Time-resolved measurements of the structure of water at constant density

Lindenberg, Aaron M.; Acremann, Yves; Lowney, D.; Heimann, P. A.; Allison, Thomas K.; Matthews, Tyler S.; Falcone, R. W.

doi:10.1063/1.1906212

Cited by 27 publications

(26 citation statements)

References 38 publications

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“…The pump causes a local increase in temperature of the solvent. Time-resolved measurements of the structure of the water solvent at constant density [22] have shown that these temperature induced changes are observed for several hundreds of picoseconds. This can influence the measured transient absorption in the infrared region, for example through a change in the solvent refractive index as proposed in Ref.…”

Section: Discussionmentioning

confidence: 97%

Observation of a persistent infrared absorption following two photon ionization of liquid water

et al. 2006

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Section: Discussionmentioning

confidence: 97%

Observation of a persistent infrared absorption following two photon ionization of liquid water

et al. 2006

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“…However, isochorically heated water maintains its initial average density at early times («1 ns), as confirmed by time-resolved diffraction studies. 39 Consequently, changes in hydrogen bonding associated with weaker hydrogen bond interactions must stem from bond distortions (larger bond angles) and increased disorder on these time scales. The observed insensitivity of the main-edge absorption peak to pressure changes at short delay times (high pressures for t « 1 ns) is in good agreement with the observed changes comparing high-density amorphous ice created at 18 bar to ambient water.…”

Section: Discussionmentioning

confidence: 99%

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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“…In contrast, the weak scattering cross section of x rays compared to electrons allows for bulk probing of condensed phase dynamics, but has so far limited x-ray scattering studies of disordered or liquid systems to 100 ps time scales [9][10][11][12]. We describe here diffuse x-ray scattering measurements in which the structural dynamics of the liquid-state and the subsequent ablation process are directly measured with subpicosecond resolution.…”

mentioning

confidence: 99%

X-Ray Diffuse Scattering Measurements of Nucleation Dynamics at Femtosecond Resolution

et al. 2008

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Femtosecond time-resolved small and wide angle x-ray diffuse scattering techniques are applied to investigate the ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is observed and the buildup of these fluctuations is measured in real time. Small-angle scattering measurements reveal snapshots of the spontaneous nucleation of nanoscale voids within a metastable liquid and support theoretical predictions of the ablation process. DOI: 10.1103/PhysRevLett.100.135502 PACS numbers: 79.20.Ds, 61.05.cp, 61.20.Lc, 64.60.ÿi The liquid state of matter can be both supercooled below its freezing point and superheated above its boiling point. Although these are nonequilibrium states, their lifetime is longer than typical laboratory observation times and they are thus classified as metastable, stuck in a local minimum of the free energy. Despite their apparent stability, these systems exhibit localized fluctuations, corresponding to nuclei of the lower energy phase which rapidly form and dissolve, a process for which there exists a critical size for stable growth of the equilibrium phase, typically of nanoscale dimensions [1-3] (depending on the degree of superheating). When the transition does occur, it occurs rapidly, as is familiar to anyone who has observed the catastrophic boiling that suddenly occurs in superheated liquid water [4]. The development of ultrafast, atomic-scale sensitive techniques enables one to capture these transient, intermediate states, which under current laboratory methods, may spontaneously transform to lower energy stable states on inaccessible time scales. Techniques like time-resolved x-ray or electron scattering record these intermediate states in the form of a diffuse scattering pattern whose shape reflects the local atomic-scale structure that characterizes the transforming material. As a result of the orientational isotropy in the system and the short correlation lengths, these are typically broad diffraction rings, in contrast to the well-defined diffracted beams one obtains from a crystalline system. The radially averaged diffracted intensity as a function of scattering angle (normalized by atomic scattering factors) is a direct measure of the liquid structure factor S Q , where Q 4 sin = is the momentum transfer, 2 is the scattering angle, and is the wavelength, which directly encodes the short-range correlations in disordered materials.Recent experiments probing atomic-scale dynamics in disordered systems using electron diffraction techniques have focused on gas-phase photochemical reactions [5],

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Time-resolved measurements of the structure of water at constant density

Cited by 27 publications

References 38 publications

Observation of a persistent infrared absorption following two photon ionization of liquid water

Observation of a persistent infrared absorption following two photon ionization of liquid water

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

X-Ray Diffuse Scattering Measurements of Nucleation Dynamics at Femtosecond Resolution

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