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Spectrally- and time-resolved vibrational surface spectroscopy: Ultrafast hydrogen-bonding dynamics at / interface
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10.1063/1.1873652
/content/aip/journal/jcp/122/13/10.1063/1.1873652
http://aip.metastore.ingenta.com/content/aip/journal/jcp/122/13/10.1063/1.1873652
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Flow cell design and beam geometry allowing simultaneous recording of the / interface SFG signal and instrument response function (IR-visible pulse cross-correlation).

Image of FIG. 2.
FIG. 2.

Frequency-domain (SFG) spectrum of the transition of at interface (dots—experimental data, green line—fit). IR pulse spectra used for the spectrally- and time-resolved SFG measurements (STiR-SFG) are shown in thin dashed and dotted lines.

Image of FIG. 3.
FIG. 3.

The SFG free induction decay and STiR-SFG measurements of vibrational coherence on surfaces: a, pulse sequence; b, the energy level diagram; c, The two-sided Feynman diagram.

Image of FIG. 4.
FIG. 4.

Right panel: STiR-SFG measurement of at interface. IR excitation (blue side). Vertical axis: IR-visible delay time (fs. horizontal axis: bottom—SFG wavelength; top—converted IR frequency. Left panel: instrument response function (IR-visible SFG-FROG cross-correlation).

Image of FIG. 5.
FIG. 5.

Time-dependent SFG spectral shift following excitation on the blue side of the spectrum, (horizontal cross sections of Fig. 4).

Image of FIG. 6.
FIG. 6.

Time-domain SFG-FID of at interface (projection of STiR-SFG image in Fig. 4 onto the time-delay axis) excited on the blue side of the spectrum . +—/ signal; dots, solid line—instrument response function fit by a Gaussian.

Image of FIG. 7.
FIG. 7.

Right panel: STiR-SFG signal of at interface, IR excitation (red side). Vertical axis, IR-visible delay time (fs); horizontal axis, SFG wavelength. Left panel: instruments response function (IR-visible SFG-FROG cross correlation).

Image of FIG. 8.
FIG. 8.

Time-dependent SFG spectral shift following excitation on the red side of the spectrum, (horizontal cross-sections of Fig. 7). The peaks of each spectrum are indicated by the dots connected by a line.

Image of FIG. 9.
FIG. 9.

Time-domain SFG-FID of at interface (projection of STiR-SFG image in Fig. 7 onto the time delay axis) excited on the red side of the spectrum . +—/ signal; dots, solid line—instrument response function fit by a Gaussian.

Image of FIG. 10.
FIG. 10.

Franck–Condon separation of the OH(OD) stretch mode from the slower H-bond modes (horizontal axis) resulting in two levels with a fluctuating energy gap .

Image of FIG. 11.
FIG. 11.

Calculated STiR-SFG signal for IR excitation on the blue side. Top panel: frequency time correlation functions, Gaussian (a) and exponential (b). (a) Calculated signal for Gaussian frequency correlation function. (b) Same for exponential frequency correlation function.

Image of FIG. 12.
FIG. 12.

(a) Calculated STiR-SFG signal for IR excitation on the red side using an oscillating frequency time correlation function, (b) Time-dependent frequency showing blueshift and damped oscillation. (c) Calculated time-domain SFG-FID (+), solid line—instrument response function (cross correlation of IR and visible fields).

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/content/aip/journal/jcp/122/13/10.1063/1.1873652
2005-04-07
2014-04-16
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Spectrally- and time-resolved vibrational surface spectroscopy: Ultrafast hydrogen-bonding dynamics at D2O/CaF2 interface
http://aip.metastore.ingenta.com/content/aip/journal/jcp/122/13/10.1063/1.1873652
10.1063/1.1873652
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