Ultrafast vibrational relaxation of O–H bending and librational excitations in liquid H2O

Huse, Nils; Ashihara, Satoshi; Nibbering, Erik T. J.; Elsaesser, Thomas

doi:10.1016/j.cplett.2005.02.007

Cited by 121 publications

(195 citation statements)

References 20 publications

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“…In addition to the strong intermolecular couplings, this explains the ultrafast nature of the vibrational relaxation dynamics in water as compared to those of nonpolar liquids. A similarly VER is observed for water when the fundamental transition of the bending vibration, the bending vibrational combination tone or the librational fundamental is excited [5,[21][22][23].…”

Section: Introductionmentioning

confidence: 75%

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OH and NH Stretching Vibrational Relaxation of Liquid Ethanolamine

Knop

Lindner

Vöhringer³

2011

Zeitschrift Für Physikalische Chemie

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Vibrational Relaxation / Liquid Dynamics / Hydrogen-Bonding / Ultrafast SpectroscopyFemtosecond mid-infrared pump-probe spectroscopy was carried out to obtain information about the dynamics of vibrational energy relaxation in liquid ethanolamine at room temperature and ambient pressure. Through partial deuteration it was possible to disentangle the dynamics resulting from the OH and the NH stretching modes that proceed independently and simultaneously in the hydrogen-bonded liquid following an ultrafast vibrational excitation by a resonant mid-infrared pulse. The OH-stretching vibrational lifetime was determined to be 450 fs while the NH-stretching lifetime was found to be 1.2 ps. This large difference in lifetimes highlights the importance of the hydrogen-donating and the hydrogen-accepting character of the vibrating groups that are engaged in hydrogen-bonding.

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Section: Introductionmentioning

confidence: 75%

“…This deuteration also circumvents a canonical heating of the sample that will inevitably occur upon laser induced vibrational excitation of the neat liquid. Depopulation of the v = 1 vibrational state occurs on a time scale of about 1 ps and is believed to occur through the bending manifold [5,14,18,[20][21][22][23][24].…”

Section: Introductionmentioning

confidence: 99%

OH and NH Stretching Vibrational Relaxation of Liquid Ethanolamine

Knop

Lindner

Vöhringer³

2011

Zeitschrift Für Physikalische Chemie

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“…This gives rise to infrared absorption bands with very complex behavior occurring on time scales well below 100 femtoseconds. [10][11][12][13][14] The observed dynamics on ultrafast time scales have been successfully identified with: the fast modulation of transition frequencies by coupled molecular oscillators, resonant energy transfer among the densely packed OH stretching oscillators, and exceptionally efficient vibrational energy relaxation. All of these findings are a manifestation of the fluctuating hydrogen bond network that forms the 'supramolecular' structure of water.…”

Section: Introductionmentioning

confidence: 95%

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

Wen

Huse

Schoenlein

et al. 2009

The Journal of Chemical Physics

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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 sub-picosecond time-constant. The latter describes the thermalization time of vibrational excitations and defines the characteristic maximum rate with which non-equilibrium 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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“…More recently, the OH bending vibration δ OH in H 2 O and D 2 O and librational modes ν L between 650cm -1 and 1800cm -1 have been investigated by femtosecond vibrational spectroscopy. 20,21,22,23,24 There is also abundant literature on the low-frequency spectral response of water between a few wavenumbers and the O···O stretching vibration ν O···O . 25,26,27,28,29,30 Static x-ray spectroscopy experiments have been used to investigate the oxygen K-edge of water, the near-edge region of which is shown in Fig.…”

Section: Introductionmentioning

confidence: 99%

Probing the hydrogen-bond network of water via time-resolved soft X-ray spectroscopy

Huse

Wen

Nordlund

et al. 2009

Phys. Chem. Chem. Phys.

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We report time-resolved studies of hydrogen bonding in liquid H 2 O, in response to direct excitation of the O-H stretch mode at 3 µm, 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 liquid phase. Distinct changes in the near-edge spectral region (XANES) are observed, and are indicative of a transient temperature rise of 10K 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 8MPa, is manifest 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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Ultrafast vibrational relaxation of O–H bending and librational excitations in liquid H2O

Cited by 121 publications

References 20 publications

OH and NH Stretching Vibrational Relaxation of Liquid Ethanolamine

OH and NH Stretching Vibrational Relaxation of Liquid Ethanolamine

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

Probing the hydrogen-bond network of water via time-resolved soft X-ray spectroscopy

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