Dynamics of the OH stretching mode in crystalline Ba(ClO4)2·3H2O

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Daniel Hutzler - , Technical University of Munich (Author)
  • Christian Brunner - , Technical University of Munich (Author)
  • Petko St Petkov - , Leipzig University (Author)
  • Thomas Heine - , Leipzig University (Author)
  • Sighart F. Fischer - , Technical University of Munich (Author)
  • Eberhard Riedle - , Ludwig Maximilian University of Munich (Author)
  • Reinhard Kienberger - , Technical University of Munich (Author)
  • Hristo Iglev - , Technical University of Munich (Author)

Abstract

The vibrational dynamics of the OH stretching mode in Ba(ClO4)2 trihydrate are investigated by means of femtosecond infrared spectroscopy. The sample offers plane cyclic water trimers in the solid phase that feature virtually no hydrogen bond interaction between the water molecules. Selective excitation of the symmetric and asymmetric stretching leads to fast population redistribution, while simultaneous excitation yields quantum beats, which are monitored via a combination tone that dominates the overtone spectrum. The combination of steady-state and time-resolved spectroscopy with quantum chemical simulations and general theoretical considerations gives indication of various aspects of symmetry breakage. The system shows a joint population lifetime of 8 ps and a long-lived coherence between symmetric and asymmetric stretching, which decays with a time constant of 0.6 ps.

Details

Original languageEnglish
Article number054307
JournalJournal of Chemical Physics
Volume148
Issue number5
Publication statusPublished - 7 Feb 2018
Peer-reviewedYes
Externally publishedYes

External IDs

PubMed 29421900