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Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra
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10.1063/1.2219439
/content/aip/journal/jcp/125/4/10.1063/1.2219439
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/4/10.1063/1.2219439
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

(Color online) Schematic optical layout, as described in text. BBO: Nonlinear optic (-BBO, for sum-frequency generation); BS: Beam splitter; CL: Cylindrical lens; DBS: Dichroic beam splitter; G: Grating; OPA: Optical parametric amplifier; TS: Translation stage.

Image of FIG. 2.
FIG. 2.

(Color) (a) Spectrally integrated time-resolved signal from neat toluene as function of probe delay, , with Fourier transform (FT, inset). Dashed line in FT denotes beat frequency that is poorly resolved in integrated signal FT. (b) Spectrally dispersed time-resolved signal from neat toluene (contour plot of spectral intensity, normalized to peak near ); anti-Stokes energies measured relative to centered at . FTs of frequency slices denoted by are shown in Figs. 3(a)–3(c), respectively, following removal of exponentially decaying baseline.

Image of FIG. 3.
FIG. 3.

Fourier transforms (FTs) of frequency slices shown in Fig. 2(b). Dashed line represents beat frequency poorly resolved in Fig. 2(a), demonstrating a benefit of spectral resolution of tr-CARS signal.

Image of FIG. 4.
FIG. 4.

(Color) Numerical simulation of spectrally resolved tr-CARS data from toluene, shown as contour plot of spectral intensity, normalized to peak near .

Image of FIG. 5.
FIG. 5.

Experimental integrated signal (solid curve) in fs/ps CARS studies of neat toluene, shown as a function of probe delay, (bottom axis). Arrow denotes optimal timing for spectrally resolved fs/ps CARS data shown in Fig. 6. Pulse duration and profile compare well with numerical simulation (dashed curve) of optimal pulse temporal profile, assuming a square wave slit, plotted at its optimal delay relative to and pulses (top axis).

Image of FIG. 6.
FIG. 6.

(a) Experimental fs/ps CARS signal from neat toluene, normalized to the peak intensity (details in text); (b) Simulation of toluene CARS signal using narrowband pulse for . Dashed curve represents simulated spectrum independent of instrument response; solid curve includes convolution with (FWHM) Gaussian spectrometer response.

Image of FIG. 7.
FIG. 7.

(Color) (a) Spectrally dispersed time-resolved CARS signal from R6G in methanol, shown as contour plot of spectral intensity (contour color scheme analogous to that of Fig. 4); frequencies measured relative to centered at ; (b) FT of this spectrally dispersed CARS signal, shown as contour plot; (c) Spectrum of R6G in methanol obtained using fs/ps CARS method.

Image of FIG. 8.
FIG. 8.

fs/ps CARS signal from neat chloroform, normalized to the peak intensity.

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/content/aip/journal/jcp/125/4/10.1063/1.2219439
2006-07-24
2014-04-17
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/4/10.1063/1.2219439
10.1063/1.2219439
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