Enhancement of the vibrational relaxation rate of surface hydroxyls through hydrogen bonds with adsorbates

Bonn, Mischa; Brugmans, Mjp Marco; Kleyn, A.W.; Santen, RA Rutger van

doi:10.1016/0009-2614(94)01411-n

Cited by 33 publications

(19 citation statements)

References 13 publications

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“…Both the center frequency of the absorption band (see inset, Fig. 1) and the population lifetime T 1 of 45 ps are the same for both O-D groups [19] (as we observed previously for the nondeuterated OH · · · O latt and OH · · · N 2 groups [20]) , implying an equal hydrogen-bond strength [20,21]. For the OH · · · O latt groups, the pump pulse burns a hole in the absorption spectrum (see also Ref.…”

Section: Vibrational Dephasing Mechanisms In Hydrogen-bonded Systemssupporting

confidence: 81%

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Vibrational Dephasing Mechanisms in Hydrogen-Bonded Systems

et al. 1996

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Section: Vibrational Dephasing Mechanisms In Hydrogen-bonded Systemssupporting

confidence: 81%

“…[16]), whereas, remarkably, for the OD · · · N 2 groups the whole absorption band decreases in amplitude. We have shown previously that the hydrogen bond between the O-D group and the adsorbate remains intact upon vibrational relaxation [20].…”

Section: Vibrational Dephasing Mechanisms In Hydrogen-bonded Systemsmentioning

confidence: 93%

Vibrational Dephasing Mechanisms in Hydrogen-Bonded Systems

et al. 1996

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“…In this context the population dynamics of hydroxyl vibrations in zeolites have been studied in the last few years. [35][36][37][38][39][40][41][42][43] Acid zeolites are industrially important materials because they are widely exploited as catalysts. 44 Catalytically active sites in the porous zeolite framework are the hydroxyl groups, which are found near aluminum atoms in the crystalline alumino-silicate structure.…”

Section: Introductionmentioning

confidence: 99%

“…The time-resolved infrared saturation experiments provided new information on the different hydroxyl groups and hydrogen bonding to the lattice, 37,38 on the deexcitation mechanism, 42 and on interactions with adsorbates. 43 Besides contributing to the insight in the molecular structure, these studies are the very first step in revealing the reaction dynamics on a molecular scale, since the coordinate of the hydroxyl stretch vibration is parallel with the reaction coordinate for the catalytic proton donation. 45 The main objective of the present study is to gain insight into population dynamics of molecular vibrations embedded in a crystalline host, for which the zeolites have proven to be good model systems.…”

Section: Introductionmentioning

confidence: 99%

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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“…Knowledge of the interaction between BrOnsted hydroxyls and adsorbed species is therefore essential for a fundamental understanding of zeolite catalysis. Time-resolved infrared spectroscopy has proven to be a powerful tool in the investigation of the vibrational dynamics of the zeolite hydroxyl [4][5][6][7][8][9][10][11][12][13][14][15][16][17][18]. This paper reports on a time-resolved infrared investigation of the effect of simple adsorbates on the dynamic properties of the catalytic BrOnsted hydroxyl.…”

Section: Zeolite Samplesmentioning

confidence: 99%