Ultrafast dynamics of hydrogen bonds directly observed by time-resolved infrared spectroscopy

Graener, H.; Ye, T. Q.; Laubereau, A.

doi:10.1063/1.455849

Cited by 183 publications

(160 citation statements)

References 12 publications

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“…The small anisotropies of the experimental signals ͑aϭ1.4 for E p ϭ140Ϯ30 J and aϭ1. 6 for E p ϭ50Ϯ10 J͒ compared to the anisotropies in the calculations ͑aϭ2.32 and aϭ2.75, respectively͒ thus indicate that part of the excitations randomize faster than our 25 ps pulses during the pumping process.…”

Section: E Polarization Diffusionmentioning

confidence: 99%

“…These experiments have provided insight into intramolecular and intermolecular energy transfer processes in the liquid phase 2-5,8 -13 as well as in the dissociation dynamics of hydrogen bonds. 6,7,14 To investigate the vibrational coupling between adsorbates and surfaces, the same time-resolved techniques have been applied to adsorbates. [15][16][17][18][19][20][21][22][23][24][25][26][27] The population dynamics of molecular vibrations in solid matrices containing some disorder 28 -33 have received less attention so far.…”

Section: Introductionmentioning

confidence: 99%

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Direct vibrational energy transfer in zeolites

Brugmans

Bakker

Lagendijk

1996

The Journal of Chemical Physics

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Direct vibrational energy transfer in zeolitesBrugmans, M.J.P.; Bonn, M.; Bakker, H.J.; Lagendijk, A. Published in:Journal of Chemical Physics DOI:10.1063/1.470876 Link to publication Citation for published version (APA):Brugmans, M. J. P., Bonn, M., Bakker, H. J., & Lagendijk, A. (1996). Direct vibrational energy transfer in zeolites. Journal of Chemical Physics, 104, 64-84. DOI: 10.1063/1.470876 General rightsIt is not permitted to download or to forward/distribute the text or part of it without the consent of the author(s) and/or copyright holder(s), other than for strictly personal, individual use, unless the work is under an open content license (like Creative Commons). Disclaimer/Complaints regulationsIf you believe that digital publication of certain material infringes any of your rights or (privacy) interests, please let the Library know, stating your reasons. In case of a legitimate complaint, the Library will make the material inaccessible and/or remove it from the website. Please Ask the Library: http://uba.uva.nl/en/contact, or a letter to: Library of the University of Amsterdam, Secretariat, Singel 425, 1012 WP Amsterdam, The Netherlands. You will be contacted as soon as possible. With two-color picosecond infrared laser spectroscopy the dynamics of O-H and O-D stretch vibrations in zeolites are investigated. Zeolites appear to be good model systems to study transfer of vibrational energy in a solid. For the O-D vibrations, transient spectral holes are burnt in the inhomogeneously broadened absorption bands by saturating the absorption with a strong pump pulse. From the spectral hole widths the homogeneous absorption linewidths are obtained. The excited population lifetimes are determined using a time-resolved pump-probe technique, and in combination with the homogeneous linewidth the pure dephasing time is revealed as well. For high concentrations of O-H oscillators the vibrational stretch excitations are found to diffuse spectrally through the inhomogeneous absorption band. This spectral diffusion process is explained by direct site-to-site transfer of the excitations due to dipole-dipole coupling ͑Förster transfer͒. The dependences of the transient spectral signals on oscillator concentration and the results of one-color polarization resolved experiments confirm this explanation. The spectral transients are satisfactorily described by simulations in which the site-to-site transfer by dipole-dipole coupling is taken into account.

