Hydrogen-bond dynamics in water explored by heterodyne-detected photon echo

Yeremenko, Sergey; Pshenichnikov, Maxim S.; Wiersma, Douwe A.

doi:10.1016/s0009-2614(02)02001-8

Cited by 173 publications

(216 citation statements)

References 32 publications

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“…Nonlinear vibrational spectroscopy, such as two dimensional infrared spectroscopy (2D IR) [26][27][28][29][30][31][32][33], is an excellent tool to monitor the local structure and dynamical properties of the hydrogen bonds in water. These experiments make use of the fact that the vibrational frequency of the OH stretch vibration is highly correlated with the OO distance of a pair of hydrogen bonded water molecules [34][35][36][37][38].…”

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Infrared Spectroscopy of Isotope-Diluted Low Density Amorphous Ice

2013

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We present two-dimensional (2D) infrared (IR) spectra of isotope diluted ice in its low density amorphous form. Amorphous ice, which is structurally more similar to liquid water than to crystalline ice, provides higher resolution spectra of the hydrogen bond potentials because all motion is frozen. In the case of OD vibration of HOD in H2O, diagonal and off-diagonal (intermode) anharmonicity as well as the relaxation rate of the first excited state increase with hydrogen bond strength in a consistent way. For the OH vibration of HOD in D2O, additional more specific couplings need to be taken into account to explain the 2D IR response, that is, a Fermi resonance with the HOD bend vibration and couplings to phonon modes that lead to quantum beating. The lifetime of the fist excited state, 240 fs, is the shortest ever reported for any phase of isotope diluted water. We present 2D IR spectra of isotope diluted ice in its low density amorphous form. Amorphous ice, which is structurally more similar to liquid water than to crystalline ice, provides higher resolution spectra of the hydrogen bond potentials because all motion is frozen. In the case of OD vibration of HOD in H2O, diagonal and off-diagonal (inter-mode) anharmonicity as well as the relaxation rate of the first excited state increases with hydrogen bond strength in a consistent way. For the OH vibration of HOD in D2O, additional more specific couplings need to be taken into account to explain the 2D IR response, that is, a Fermi resonance with the HOD bend vibration and couplings to phonon modes that lead to quantum beating. The lifetime of the fist excited state, 240 fs, is the shortest ever reported for any phase of isotope diluted water.

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Section: Introductionmentioning

confidence: 99%

Two-Dimensional Infrared Spectroscopy of Isotope-Diluted Low Density Amorphous Ice

2013

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“…19,20 From temperature dependent simulations 21,22 and experimental studies of isotope diluted water, ranging from ambient conditions 23,24 up to the supercritical regime 25 is understood that FFCF decay depends critically on temperature. Furthermore from time resolved optical Kerr effect (HD-OKE) measurements in supercooled water has been observed that water dynamics are characterized by a distribution of different timescales due to the presence of a variety of relaxing structures.…”

Section: Introductionmentioning

confidence: 99%

Two-Dimensional Infrared Spectroscopy of Supercooled Water

Perakis

Hamm

2010

J. Phys. Chem. B

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We present two-dimensional infrared (2D IR) spectra of the OD stretch vibration of isotope diluted water (HOD/H2O) from ambient conditions (293 K) down to the metastable supercooled regime (260 K). We observe that spectral diffusion slows down from 700 fs to 2.6 ps as we lower the temperature. A comparison between measurements performed at the magic angle with those at parallel polarization shows that the 2D IR line shape is affected by the frequency-dependent anisotropy decay in the case of parallel polarization, altering the extracted correlation decay. A fit within the framework of an Arrhenius law reveals an activation energy of Ea = 6.2 ± 0.2 kcal/mol and a pre-exponential factor of 1/A = 0.02 ± 0.01 fs. Alternatively, a power law fit results in an exponent γ = 2.2 and a singularity temperature Ts = 221 K. We tentatively conclude that the power law provides the better physical picture to describe the dynamics of liquid water around the freezing point. 2D IR spectroscopy of supercooled water AbstractWe present 2D IR spectra of the OD stretch vibration of isotope diluted water (HOD/H 2 O) from ambient conditions (293 K) down to the metastable supercooled regime (260 K). We observe that spectral diffusion slows down from 700 fs to 2.6 ps as we lower the temperature.Comparison between measurements performed at magic angle with those at parallel polarization shows that the 2D IR lineshape is affected by the frequency dependent anisotropy decay in the case of parallel polarization, altering the extracted correlation decay. A fit within the framework of an Arrhenius law reveals an activation energy of E a = 6.2 ± 0.2 kcal/mol and a pre-exponential factor of 1/A = 0.02 ± 0.01 fs. Alternatively, a power law fit results in an exponent γ = 2.2 and a singularity temperature T s = 221 K. We tentatively conclude that the power law provides the better physical picture to describe the dynamics of liquid water around the freezing point.

