Role of Vibrational Dynamics on Excited-State Electronic Coherence in a Binuclear Platinum Complex

Joseph J. Radler, David B. Lingerfelt, Felix N. Castellano, Lin X. Chen, Xiaosong Li*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

9 Scopus citations


Long-lived quantum coherence between excited electronic states can enable highly efficient energy and charge transport processes in chemical systems. Recent pump-probe experiments on binuclear platinum complexes identified persistent, periodic beating of transient absorption anisotropy signals, indicating long excited-state coherence lifetimes. Our previous simulations of the electronic dynamics of these complexes indicate that coherence lifetimes are sensitive to the balance between competitive electronic couplings. The complexes with shorter Pt-Pt distances underwent no appreciable dephasing in the limit of static nuclei, motivating the inclusion of nuclear motion into our simulations. The tert-butyl-substituted complex is studied in this work using the Ehrenfest method for mixed quantum-classical dynamics to investigate the role of vibrational dynamics on a complex shown to support long coherence lifetimes. Results indicate that the inclusion of excited-state vibrations drives a rapid collapse of the two-state coherence prior to the experimentally determined intersystem crossing. This further suggests singlet excited-state coherences may not be prerequisites for long-lived triplet coherences.

Original languageEnglish (US)
Pages (from-to)5071-5077
Number of pages7
JournalJournal of Physical Chemistry A
Issue number23
StatePublished - Jun 14 2018

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry


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