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Section: E Polarization Diffusionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Direct vibrational energy transfer in zeolites

Brugmans

Bakker

Lagendijk

1996

The Journal of Chemical Physics

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“…[29][30][31][32][33]66 The main feature of the latter system is that vibrational relaxation of the excited OH (OD) stretching mode results in ultrafast breaking of the hydrogen bond at a time scale shorter than 2 ps. The broken hydrogen bond recovers at a time scale of ∼10 to 20 ps after which the temperature equilibration of the sample settles up.…”

Section: Pathways For Vibrational Energy Relaxationmentioning

confidence: 99%

“…This process is analogous to the theoretically predicted and experimentally observed VER in alcohols, where energy transfer directly to the hydrogen bond leads to its subsequent rupture. [27][28][29][30][31][32][33] The OH-stretching mode dynamics in heavy water has also been studied by an IR pump visible probe pulse technique. 2,23 In this method, a femtosecond IR pump pulse excites the vibrational transition while the response of the system is monitored via spontaneous Raman scattering induced by a visible probe pulse.…”

Section: Introductionmentioning

confidence: 99%

Hydrogen Bonding and Vibrational Energy Relaxation in Water−Acetonitrile Mixtures

et al. 2004

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We present a study of the effect of hydrogen bonding on vibrational energy relaxation of the OH-stretching mode in pure water and in water-acetonitrile mixtures. The extent of hydrogen bonding is controlled by dissolving water at various concentrations in acetonitrile. Infrared frequency-resolved pump-probe measurements were used to determine the relative abundance of hydrogen-bonded versus non-hydrogen-bonded OH bonds in water-acetonitrile mixtures. Our data show that the main pathway for vibrational relaxation of the OH-stretching mode in pure water involves the overtone of the bending mode. Hydrogen bonding is found to accelerate the population relaxation from 3 ps in dilute solutions to 700 fs in neat water, as a result of increasing overlap between donor and acceptor modes. Hydroxyl groups that initially are not hydrogen bonded have two relaxation pathways: by direct nonresonant relaxation to the bending mode with a time constant of 12 ps or by making a hydrogen bond to a neighboring water molecule first (∼2 ps) and then relaxing as a hydrogen-bonded OH oscillator.

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“…Infrared spectroscopy thus represents the most popular experimental methods to study the microscopic structure of the hydrogen bonded systems. [2][3][4][5][6][7][8] The neutron-or x-ray diffraction techniques [9][10][11][12][13] and the dielectric relaxation 14,15 can provide further information about the structure and dynamics of the hydrogen bonded systems. Indirect information about the hydrogen bonding can be deduced also from macroscopic properties (e.g., from the viscosity measurements or PvT behaviour and phase equilibrium data).…”

Section: Introductionmentioning

confidence: 99%

Size distribution of associated clusters in liquid alcohols: Interpretation of simulation results in the frame of SAFT approach

Janeček

Paricaud

2013

The Journal of Chemical Physics

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The size distribution and topology of associated clusters for primary alcohols is studied using molecular dynamics simulations. Liquid ethanol, propanol, butanol, hexanol, and octanol are simulated at pressure P = 1 bar and temperatures T = 300 K, T = 350 K, and T = 400 K. The fractions of molecules with different sets of hydrogen bonded partners, the size of associated cluster and the site-site distribution functions between atoms participating on hydrogen bonding are extracted from simulated trajectories. For all alcohols longer than ethanol, the length of the alkyl chain has only a marginal effect on the association. Consequently, related properties like coordination numbers of hydroxyl group, size distribution of associates, or fractions of differently coordinated alcohol molecules are independent on the molecular size. Although we employed a force-field without involved polarizability, we observe a positive cooperativity of hydrogen bonding simply as a consequence of steric and electrostatic interactions. The size and topology of associates is analyzed within the frame of 3B model of statistical association fluid theory. Although this approach enables good thermodynamic description of systems containing associating compounds, several insufficiencies appear in the description at molecular level. © 2013 AIP Publishing LLC.[http://dx.doi.org/10.1063/1.4827107]

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Ultrafast dynamics of hydrogen bonds directly observed by time-resolved infrared spectroscopy

Cited by 183 publications

References 12 publications

Direct vibrational energy transfer in zeolites

Direct vibrational energy transfer in zeolites

Hydrogen Bonding and Vibrational Energy Relaxation in Water−Acetonitrile Mixtures

Size distribution of associated clusters in liquid alcohols: Interpretation of simulation results in the frame of SAFT approach

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