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

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We present the first femtosecond soft x-ray spectroscopy in liquids, enabling the observation of changes in hydrogen bond structures in water via core-hole excitation. The oxygen K-edge of vibrationally excited water is probed with femtosecond soft x-ray pulses, exploiting the relation between different water structures and distinct x-ray spectral features. After excitation of the intramolecular OH stretching vibration, characteristic x-ray absorption changes monitor the conversion of strongly hydrogen-bonded water structures to more disordered structures with weaker hydrogen-bonding described by a single subpicosecond time constant. The latter describes the thermalization time of vibrational excitations and defines the characteristic maximum rate with ... continued below

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Wen, Haidan; Huse, Nils; Schoenlein, Robert W. & Lindenberg, Aaron M. May 1, 2010.

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We present the first femtosecond soft x-ray spectroscopy in liquids, enabling the observation of changes in hydrogen bond structures in water via core-hole excitation. The oxygen K-edge of vibrationally excited water is probed with femtosecond soft x-ray pulses, exploiting the relation between different water structures and distinct x-ray spectral features. After excitation of the intramolecular OH stretching vibration, characteristic x-ray absorption changes monitor the conversion of strongly hydrogen-bonded water structures to more disordered structures with weaker hydrogen-bonding described by a single subpicosecond time constant. The latter describes the thermalization time of vibrational excitations and defines the characteristic maximum rate with which nonequilibrium populations of more strongly hydrogen-bonded water structures convert to less-bonded ones. On short time scales, the relaxation of vibrational excitations leads to a transient high-pressure state and a transient absorption spectrum different from that of statically heated water.

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  • Journal Name: JOURNAL OF CHEMICAL PHYSICS; Journal Volume: 131; Journal Issue: 23; Related Information: Journal Publication Date: 21 Dec. 2009

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  • Report No.: LBNL-3365E
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 983224
  • Archival Resource Key: ark:/67531/metadc1012340

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  • May 1, 2010

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  • Oct. 14, 2017, 8:36 a.m.

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  • Oct. 17, 2017, 7:02 p.m.

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Wen, Haidan; Huse, Nils; Schoenlein, Robert W. & Lindenberg, Aaron M. Ultrafast conversions between hydrogen bonded structures in liquid water observed by femtosecond x-ray spectroscopy, article, May 1, 2010; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc1012340/: accessed December 11, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.