Libration induced stretching mode excitation for pump-probe spectroscopy in pure liquid water

Amir, Wafa; Gallot, Guilhem; Hache, F.

doi:10.1063/1.1800952

Cited by 7 publications

(13 citation statements)

References 28 publications

(24 reference statements)

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“…This feature has been thoroughly studied recently. 19 It is therefore important to be able to extract the signal of the HCl/H 2 O solution from the background due to water. Such an extraction is not straightforward and requires a careful understanding of the origin of the signal in this binary mixture.…”

Section: A Experimental Setup and Proceduresmentioning

confidence: 99%

“…Therefore, the system has to be carefully analyzed to suppress the background signal of pure water from the signal measured with the protonated mixture. The following calculations take into account the unusual vibrational properties of pure water in this spectral domain, 19 where librational mode plays a major role. Pure water can be described using a four-level quantum system ͑see Fig.…”

Section: B Calculation Of Pump-probe Signal In Binary H 2 O / Hcl MImentioning

confidence: 99%

“…Cross sections for pure water are taken from previous work. 19 Cross sections for solute come from the experimental data. Figures 3 and 4 are calculated for a solute concentration of 1% in the number of molecules of hydrated proton with respect to the number of water molecules ͑0.5M͒.…”

Section: A Full Three-level Quantum System Simulationmentioning

confidence: 99%

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Time-resolved observation of the Eigen cation in liquid water

Amir

Gallot

Hache

et al. 2007

The Journal of Chemical Physics

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Experimental observation and time relaxation measurement of the hydrated proton Eigen form [H(3)O(+)(H(2)O)(3)] are presented here. Vibrational time-resolved spectroscopy is used with an original method of investigating the proton excess in water. The anharmonicity of the time-resolved spectra is characteristic of the Eigen-type proton geometry. Proton relaxation occurs in less than 200 fs. A calculation of the potential energy confirms the experimental result and the Eigen cation lifetime is in good agreement with previous molecular dynamics simulations.

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Section: A Experimental Setup and Proceduresmentioning

confidence: 99%

Section: B Calculation Of Pump-probe Signal In Binary H 2 O / Hcl MImentioning

confidence: 99%

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Time-resolved observation of the Eigen cation in liquid water

Amir

Gallot

Hache

et al. 2007

The Journal of Chemical Physics

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“…An important interaction determining the structure and functionality of numerous molecular systems in nature is hydrogen bonding. Nonlinear vibrational spectroscopy in both the frequency and the time domain has been used to investigate intramolecular 28–31 as well as intermolecular hydrogen bonds in dimers 32–39, small clusters 40, 41, or liquids 42–59. Formation of a hydrogen bond XH…Y between a hydrogen donor X and hydrogen acceptor Y leads to pronounced changes in the high‐frequency XH stretching vibrational spectrum 60.…”

Section: Introductionmentioning

confidence: 99%

Density functional theory simulations of two‐dimensional infrared spectra for hydrogen‐bonded acetic acid dimers

Dreyer

2005

Int J of Quantum Chemistry

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Two-dimensional coherent infrared spectra are simulated based on density functional theory calculations to analyze vibrational couplings in hydrogenbonded acetic acid dimers. Anharmonic sixth-order force fields covering up to threebody interactions are calculated for up to 11 normal modes. Three mechanisms for vibrational coupling within the two intermolecular hydrogen bonds are considered: anharmonic coupling of the high-frequency OOH stretching mode to low-frequency modes, Fermi resonance coupling the of OOH stretching mode to fingerprint mode combination tones, and a combination of both. Predicted coherent two-dimensional infrared spectra show distinct signatures for the different coupling mechanisms.

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“…As a result the fastest dynamics of water (500 nm thickness) at room temperature has now been determined with 70 fs time resolution. These recent experimental results on neat water emphasize the necessity of theoretical studies on the determination of the couplings of librational modes with the O−H stretching oscillator [194], as well as intermolecular resonant vibrational energy transfer [195,196], fluctuations of the hydrogen bond network of neat water [176,197], and reorientational dynamics [198]. 7.9).…”

Section: Coherent Response Of Neat Liquid Watermentioning

confidence: 92%

Vibrational dynamics of hydrogen bonds

Nibbering

Dreyer

Kühn

et al.

Analysis and Control of Ultrafast Photoinduced Reactions

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Hydrogen bonds are ubiquitous and of fundamental relevance in nature. Representing a local attractive interaction between a hydrogen donor and an adjacent acceptor group, they result in the formation of single or multiple local bonds with binding energies in the range from 4 to 50 kJ mol −1 , much weaker than a covalent bond, but stronger than most other intermolecular forces and thus decisive for structural and dynamical properties of a variety of molecular systems [1][2][3][4]. Disordered extended networks of intermolecular hydrogen bonds exist in liquids such as water and alcohols, determining to a large extent their unique physical and chemical properties. At elevated temperatures, such liquids undergo pronounced structural fluctuations on a multitude of time scales, due to the limited interaction strength. In contrast, well-defined molecular structures based on both intra-and intermolecular hydrogen bonds exist in polyatomic molecules, molecular dimers and pairs and -in particular -in macromolecules such as DNA and other biomolecular systems.Vibrational spectra of hydrogen-bonded systems reflect the local interaction strength and geometries as well as the dynamics and couplings of nuclear motions. Steady-state infrared and Raman spectra have been measured and modeled theoretically for numerous systems, making vibrational spectroscopy one of the major tools of hydrogen bond research [5]. In many cases, however, conclusive information on structure and -in particular -dynamics is difficult to derive from stationary spectra which average over a multitude of molecular geometries and time scales. In recent years, vibrational spectroscopy in the ultrafast time domain [6] is playing an increasingly important role for observing hydrogen bond dynamics in real-time, for separating different types of molecular couplings, and for determining them in a quantitative way [7]. Using such

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Libration induced stretching mode excitation for pump-probe spectroscopy in pure liquid water

Cited by 7 publications

References 28 publications

Time-resolved observation of the Eigen cation in liquid water

Time-resolved observation of the Eigen cation in liquid water

Density functional theory simulations of two‐dimensional infrared spectra for hydrogen‐bonded acetic acid dimers

Vibrational dynamics of hydrogen bonds

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