithm for partially coherent x-ray computed tomography (XCT) including Fresnel diffraction is developed and applied to an optical fiber. The algorithm is applicable to a high-resolution tube-based laboratory-scale x-ray tomography instrument. The computing time is only a few times longer than the projective counterpart. The algorithm is used to reconstruct, with projections and diffraction, a tilt series acquired at the micrometer scale of a graded-index optical fiber using maximum likelihood and a Bayesian method based on the work of Bouman and Sauer. The inclusion of Fresnel diffraction removes some reconstruction artifacts and use of a Bayesian prior probability distribution removes others, resulting in a substantially more accurate reconstruction.

Levine, Zachary H. (ORCID:000000029928276X)↗

DOE OSTI2021

Stabilization of the 81-channel coherent beam combination using machine learning

We develop a rapidly converging algorithm for stabilizing a large channel-count diffractive optical coherent beam combination. An 81-beam combiner is controlled by a novel, machine-learning based, iterative method to correct the optical phases, operating on an experimentally calibrated numerical model. A neural-network is trained to detect phase errors based on interference pattern recognition of uncombined beams adjacent to the combined one. Due to the non-uniqueness of solutions in the full space of possible phases, the network is trained within a limited phase perturbation/error range. This also reduces the number of samples needed for training. Simulations have proven that the network can converge in one step for small phase perturbations. When the trained neural-network is applied to a realistic case of 360 degree full range, an iterative scheme exploits random walking at the beginning, with the accuracy of prediction on phase feedback direction, to allow the neural-network to step into the training range for fast convergence. This neural-network-based iterative method of phase detection works tens of times faster than the commonly used stochastic parallel gradient descent approach (SPGD) using a single-detector and random dither when both are tested with random phase perturbations.

Wang, Dan↗

DOE OSTI2021

Generation of structured coherent extreme ultraviolet beams from an MgO crystal

Short wavelength high-harmonic sources are undergoing intense development for applications in spectroscopy and microscopy. Despite recent progress in peak and average power, spatial control over coherent extreme ultraviolet (XUV) beams remains a formidable challenge due to the lack of suitable optical elements for beam shaping and control. In this work, we demonstrate a robust and precise approach that structures XUV high-order harmonics in space as they are emitted from a nanostructured MgO crystal. Our demonstration paves the way for bridging the numerous applications of shaped light beams from the visible to the short wavelengths, with potential uses for applications in microscopy and nanoscale machining.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Hyperspectral acquisition with ScanImage at the single pixel level: application to time domain coherent Raman imaging

We present a comprehensive strategy and its practical implementation using the commercial ScanImage software platform to perform hyperspectral point scanning microscopy when a fast time-dependent signal varies at each pixel level. In the proposed acquisition scheme, the scan along the X-axis is slowed down while the data acquisition is maintained at a high pace to enable the rapid acquisition of the time-dependent signal at each pixel level. The ScanImage generated raw 2D images have a very asymmetric aspect ratio between X and Y, the X axis encoding both for space and time acquisition. The results are X-axis macro-pixel where the associated time-dependent signal is sampled to provide hyperspectral information. We exemplified the proposed hyperspectral scheme in the context of time-domain coherent Raman imaging, where a pump pulse impulsively excites molecular vibrations that are subsequently probed by a time-delayed probe pulse. In this case, the time-dependent signal is a fast acousto-optics delay line that can scan a delay of 4.5ps in 25 μ s at each pixel level. With this acquisition scheme, we demonstrate ultra-fast hyperspectral vibrational imaging in the low frequency range [10 cm −1 , 150 cm −1 ] over a 500 μm field of view (64 x 64 pixels) in 130ms (∼ 7.5 frames/s). The proposed acquisition scheme can be readily extended to other applications requiring the acquisition of a fast-evolving signal at each pixel level.