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“…14 Bulk water dynamics occur over a range of time scales, from tens of femtoseconds to several picoseconds. [15][16][17][18][19][20][21][22] These dynamics are complex and encompass elastic and inelastic interactions with the surrounding water molecules. Vibrational lifetimes, excitation transfer, dephasing and orientational correlation times are all observed to decay by ∼2 ps for bulk water.…”

Section: Introductionmentioning

confidence: 99%

“…49 Here, we present a detailed account of the vibrational echo experiments on AOT reverse micelles that have been reported previously, 49 including new frequency-dependent data, as well as vibrational pump-probe experiments that examine the population dynamics of the hydroxyl stretch. Vibrational echo spectroscopy [16][17][18]20,[50][51][52][53][54][55][56] is uniquely capable of determining system dynamics by removing the inhomogeneous broadening contribution from the line shape 16,[56][57][58][59][60][61][62] and tracking the underlying dynamics. 63, 64 The properties of hydrogen-bond networks can be studied using IR spectroscopy of the hydroxyl stretching mode, because of the strong influence of the number and strength of hydrogen bonds on the hydroxyl stretch frequency.…”

Section: Introductionmentioning

confidence: 99%

Dynamics of Nanoscopic Water: Vibrational Echo and Infrared Pump−Probe Studies of Reverse Micelles

2005

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The dynamics of water in nanoscopic pools 1.7-4.0 nm in diameter in AOT reverse micelles were studied with ultrafast infrared spectrally resolved stimulated vibrational echo and pump-probe spectroscopies. The experiments were conducted on the OD hydroxyl stretch of low-concentration HOD in the H 2 O, providing a direct examination of the hydrogen-bond network dynamics. Pump-probe experiments show that the vibrational lifetime of the OD stretch mode increases as the size of the reverse micelle decreases. These experiments are also sensitive to hydrogen-bond dissociation and reformation dynamics, which are observed to change with reverse micelle size. Spectrally resolved vibrational echo data were obtained at several frequencies. The vibrational echo data are compared to data taken on bulk water and on a 6 M NaCl solution, which is used to examine the role of ionic strength on the water dynamics in reverse micelles. Two types of vibrational echo measurements are presented: the vibrational echo decays and the vibrational echo peak shifts. As the water nanopool size decreases, the vibrational echo decays become slower. Even the largest nanopool (4 nm, ∼1000 water molecules) has dynamics that are substantially slower than bulk water. It is demonstrated that the slow dynamics in the reverse micelle water nanopools are a result of confinement rather than ionic strength. The data are fit using time-dependent diagrammatic perturbation theory to obtain the frequency-frequency correlation function (FFCF) for each reverse micelle. The results are compared to the FFCF of water and show that the largest differences are in the slowest time scale dynamics. In bulk water, the slowest time scale dynamics are caused by hydrogen-bond network equilibration, i.e., the making and breaking of hydrogen bonds. For the smallest nanopools, the longest time scale component of the water dynamics is ∼10 times longer than the dynamics in bulk water. The vibrational echo data for the smallest reverse micelle displays a dependence on the detection wavelength, which may indicate that multiple ensembles of water molecules are being observed.

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Hydrogen-bond dynamics in water explored by heterodyne-detected photon echo

Cited by 173 publications

References 32 publications

Two-Dimensional Infrared Spectroscopy of Isotope-Diluted Low Density Amorphous Ice

Two-Dimensional Infrared Spectroscopy of Isotope-Diluted Low Density Amorphous Ice

Two-Dimensional Infrared Spectroscopy of Supercooled Water

Dynamics of Nanoscopic Water: Vibrational Echo and Infrared Pump−Probe Studies of Reverse Micelles

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