Some new aspects in stimulated raman scattering from hydrogen gas.
Stimulated Raman scattering from hydrogen gas, discussing simultaneous SRS of harmonic ruby radiation and vibrational rotational lines
Duardo, J. A.↗
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Squeezed Light Stimulated Raman Scattering (SRS) Microscopy for Bioenergy Applications
Stimulated Raman scattering (SRS) microscopy using picosecond near-IR pulses have provided a great penetration depth with reduced fluorescence interference when imaging biological samples for bioenergy applications. These tools have provided insight into 1) tracking the degradation of chemical composites in biomass feedstocks to investigate the recalcitrant factors during the deconstruction processes, 2) monitoring the production of chemicals in photosynthetic plants and wood-digesting microorganisms, and 3) probing plant-bacteria interactions. However, the above processes are usually slow and require continuous imaging for an extended period. This is challenging for classic SRS because the laser power needed to achieve enough sensitivity causes photodamage in the samples during such long experiments. Quantum-squeezed light with reduced noise in the intensity quadrature can improve the sensitivity of classic SRS microscopy beyond the shot noise limit. The successful squeezing of one of the picosecond pulses in the above SRS will improve sensitivity and reduce photodamage, greatly expanding the range of studies available to SRS microscopy.
BIOMASS FUELS↗
Stimulated Raman Scattering Microscopy: Real-Time In-Situ Physical and Chemical Characterization of Reverse Osmosis Desalination Membrane Scaling
We introduce a stimulated Raman scattering (SRS) methodology designed for rapid, real-time, and in situ monitoring of RO membrane scaling adapted for bench-scale desalination flow cells. The methodology can provide new insights into membrane scaling dynamics by offering time-resolved reflection imaging of inorganic crystal growth, coupled with chemical identification from Raman spectral data. These capabilities allow for direct local measurement of the membrane surface area covered by different scalants as well as an approximation of the scalant volume using three-dimensional, integrated Raman intensity. The 2D and 3D SRS results obtained from CaSO 4 scaling experiments are compared to and are in reasonable agreement with those provided by confocal microscopy. The real-time physical and chemical characterization capabilities presented here could be extended to study combinations of inorganic, organic, and biological fouling. Overall, the SRS methodology represents an advancement in real-time sensing of membrane fouling that offers the potential for improved operation, lower cost, and more resilient RO membrane systems for sustainable water management.
42 ENGINEERING↗
Reassessment of the theory of stimulated Raman scattering
A modification of the standard theory of stimulated Raman scattering (SRS) first proposed by Sparks (1974, 1975) is analyzed and shown to incorporate a possibly important physical effect; however, its original formulation is incorrect. The analysis is based on an exact numerical integration of the coupled equations of the modified theory, the results of which are compared with both the conventional theory of SRS and with one set of experimental data. A reformulation of the modified theory is suggested that leads to a gain which is in somewhat better agreement with the data than is the conventional theory.
Fralick, G. C.↗
A study of transient stimulated Raman scattering and self-focusing in the picosecond time regime
Two third order processes, stimulated Raman scattering and self-focusing, with picosecond pulses are studied. In the case of transient stimulated scattering, the gain is reduced from the steady state value, and qualitatively new features, such as shortening and delay of the Stokes pulse relative to the laser pulse, appear. These predictions are extended to realistic laser pulses, and experiments confirm all of the theoretical predictions. The self-focusing and frequency broadening of picosecond pulses is studied in the absence of stimulated Raman scattering in several materials with large orientational Kerr constants. Measurements of the relaxation time indicate that the orientational Kerr effect is important in the self-focusing of picosecond pulses. Self-focused filaments are observed to propagate with constant diameters over a distance greater than 10 cm, but disappear before the end of a 20 cm cell. The filaments radiate light continuously along their path and the spectrum of the light shows that the frequency content extends symmetrically for several hundred wave numbers on either side of the laser frequency.
Reintjes, J. F.↗
Modeling of transverse stimulated Raman scattering in KDP/DKDP in large-aperture plates suitable for polarization control
Transverse stimulated Raman scattering (TSRS) in potassium dihydrogen phosphate (KDP) and deuterated potassium dihydrogen phosphate (DKDP) plates for large-aperture, inertial confinement fusion (ICF)-class laser systems is a well-recognized limitation giving rise to parasitic energy conversion and laser-induced damage. The onset of TSRS is manifested in plates exposed to the ultraviolet section of the beam. TSRS amplification is a coherent process that grows exponentially and is distributed nonuniformly in the crystal and at the crystal surfaces. To understand the growth and spatial distribution of TSRS energy in various configurations, a modeling approach has been developed to simulate the operational conditions relevant to ICF-class laser systems. Specific aspects explored in this work include (i) the behavior of TSRS in large-aperture crystal plates suitable for third-harmonic generation and use as wave plates for polarization control in current-generation ICF-class laser system configurations; (ii) methods, and their limitations, of TSRS suppression and (iii) optimal geometries to guide future designs.
