期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 11, 期 20, 页码 3951-3957出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/b822210j
关键词
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资金
- Director, Office of Science, Office of Basic Energy Sciences, the Chemical Sciences, Geosciences, and Biosciences Division under the Department of Energy [DE-AC02-05CH11231]
- Department of Energy through the Stanford PULSE Institute
- National Science Foundation (NSF) [CHE-0518637]
We report time-resolved studies of hydrogen bonding in liquid H2O, in response to direct excitation of the O-H stretch mode at 3 mm, probed via soft X-ray absorption spectroscopy at the oxygen K-edge. This approach employs a newly developed nanofluidic cell for transient soft X-ray spectroscopy in the liquid phase. Distinct changes in the near-edge spectral region (XANES) are observed, and are indicative of a transient temperature rise of 10 K following transient laser excitation and rapid thermalization of vibrational energy. The rapid heating occurs at constant volume and the associated increase in internal pressure, estimated to be 8 MPa, is manifested by distinct spectral changes that differ from those induced by temperature alone. We conclude that the near-edge spectral shape of the oxygen K-edge is a sensitive probe of internal pressure, opening new possibilities for testing the validity of water models and providing new insight into the nature of hydrogen bonding in water.
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