Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals

Roy, Sukesh; Meyer, Terrence R.; Gord, James R.

doi:10.1063/1.2159576

Cited by 88 publications

(69 citation statements)

References 11 publications

(9 reference statements)

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“…Recent advances in the microscopic applications of this technique have improved signal collection through the use of tightly focused beams 2 which relax the phase matching condition, and techniques for limiting the non-resonant signal. 3,4 Spectroscopic studies have separated resonant from non-resonant signal in the time-domain 3 and designed more efficient 5,6 collection sequences. The enhancement of CARS by intense plasmon fields could potentially enhance signal further and is the motivation for this work.…”

mentioning

confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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We present the first density functional simulations of coherent anti-Stokes Raman scattering (CARS) and an analysis of the chemical effects upon binding to a metal surface. Spectra are obtained from first-principles electronic structure calculations and are compared with available experiments and previously available theoretical results following from Hartree–Fock polarizability derivatives. A first approximation to the nonresonant portion of the CARS signal is also explored. We examine the silver pyridine cluster models of the surface chemical signal enhancement, previously introduced for surface-enhanced Raman scattering. Chemical resonant intensity enhancements of roughly 102 are found for several model clusters. The prospects of realizing further enhancement of CARS signal with metal surfaces is discussed in light of the predicted chemical enhancements.

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confidence: 99%

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Parkhill

Rappoport

Aspuru‐Guzik

2011

J. Phys. Chem. Lett.

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“…1, and the ps-CARS optical setup has been described in detail previously. 17 Briefly, it consists of a ps-duration, pulsed Nd:YAG laser (Ekspla, Model SL230) that operates at 10 Hz and produces nearly transform-limited pulses [fullwidth-at-half-maximum (FWHM) duration of $150 ps and maximum pulse energy of 100 mJ/pulse] at 532 nm; this beam is split into pump and probe beams, each with an energy of 800 lJ/pulse. A fraction of this laser output is also split off to pump a home-made modeless dye laser (FWHM bandwidth of $5 nm and FWHM duration of $110 ps) for generating the Stokes beam at 606 nm with an energy of 3 mJ/pulse.…”

Section: Methodsmentioning

confidence: 99%

“…We have applied picosecond coherent anti-Stokes Raman scattering (ps-CARS), which is a well-established non-invasive approach to measuring temperature in a reacting environment with excellent accuracy and precision, [16][17][18][19] to allow thermometric measurements of the gas-phase species in thermal equilibrium with reacting, energetic nanoparticle samples following laser flash heating. This point-wise detection approach permits spatially resolved measurements under single-laser-shot conditions, and the temporal resolution of this approach is limited only by the greater of the durations of the flash-heating laser [several nanoseconds (ns) in this work] and the sub-ns pulse durations used in the ps-CARS techniques.…”

Section: Introductionmentioning

confidence: 99%

Spatially and temporally resolved temperature and shock-speed measurements behind a laser-induced blast wave of energetic nanoparticles

Roy

Jiang

Stauffer

et al. 2013

Journal of Applied Physics

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Spatially and temporally resolved temperature measurements behind an expanding blast wave are made using picosecond (ps) N2 coherent anti-Stokes Raman scattering (CARS) following laser flash heating of mixtures containing aluminum nanoparticles embedded in ammonium-nitrate oxidant. Production-front ps-CARS temperatures as high as 3600 ± 180 K-obtained for 50-nm-diameter commercially produced aluminumnanoparticle samples-are observed. Time-resolved shadowgraph images of the evolving blast waves are also obtained to determine the shock-wave position and corresponding velocity. These results are compared with near-field blast-wave theory to extract relative rates of energy release for various particle diameters and passivating-layer compositions.Keywords aluminum nanoparticles, coherent anti-Stokes Raman scattering, energetic nanoparticles, energy release, laser flash-heating, particle diameters, relative rates, coherent scattering, Raman spectroscopy Disciplines Mechanical Engineering CommentsThe following article appeared in Journal of Applied Physics 113, 184310 (2013) Spatially and temporally resolved temperature and shock-speed measurements behind a laser-induced blast wave of energetic nanoparticles Spatially and temporally resolved temperature measurements behind an expanding blast wave are made using picosecond (ps) N 2 coherent anti-Stokes Raman scattering (CARS) following laser flash heating of mixtures containing aluminum nanoparticles embedded in ammonium-nitrate oxidant. Production-front ps-CARS temperatures as high as 3600 6 180 K-obtained for 50-nmdiameter commercially produced aluminum-nanoparticle samples-are observed. Time-resolved shadowgraph images of the evolving blast waves are also obtained to determine the shock-wave position and corresponding velocity. These results are compared with near-field blast-wave theory to extract relative rates of energy release for various particle diameters and passivating-layer compositions. V C 2013 AIP Publishing LLC.[http://dx

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“…Such a variation in temperature would normally be accompanied by a factor of several hundred reduction in signal intensity in rotational CARS measurements. 19 However, by taking advantage of the significantly larger coherence dephasing rates encountered in lower temperature gas zones as opposed to high temperature zones, 21,22 a probe delay of 350 ps brings the CARS signal levels from both hot zones and cold zones to within a factor of 20 of each other, well within the 16-bit dynamic range of a typical CCD.…”

Section: (Right)mentioning

confidence: 99%

Communication: Simplified two-beam rotational CARS signal generation demonstrated in 1D

Bohlin

Patterson²,

Kliewer³

2013

The Journal of Chemical Physics

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We explore a novel phase matching scheme for gas-phase rotational coherent anti-Stokes Raman spectroscopy (CARS). The scheme significantly simplifies the employment of the technique in general. Two laser beams, one broadband and one narrowband, are crossed at arbitrary angle and the generated rotational CARS signal, copropagating with the probe beam, is isolated using a polarization gating technique. The effect of phase-vector mismatch for various experimental implementations was measured experimentally and compared to calculations. The spatial resolution of the current technique is improved by more than an order of magnitude over standard gas-phase CARS experimental arrangements, providing an interaction length of less than 50 μm when desired. Both the pump and Stokes photons originate from the broadband pulse, and are therefore automatically overlapped temporally and spatially. Significantly improved signal levels are achieved because of both the ease of alignment and the higher pulse energy available to the pump and Stokes fields. We demonstrate the technique for single-laser-shot 1D rotational CARS signal generation over approximately a 1 cm field in a flame.

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Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals

Abstract: Published by the AIP PublishingArticles you may be interested in Analysis of time resolved femtosecond and femtosecond/picosecond coherent anti-Stokes Raman spectroscopy: Application to toluene and Rhodamine 6G

Cited by 88 publications

References 11 publications

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Modeling Coherent Anti-Stokes Raman Scattering with Time-Dependent Density Functional Theory: Vacuum and Surface Enhancement.

Spatially and temporally resolved temperature and shock-speed measurements behind a laser-induced blast wave of energetic nanoparticles

Communication: Simplified two-beam rotational CARS signal generation demonstrated in 1D

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