47 OTHER INSTRUMENTATION↗
Stimulated Raman scattering in an infrared active, nontotally symmetric vibration of alpha-quartz.
Stimulated Raman scattering in IR active nontotally symmetric vibration of alpha quartz crystal, noting parametric oscillation
RAMAN SCATTERING↗
Stimulated Raman scattering and the extreme high-velocity H2O maser features in W49
Stimulated Raman scattering of the intense 22.2-GHz water-vapor maser radiation within W49 is examined as a possible explanation of the extremely broad spectrum of W49 extending to + or - 200 km/sec apparent Doppler velocity. Under the most favorable conditions, Raman scattering from ammonia molecules is calculated to be observable. It is unlikely that the Raman process contributes appreciably in the case of W49, as it fails to predict the observed spatial and spectral distribution of the radiation.
Boyd, R. W.↗
Experimental investigation of transient stimulated Raman scattering in a linearly dispersionless medium.
The results of numerical calculations of the transient stimulated Raman scattering reported previously have been verified experimentally under conditions where both linear dispersion and self-focusing effects were negligible. The existence of a delay between maxima of the laser and Stokes pulses is experimentally demonstrated for the first time, while the pulse shortening in time via Raman scattering is established more firmly than in previous work. The incident-laser-pulse duration, generated-Stokes-pulse duration, and delay between intensity maxima for the laser and Stokes pulses were measured with the two-photon absorption-fluorescence technique. The effective phonon-dephasing time is determined via spontaneous Raman scattering. By using these measured quantities, inferences are made as to the magnitude of the transient gain and the shape of the exciting picosecond laser pulse.
Carman, R. L.↗
Development and applications of tunable, narrow band lasers and stimulated Raman scattering devices for atmospheric lidar
The main thrust of the program was the study of stimulated Raman processes for application to atmospheric lidar measurements. This has involved the development of tunable lasers, the detailed study of stimulated Raman scattering, and the use of the Raman-shifted light for new measurements of molecular line strengths and line widths. The principal spectral region explored in this work was the visible and near-IR wavelengths between 500 nm and 1.5 microns. Recent alexandrite ring laser experiments are reported. The experiments involved diode injection-locking, Raman shifting, and frequency-doubling. The experiments succeeded in producing tunable light at 577 and 937 nm with line widths in the range 80-160 MHz.
Wilkerson, Thomas D.↗
Stimulated Raman scattering of light absorbing media excited by ultrashort laser pulses
The fluctuation-dissipation theory of spontaneous and stimulated vibration Raman scattering is worked out taking into account the dissipation losses at frequencies of laser pump and scattering radiation. General expressions are found, which describe the absolute intensities and shape, energy and duration of scattered pulses in terms of the parameters of the medium and the the input laser pulses. The general regularities are analyzed in detail. Conditions are found for the realization of spontaneous or stimulated Raman scattering and its dependence on absorption, pulse duration and other parameters of the problem.
Marchevskiy, F. N.↗
Longitudinal Single‐Cell Imaging of Engineered Strains with Stimulated Raman Scattering to Characterize Heterogeneity in Fatty Acid Production
Abstract Understanding metabolic heterogeneity is critical for optimizing microbial production of valuable chemicals, but requires tools that can quantify metabolites at the single‐cell level over time. Here, longitudinal hyperspectral stimulated Raman scattering (SRS) chemical imaging is developed to directly visualize free fatty acids in engineered Escherichia coli over many cell cycles. Compositional analysis is also developed to estimate the chain length and unsaturation of the fatty acids in living cells. This method reveals substantial heterogeneity in fatty acid production among and within colonies that emerges over the course of many generations. Interestingly, the strains display distinct types of production heterogeneity in an enzyme‐dependent manner. By pairing time‐lapse and SRS imaging, the relationship between growth and production at the single‐cell level are examined. The results demonstrate that cell‐to‐cell production heterogeneity is pervasive and provides a means to link single‐cell and population‐level production.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Erratum: “Nonlinear models for coupling the effects of stimulated Raman scattering to inertial confinement fusion codes” [Phys. Plasmas 30, 042714 (2023)]
This is a correction to: Nonlinear models for coupling the effects of stimulated Raman scattering to inertial confinement fusion codes
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Stimulated Raman scattering seeded by a fibre continuum
A broadband continuum generated in a germanosilicate optical fiber has been used as a coherent seed to initiate stimulated Raman scattering in gases. The technique used is described. The results show a fivefold increase in conversion efficiency and a similar reduction in the requisite pump power.
