Journal article
Direct Dynamics Studies of a Binuclear Metal Complex in Solution: The Interplay Between Vibrational Relaxation, Coherence, and Solvent Effects
Center for Atomic-scale Materials Design, Centers, Technical University of Denmark1
Department of Chemistry, Technical University of Denmark2
Physical and Biophysical Chemistry, Department of Chemistry, Technical University of Denmark3
Department of Physics, Technical University of Denmark4
NanoChemistry, Department of Chemistry, Technical University of Denmark5
Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark6
By using a newly implemented QM/MM multiscale MD method to simulate the excited state dynamics of the Ir2(dimen)42+ (dimen = 1,8-diisocyano-p-menthane) complex, we not only report on results that support the two experimentally observed coherent dynamical modes in the molecule but also reveal a third mode, not distinguishable by spectroscopic methods.
We directly follow the channels of energy dissipation to the solvent and report that the main cause for coherence decay is the initial wide range of configurations in the excited state population. We observe that the solvent can actually extend the coherence lifetime by blocking channels for intramolecular vibrational energy redistribution (IVR).
| Language: | English |
|---|---|
| Year: | 2014 |
| Pages: | 2414-2418 |
| ISSN: | 19487185 |
| Types: | Journal article |
| DOI: | 10.1021/jz500850s |
| ORCIDs: | Dohn, Asmus Ougaard , Kjær, Kasper Skov , Nielsen, Martin Meedom , Jacobsen, Karsten Wedel , Henriksen, Niels Engholm and Møller, Klaus Braagaard |
