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Femtosecond coherent anti-Stokes Raman-scattering polarization beat spectroscopy of complex in solid krypton
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10.1063/1.2358987
/content/aip/journal/jcp/125/16/10.1063/1.2358987
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/16/10.1063/1.2358987

Figures

Image of FIG. 1.
FIG. 1.

A schematic presentation of the creation of the CARS polarization via the path , where and refer to the ground and excited electronic states of the species, respectively.

Image of FIG. 2.
FIG. 2.

The effect of Xe concentration on the CARS signal (right side), and the power spectrum (Fourier transform of the signal, left) at .

Image of FIG. 3.
FIG. 3.

The spectrum for the wave packet with at . The labels show the vibrational states involved in the generation of a particular peak in the spectrum, with primed numbers referring to the complex, and numbers without prime to the free .

Image of FIG. 4.
FIG. 4.

The spectrum for the wave packet with at . The labels show the vibrational states involved in the generation of a particular peak in the spectrum, with primed numbers referring to the complex, and numbers without prime to the free .

Image of FIG. 5.
FIG. 5.

The spectrum for the wave packet with at . and are the distances in wave numbers from the free quantum beat band, see Eqs. (12) and (13).

Image of FIG. 6.
FIG. 6.

The effect of temperature on the wave packet spectrum. Both the polarization and quantum beat bands are narrowed and shifted with the decreasing temperature.

Image of FIG. 7.
FIG. 7.

The Raman wave packet weights (solid lines) and (dotted lines) for free and complex, respectively. (a) The wave packet is obtained by pulse sequence, where the pulses are centered at 100 and . (b) The wave packet case originates from sequence of pulses at 200 and . Potentials are derived from the present experimental results in Sec. IV.

Image of FIG. 8.
FIG. 8.

A portion of the lattice atoms in the simulation cube surrounding the impurity iodine molecule. The codoped Xe atom positions are categorized in trapping cases 1–4: (1) A “head-on” position along the molecular axis direction. (2) A “belt” position perpendicular to the molecule. (3) An “ignorant” position 63° off the molecular axis. (4) A “window” position 41° off the axis. The dopant distances to the molecular center are 6.01, 3.47, 4.48, and , respectively. A fcc unit shell is sketched to guide the eye.

Image of FIG. 9.
FIG. 9.

Potential energy surfaces for (upper half) and (lower half) as a function of parallel and perpendicular distances and between the rare gas atom and the middle of the bond . The contour level step is .

Image of FIG. 10.
FIG. 10.

(a) The CARS signal simulated for the 2–6 wave packet with 15% complex concentration. The decay is due to the multiplication by . A portion of the experimental signal is overlaid for comparison. (b) The FFT power spectra obtained from the traces in (a) for the polarization beat region. (c) The FFT power spectra in the fundamental region. (d) The FFT power spectra in the first overtone region. The experimental spectrum is the same as in Fig. 3.

Image of FIG. 11.
FIG. 11.

(a) The CARS signal simulated for the 8–9 wave packet with 1:4 complex:free concentration ratio. The decay is due to the multiplication by . A portion of the experimental signal is shown for comparison. (b) The FFT power spectra obtained from the traces in (a) for the fundamental region. The simulation (solid line) reproduces the experimental (dashed) peak locations: the polarization peaks at and , and the fundamental (8–9) at . The weak contribution from the pure complex (dash-dotted peak) is plotted as the FFT amplitude (instead of power) to illustrate the amplification effect. (c) The FFT power spectra in the polarization beat region. The shift of the peak to slightly higher frequency as compared with the experiment is visible also in the time domain plot (a). See Fig. 5 for labeling.

Tables

Generic image for table
Table I.

Wave numbers (in ) for quantum and polarization beat bands for the superposition from both the experiments and the Morse oscillator fits [Eqs. (14) and (15)]. A “-” sign indicates that the peak is not visible in the spectrum.

Generic image for table
Table II.

Wave numbers (in ) for quantum and polarization beat bands for the superposition from both the experiments and the Morse oscillator fits [Eqs. (14) and (15)]. A “-” sign indicates that the peak is not visible in the spectrum.

Generic image for table
Table III.

Dephasing rates (in ) for free and complex at and , calculated from the frequency-domain fits. (No value: The band needed for analysis is either missing or too weak in the spectrum).

Generic image for table
Table IV.

The difference of solvation energies (in ) of with . The complex case labels are defined in Fig. 8. The two lattice constants and used in geometry optimization are 5.67 and , respectively. Standard deviations for the well depth averages are given in parentheses.

Generic image for table
Table V.

The shifts of the fundamental vibrational transition frequencies for the complex cases from the pure values. The negative values correspond to redshifted frequencies. All values in .

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/content/aip/journal/jcp/125/16/10.1063/1.2358987
2006-10-23
2014-04-21
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Femtosecond coherent anti-Stokes Raman-scattering polarization beat spectroscopy of I2–Xe complex in solid krypton
http://aip.metastore.ingenta.com/content/aip/journal/jcp/125/16/10.1063/1.2358987
10.1063/1.2358987
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