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Results for “stimulated Raman”
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Selective photo-excitation of molecules enabled by stimulated Raman pre-excitation
Double resonance excitation, where the energies of vibrational and electronic molecular transitions are combined in a single, sequential excitation process, was introduced in the 1970s but has only been recently applied to microscopy due to the immense progress in Raman spectroscopy. The value of the technique is in combining the chemical selectivity of IR or Raman excitation with the much larger cross-sections of electronic transitions. Recently, it has been shown to be particularly suited for the detection and identification of chromophores at low concentrations and in the presence of spectral crosstalk. However, despite its low quantum yield per pulse sequence, we believe the technique has potential for selective photochemical transformations. There are some cases (e.g., the selective excitation of optogenetic switches) where the low yield may be overcome by repeated excitations to build up biochemically relevant concentrations. Here we show that double resonance excitation using general, non-resonant Raman pre-excitation is a viable candidate for selectively promoting molecules to chemically active energy levels. Further, the use of non-resonant Raman pre-excitation is less constraining than resonant Raman (used in previous double resonance microscopy works) since the choice of Raman pump-Stokes frequencies may be rather freely chosen.
Ultrafast coherent photoexcited dynamics in a trimeric dendrimer probed by X-ray stimulated-Raman signals
The photoinduced ultrafast coherent inter-chromophore energy redistribution in a triarylamine trimer is explored using nonadiabatic excited state molecular dynamics followed by simulations of X-ray Raman signals.
Forward picosecond Stokes-pulse generation in transient stimulated Raman scattering
Transient molecular vibration excitation by picosecond laser pulses found dependent on shape of Stokes pulses in Raman scattering study
Molecular velocimetry using stimulated Raman spectroscopy
Molecular flow velocity of N2 was measured in a supersonic wind tunnel using inverse Raman spectroscopy. This technique employs the large Doppler shift exhibited by the molecules when the pump and probe laser beams are counter-propagating (backward scattering). A retrometer system is employed to yield a vibration-free optical configuration which has the additional advantage of obtaining both the forward and backward scattered spectra simultaneously. The linebreadths and their relative Doppler shift can be used to determine the static pressure, translational temperature, and molecular flow velocity. A demonstration of the concept was performed in a supersonic wind tunnel and included: (1) measurements over the Mach number range 2.50 to 4.63; (2) static pressure measurements (at Mach 2.50) corresponding to a Reynolds number per foot range of 1 to 5 x 10 to the 6th power; and (3) measurements behind the shock wave of a flat plate model.
Rotational collisional narrowing in the NO fundamental Q branch, studied with CW stimulated Raman spectroscopy
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Stimulated Raman up-conversion of electromagnetic waves by a gyrating electron beam
A gyrating electron beam supports negative energy modes near the harmonics of electron-cyclotron frequency. An electromagnetic wave passing through such a beam parametrically up-converts into high-frequency electromagnetic modes separated from the pump frequency by the electron-cyclotron harmonics. The growth rate for this process varies directly as the oscillatory velocity of beam electrons caused by the pump and as square root of the beam density. It has a maximum at values of scattering angle close to 180 deg and is also implicitly dependent on the beam veocity and the cyclotron frequency of electrons. The effect of a cold electron component is to reduce the growth rate.
Theoretical studies of Resonance Enhance Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor
It is well known that the presence of a real atomic level which is nearly resonant with the pump field can greatly enhance the Raman emission cross section. In order to accurately calculate the Raman gain in systems where resonance enhancement plays a dominant role, expressions for the pump and signal susceptibilities must be derived. These expressions should be valid for arbitrary field strengths in order to allow for pump and signal saturation. In addition, the theory should allow for arbitrary longitudinal and transverse relaxation rates. This latter point is extremely vital for three level atomic systems such as the alkali earth metals since they do not have population reservoirs and can have widely varying spontaneous lifetimes on the three pertinent transitions. Moreover, the dephasing rates are strong functions of electron states and are therefore also different for the three coupled pairs of levels. These considerations are not as important when molecular systems are concerned since the large reservoir of rotational states serve to produce essentially equal longitudinal recovery rates for the population of the three levels. The three level system with three arbitrary longitudinal and transverse relaxation rates was solved. There is no need for setting either pair of rates equal and the expressions are valid for arbitrarily strong fields.
Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor
This work focused on understanding the effects of arbitrary transverse and longitudinal relaxation rates on the susceptibilities of coherently driven three-level systems. The approximation of a single relaxation rate often made in previous work is strongly invalidated by the variation in the spontaneous emission lifetime between various atomic level pairs in systems such as cesium. It is of great importance to the problem of nonlinear infrared generation to determine the dependence of both real and imaginary susceptibility on relaxation rates. The imaginary susceptibility on the pump transition determines the absorption of pump photons and the imaginary susceptibility on the laser transition determines the spectral dependence of the gain. This is of particular importance for pure Raman emission (i.e., absorption at linecenter of the gain transition) as it determines the tunability characteristics we are aiming to predict. The real susceptibility is important when cavities are used at the signal field as this will determine the loaded resonance of the Raman oscillator. Researchers show that in some cases which result from having different relaxation rates mode splitting may result, allowing more than one frequency to have the same Raman wavelength, possibly resulting in a temporal instability.
Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency-doubled Alexandrite laser wavelength in cesium vapor
The solutions for the imaginary susceptibility of the Raman field transition with arbitrary relaxation rates and field strengths are examined for three different sets of relaxation rates. These rates correspond to: (1) Far Infrared (FIR) Raman lasers in the diabatic collision regime without consideration of coupled population decay in a closed system, (2) Raman FIR lasers in the diabatic collision regime with coupled population conserving decay, and (3) IR Raman gain in cesium vapor. The model is further expanded to include Doppler broadening and used to predict the peak gain as a function of detuning for a frequency doubled Alexandrite laser-pumped cesium vapor gain cell.
Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelength in cesium vapor
The third phase of research will focus on the propagation and energy extraction of the pump and SERS beams in a variety of configurations including oscillator structures. In order to address these questions a numerical code capable of allowing for saturation and full transverse beam evolution is required. The method proposed is based on a discretized propagation energy extraction model which uses a Kirchoff integral propagator coupled to the three level Raman model already developed. The model will have the resolution required by diffraction limits and will use the previous density matrix results in the adiabatic following limit. Owing to its large computational requirements, such a code must be implemented on a vector array processor. One code on the Cyber is being tested by using previously understood two-level laser models as guidelines for interpreting the results. Two tests were implemented: the evolution of modes in a passive resonator and the evolution of a stable state of the adiabatically eliminated laser equations. These results show mode shapes and diffraction losses for the first case and relaxation oscillations for the second one. Finally, in order to clarify the computing methodology used to exploit the speed of the Cyber's computational speed, the time it takes to perform both of the computations previously mentioned to run on the Cyber and VAX 730 must be measured. Also included is a short description of the current laser model (CAVITY.FOR) and a flow chart of the test computations.
Laser-induced stimulated Raman scattering in the forward direction of a droplet - Comparison of Mie theory with geometrical optics
This paper uses Mie theory to treat electromagnetic scattering and to evaluate field enhancement in the forward direction of a small droplet irradiated by a high-energy beam and compares the results of calculations with the field-enhancement evaluation obtained via geometrical optics treatment. Results of this comparison suggest that the field enhancement located at the critical ring region encircling the axis in the forward direction of the droplet can support laser-induced Raman scattering. The results are supported by experimental observations of the interaction of a 120-micron-diam water droplet with a high-energy Nd:YAG laser beam.
Collisional broadening of rotational lines in the stimulated Raman pentad Q-branch of CD4
Self- and argon-broadening coefficients are reported for a number of Raman Q-branch transitions in the nu(1) and nu(2) + nu(4) bands of (C-12)D4 at room temperature (296 K). The coefficients display a variation with j and with C exp n (symmetry species A, E, F) that is essentially independent of collision partner and which is similar to the j- and C exp n-dependence found in previous measurements of the IR line-broadening coefficients. The rotationally inelastic collision rates previously measured by Foy et al. (1988) for (C-13)D4 (V4 = 0, 1) in collision with (C-13)D4 or Ar account for only a part of the Raman broadening rate, suggesting possibly significant contributions to the linewidths from efficient V-V transfer or elastic dephasing collisions.
Stimulated Raman amplification, oscillation, and linewidth in barium nitrate
Measurements of Raman gain in a Ba(NO3)2 crystal are reported at 532 nm using a Raman oscillator/amplifier arrangement for differential absorption lidar measurements of ozone. The experimentally determined gain coefficient will be compared with theoretical results. The effect of single and multi-longitudinal mode pumping upon the amplification process will be discussed. Measurement of the Raman linewidth for 1st 2nd and 3d stokes shifts arc presented.
Four-dimensional dynamics of multirotational transition stimulated rotational Raman scattering in air
Stimulated rotational Raman scattering in air is a powerful parasitic process that degrades high intensity laser beams and pulses propagated over significant distances. Conversely, it is used beneficially in the context of Raman lasers. Through this inelastic scattering process, laser photons are converted to higher (anti-Stokes) or lower (Stokes) energies, according to rotational mode transitions in nitrogen and oxygen diatomic molecules. The full wave-mixing problem involves numerous frequencies, and it is consistently assumed that only one rotational mode contributes to the conversion process. We instead present a dynamic 4D multirotational model that is implemented in a parallelized manner within the Virtual Beamline++ optical modeling package allowing high-resolution 4D studies. We highlight the effect that spontaneous emission plays in large and small beam-width setups, even in the highly saturating regime. The weaker transition modes play a large role in the persistent dynamics and can lead to complex spatiotemporal coupling through nonlinear competition of the modes. We highlight how and why these weaker modes persist, how the size and shape of speckle patterns depends highly on the initial beam profile, and how weaker modes can transiently become stronger as a result of such competition.
Stimulated Raman-scattering threshold behavior of binary mixture micrometer-sized droplets
Stimulated Raman scattering (SRS) from binary liquid mixture micrometer-sized droplets irradiated by nanosecond laser pulses exhibits previously unreported features. SRS emission at wavelength shifts corresponding to combination frequencies of the individual component Stokes shifts are observed in droplets but not in bulk mixtures. Furthermore, droplet SRS thresholds are determined by component refractive indices and concentrations, in contrast to bulk thresholds, for which self-focusing likely plays a dominant role.
Nearly degenerate two-color impulsive coherent Raman hyperspectral imaging
Impulsive stimulated Raman scattering (ISRS) is a robust technique for studying low frequency (<300 cm –1 ) Raman vibrational modes, but ISRS has faced difficulty in translation to an imaging modality. A primary challenge is the separation of the pump and probe pulses. Here we introduce and demonstrate a simple strategy for ISRS spectroscopy and hyperspectral imaging that uses complementary steep edge spectral filters to separate the probe beam detection from the pump and enables simple ISRS microscopy with a single-color ultrafast laser source. ISRS spectra are obtained that span from the fingerprint region down to <50 cm –1 vibrational modes. Furthermore, hyperspectral imaging and polarization-dependent Raman spectra are also demonstrated.
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.