The vibrational dynamics of theOH 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 thewater 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.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:21498 |
| Date | 19 June 2018 |
| Creators | Heine, Thomas, Hutzler, Daniel, Brunner, Christian, Petkov, Petko St., Fischer, Sighart F., Riedle, Eberhard, Kienberger, Reinhard, Iglev, Hristo |
| Publisher | AIP Publishing |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 0021-9606, 054307 |
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