期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 121, 期 9, 页码 1932-1939出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.6b12099
关键词
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资金
- Ultrafast Initiative of the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, through Argonne National Laboratory [DE-AC02-06CH11357]
- National Science Foundation [CHE-1565520, CHE-1363007, CHE-1362942]
- Student Technology Fee
- State of Washington through the University of Washington Clean Energy Institute
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1362942] Funding Source: National Science Foundation
Materials and molecular systems exhibiting long-lived electronic coherence can facilitate coherent transport, opening the door to efficient charge and energy transport beyond traditional methods. Recently, signatures of a possible coherent, recurrent electronic motion were identified in femtosecond pumpprobe spectroscopy experiments on a binuclear platinum complex, where a persistent periodic beating in the transient absorption signals anisotropy was observed. In this study, we investigate the excitonic dynamics that underlie the suspected electronic coherence for a series of binuclear platinum complexes exhibiting a range of interplatinum distances. Results suggest that the long-lived coherence can only result when competitive electronic couplings are in balance. At longer Pt-Pt distances, the electronic couplings between the two halves of the binuclear system weaken, and exciton localization and recombination is favored on short time scales. For short Pt-Pt distances, electronic couplings between the states in the coherent superposition are stronger than the coupling with other excitonic states, leading to long-lived coherence.
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