Selker, M. D.↗
Observations of stimulated Raman scattering and laser-induced breakdown in millimeter-sized droplets
We report the first observations, to our knowledge, of nonlinear optical effects in large (millimeter-sized) droplets. Stimulated Raman scattering (SRS) and laser-induced breakdown (LIB) are simultaneously observed in acoustically levitated millimeter-sized glycerol droplets irradiated by either a frequency-doubled (532-nm) or a frequency-tripled (355-nm) Nd:YAG laser. The two processes, which occur above a nearby coincident irradiation threshold, are conjectured to arise from a common initiation mechanism: self-focusing. LIB generates vapor bubbles within the droplet, resulting in the quenching of SRS emission.
Biswas, A.↗
Label-free nanoscopy of cell metabolism by ultrasensitive reweighted visible stimulated Raman scattering
Nanoscopic imaging of cell metabolism is hindered by the incompatibility of small metabolites with fluorescent dyes and the limited resolution of imaging mass spectrometry. We present ultrasensitive reweighted visible stimulated Raman scattering (URV-SRS), a label-free vibrational nanoscopy technique that enables multiplexed detection of metabolic nanostructures within cells. We developed an extensively chirped spectral focusing visible SRS microscope that achieves a detection limit of 4,000 molecules and introduced a self-supervised learning-based denoiser to robustly suppress non-independent SRS noise by over 7.2 dB. The instrumentation-based signal enhancement and computation-based noise suppression synergistically improved the detection sensitivity by 50 times over near-infrared SRS. Leveraging this enhanced sensitivity, we further pushed the resolution to nanoscopic levels by introducing Fourier reweighting to amplify sub-100 nm spatial frequencies previously overwhelmed by noise. Validated by Fourier ring correlation, URV-SRS achieves a lateral resolution of 86 nm in cellular imaging. Here, we applied URV-SRS to elucidate the reprogramming of metabolic nanostructures associated with virus replication in Vero E6 host cells and to compositionally delineate subcellular fatty acid synthesis in engineered Escherichia coli, demonstrating its capability towards nanoscopic spatial metabolomics.
59 BASIC BIOLOGICAL SCIENCES↗
Direct evidence of the effect of a moderate external magnetic field on stimulated Raman scattering in the kinetic regime
We present results from an experiment carried out at the OMEGA-EP laser facility that investigated the effect of a perpendicular magnetic field on stimulated Raman scattering (SRS) and report the first direct measurement of magnetic mitigation of SRS. A 13-T magnetic field generated by pulsed-power coils was imposed on a gas jet plasma, and a novel three-picket interaction beam was used to explore SRS reflectivity for several plasma conditions within single shots. The time-resolved backscattered light shows that SRS was mitigated by the external 13-T magnetic field in the kinetic regime (kλ D ∼ 0.3, where k is the electron plasma wave's wavenumber and λ D is electron Debye length) and at a density of n e /n cr ∼ 0.10. On the other hand, we also measured an enhancement of SRS reflectivity at lower density (n e /n cr < 0.08). We discuss experimental results in the context of magnetohydrodynamic and particle-in-cell simulations that scan SRS dynamics for a variety of plasma conditions. While the experimental evidence of SRS mitigation validates prior work on the kinetic simulation of SRS in an external magnetic field, we also find that other mechanisms such as SRS rescatter can lead to an enhancement of measured SRS reflectivity in simulations of parameters relevant to our experiment.
Gas jet↗
Measurement of Off-Body Velocity, Pressure, and Temperature in an Unseeded Supersonic Air Vortex by Stimulated Raman Scattering
A noninvasive optical method is used to make time-averaged (30 sec) off-body measurements in a supersonic airflow. Seeding of tracer particles is not required. One spatial component of velocity, static pressure, and static temperature are measured with stimulated Raman scattering. The three flow parameters are determined simultaneously from a common sample volume (0.3 by 0.3 by 15 mm) using concurrent measurements of the forward and backward scattered line shapes of a N2 vibrational Raman transition. The capability of this technique is illustrated with laboratory and large-scale wind tunnel testing that demonstrate 5-10% measurement uncertainties. Because the spatial resolution of the present work was improved to 1.5 cm (compared to 20 cm in previous work), it was possible to demonstrate a modest one-dimensional profiling of cross-flow velocity, pressure, and translational temperature through the low-density core of a stream-wise vortex (delta-wing model at Mach 2.8 in NASA Langley's Unitary Plan Wind Tunnel).
Herring, Gregory C.↗