Metais, Samuel↗

DOE OSTI2020

Total internal reflection enabled wide-field coherent anti-Stokes Raman scattering microscopy

Wide-field coherent anti-Stokes Raman scattering (CARS) microscopy offers an attractive means for the rapid and simultaneous acquisition of vibrationally resolved images across a large field of view. A major challenge in the implementation lies in how to achieve sufficiently strong excitation fields necessary to drive the third-order optical responses over the large focal region. Here, we report a new wide-field CARS microscope enabled by a total internal reflection excitation scheme using a femtosecond Ti:Sapphire oscillator to generate pump and broadband near-infrared Stokes pulses. The spectrally broad Stokes pulse, in combination with its inherent chirp, offers not only access to a wide range of Raman modes spanning ∼ <#comment/> 1000 to ∼ <#comment/> 3500 c m − <#comment/> 1 but also a straightforward means to select vibrational transitions within this range by simply varying the time delay between the pulses. The unique capabilities of this wide-field CARS microscope were validated by acquiring high-quality CARS images from the model and complex biological samples on conventional microscope coverslips.

Doughty, Benjamin (ORCID:0000000164299329)↗

DOE OSTI2020

1-D imaging of rotation-vibration non-equilibrium from pure rotational ultrafast coherent anti-Stokes Raman scattering

We present one-dimensional (1-D) imaging of rotation-vibration non-equilibrium measured by two-beam pure rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Simultaneous measurements of the spatial distribution of molecular rotation-vibration non-equilibrium are critical for understanding molecular energy transfer in low temperature plasmas and hypersonic flows. However, non-equilibrium CARS thermometry until now was limited to point measurements. The red shift of rotational energy levels by vibrational excitation was used to determine the rotational and vibrational temperatures from 1-D images of the pure rotational spectrum. Vibrational temperatures up to 5500 K were detected in a CH4/N2 nanosecond-pulsed pin-to-pin plasma within 2 mm near the cathode. As a result, this approach enables study of non-equilibrium systems with 40 µm spatial resolution.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Total internal reflection enabled wide-field coherent anti-Stokes Raman scattering microscopy

Wide-field coherent anti-Stokes Raman scattering (CARS) microscopy offers an attractive means for the rapid and simultaneous acquisition of vibrationally resolved images across a large field of view. A major challenge in the implementation lies in how to achieve sufficiently strong excitation fields necessary to drive the third-order optical responses over the large focal region. Here, we report a new wide-field CARS microscope enabled by a total internal reflection excitation scheme using a femtosecond Ti:Sapphire oscillator to generate pump and broadband near-infrared Stokes pulses. The spectrally broad Stokes pulse, in combination with its inherent chirp, offers not only access to a wide range of Raman modes spanning ${\sim}{1000}$ to ${\sim}{3500}\;{{\rm cm}^{- 1}}$ but also a straightforward means to select vibrational transitions within this range by simply varying the time delay between the pulses. The unique capabilities of this wide-field CARS microscope were validated by acquiring high-quality CARS images from the model and complex biological samples on conventional microscope coverslips.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Suppression of coherent interference to electric-field-induced second-harmonic (E-FISH) signals for the measurement of electric field in mesoscale confined geometries

We present spatially enhanced electric-field-induced second-harmonic (SEEFISH) generation with a chirped femtosecond beam for measurements of electric field in mesoscale confined geometries subject to destructive spurious second-harmonic generation (SHG). Spurious SHG is shown to interfere with the measured E-FISH signal coherently, and thus simple background subtraction is not sufficient for single-beam E-FISH approaches, especially in a confined system with a large surface-to-volume ratio. The results show that a chirped femtosecond beam is effective in preventing higher-order mixing and white light generation in windows near the beam focal point which further contaminates the SEEFISH signal. The successful measurements of electric field of a nanosecond dielectric barrier discharge in a test cell demonstrated that spurious SHG detected with a congruent traditional E-FISH approach can be eliminated using the SEEFISH approach.

Vorenkamp, Madeline↗

DOE OSTI2024

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↗

DOE OSTI2025

Localization and coherent imaging of hidden moving objects using laser speckle

Imaging and sensing of moving objects through opaque scattering media is a challenging but important problem in a variety of applications, including environmental sensing, biomedical imaging, and material inspection. We have previously demonstrated a technique to coherently image a moving object through thick, heavily scattering random media using correlations of speckle images as a function of the object’s spatial translation. Here, we demonstrate that this technique can be combined with localization to achieve imaging without prior knowledge of the object’s motion, greatly extending the application domain. This method is effective beyond the thin or weakly scattering regime and, rather than motion being deleterious, exploits the information available when the hidden object is moving, as could be the case in a cluttered terrestrial environment or through substantial levels of biological tissue scatter.

Hastings, Ryan L. (ORCID:0009000095977807)↗