Picosecond ir hole-burning spectroscopy on HDO ice<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mi>Ih</mml:mi></mml:math>

Seifert, G.; Weidlich, Kai; Graener, H.

doi:10.1103/physrevb.56.r14231

Cited by 20 publications

(30 citation statements)

References 16 publications

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“…The red lobe (1-2 transition) is attributed to excited state absorption of the stretch vibration. In agreement with previous hole-burning 38 and pump-probe experiments, 39 the 1-2 transition is significantly broader than the corresponding 0-1 transition. This asymmetry is very pronounced for the OH stretch vibration in HOD/D 2 O (Fig.…”

Section: Resultssupporting

confidence: 79%

“…42 One intriguing observation of previous pump-probe experiments were the extreme asymmetry in linewidth between the 0-1 and 1-2 transitions of the OH vibrator of HOD/D 2 O. 38,39 The 1-2 transition, which is reached only in a nonlinear experiment, has an exceptionally broad linewidth of ≈350 cm −1 , comparable with that of liquid water, while that of the 0-1 transition is much narrower with ≈50 cm −1 . 39 It is generally assumed that the broad linewidth observed in liquid water reflects the large inhomogeneity in hydrogen bonding, contrary to the much narrower linewidth expected in ice, where disorder surely is less, despite the proton disorder discussed above.…”

Section: Introductionmentioning

confidence: 99%

“…The additional information obtained from nonlinear over linear spectroscopy concern the couplings between the various degrees of freedom of ice, as well as the contribution of disorder, due to the sensitivity of nonlinear spectroscopy in distinguishing homogeneous from inhomogeneous broadening. 37 Previous nonlinear spectroscopic studies of ice have resolved the vibrational dynamics of ice Ih using hole burning 38 and two-color mid IR pump-probe spectroscopy. 39 The temperature dependence of the vibrational lifetime has been explored, 40 its spectral features, 38,39 its dilution-dependence as well as its anisotropy 41 and the dynamics of ice in reverse micelles.…”

Section: Introductionmentioning

confidence: 99%

“…37 Previous nonlinear spectroscopic studies of ice have resolved the vibrational dynamics of ice Ih using hole burning 38 and two-color mid IR pump-probe spectroscopy. 39 The temperature dependence of the vibrational lifetime has been explored, 40 its spectral features, 38,39 its dilution-dependence as well as its anisotropy 41 and the dynamics of ice in reverse micelles. 42 One intriguing observation of previous pump-probe experiments were the extreme asymmetry in linewidth between the 0-1 and 1-2 transitions of the OH vibrator of HOD/D 2 O.…”

Section: Introductionmentioning

confidence: 99%

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Two-dimensional infrared spectroscopy of isotope-diluted ice Ih

Perakis

Widmer

Hamm

2011

The Journal of Chemical Physics

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We present experimental 2D IR spectra of isotope diluted ice Ih (i.e., the OH stretch mode of HOD in D2O and the OD stretch mode of HOD in H2O) at T = 80 K. The main spectral features are the extremely broad 1-2 excited state transition, much broader than the corresponding 0-1 groundstate transition, as well as the presence of quantum beats. We do not observe any inhomogeneous broadening that might be expected due to proton disorder in ice Ih. Complementary, we perform simulations in the framework of the Lippincott-Schroeder model, which qualitatively reproduce the experimental observations. We conclude that the origin of the observed line shape features is the coupling of the OH-vibrational coordinate with crystal phonons and explain the beatings as a coherent oscillation of the O⋅⋅⋅O hydrogen bond degree of freedom.

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Section: Resultssupporting

confidence: 79%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Two-dimensional infrared spectroscopy of isotope-diluted ice Ih

Perakis

Widmer

Hamm

2011

The Journal of Chemical Physics

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“…While crystalline ice Ih has been studied extensively also by nonlinear vibrational spectroscopic tools [23][24][25][26][27], to the best of our knowledge, no such measurements have ever been performed for amorphous ice. 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.…”

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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