Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 130, Issue 23, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.3155372
Keywords
dipole coupling; excited states; fluorescence; Markov processes; nonradiative transitions; quantum theory; radiative lifetimes; wave functions
Funding
- U. S. Department of Energy [DE-AC02-05CH1123, DE-AC03-76SF000098]
- Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences
- JSPS Postdoctoral Fellowship for Research Abroad
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A new quantum dynamic equation for excitation energy transfer is developed which can describe quantum coherent wavelike motion and incoherent hopping in a unified manner. The developed equation reduces to the conventional Redfield theory and Foumlrster theory in their respective limits of validity. In the regime of coherent wavelike motion, the equation predicts several times longer lifetime of electronic coherence between chromophores than does the conventional Redfield equation. Furthermore, we show quantum coherent motion can be observed even when reorganization energy is large in comparison to intersite electronic coupling (the Foumlrster incoherent regime). In the region of small reorganization energy, slow fluctuation sustains longer-lived coherent oscillation, whereas the Markov approximation in the Redfield framework causes infinitely fast fluctuation and then collapses the quantum coherence. In the region of large reorganization energy, sluggish dissipation of reorganization energy increases the time electronic excitation stays above an energy barrier separating chromophores and thus prolongs delocalization over the chromophores.
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