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Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x-ray spectroscopy
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View: Figures


Image of FIG. 1.
FIG. 1.

Schematic drawing of the femtosecond soft x-ray beamline at the Advanced Light Source. A femtosecond Ti:sapphire laser system supplies two synchronous laser pulses. One of them is sent into the synchrotron to generate a femtosecond x-ray pulse, the second pulse is frequency-converted to the infrared via an OPA with subsequent DFG and is used for excitation of the OH stretching mode in an infrared pump\x-ray probe experiment.

Image of FIG. 2.
FIG. 2.

Static and differential absorption spectra. (a) Static oxygen x-ray absorption spectrum of a 400-nm-thick water film. Dashed lines mark local absorption maxima which define the characteristic spectral regions: the pre-edge (I), main-edge (II), and postedge (III) of the water x-ray spectrum. (b) Differential absorption spectra of the oxygen XANES region recorded at 150 ps (black) and 300 ns (gray) delay. Arrows indicate the spectral positions at which pump-probe transients are recorded (cf. Fig. 3).

Image of FIG. 3.
FIG. 3.

Absorbance change as a function of time delay between the infrared pump pulses and the x-ray probe pulses at three characteristic spectral positions: 534.3 eV (red), 536.3 eV (black), and 542.0 eV (blue). Solid lines are single exponential fits to the data with a time constant of 0.7 ps. The inset shows a time transients on nanosecond time scales recorded on a 400-nm-thick sample, in which the solid red line represents a fit to the data of the form with and . increases with increasing sample thickness.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x-ray spectroscopy