期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 102, 期 9, 页码 3202-3207出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0404916102
关键词
hydrogen bonding; infrared pump-probe spectroscopy; energy transfer
We present femtosecond midinfrared pump-probe measurements of the molecular motion and energy-transfer dynamics of a water molecule that is enclosed by acetone molecules. These confined water molecules show hydrogen-bond and orientational dynamics that are much slower than in bulk liquid water. This behavior is surprising because the hydrogen bonds to the C=O groups of the acetone molecules are weaker than the hydrogen bonds in bulk water. The energy transfer between the O-H groups of the confined water molecules has a time constant of 1.3 +/- 0.2 ps, which is >20 times slower than in bulk water. We find that this energy transfer is governed completely by the rate at which hydrogen bonds are broken and reformed, and we identify the short-lived molecular complex that forms the transition state of this process.
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