4.7 Article

The role of resonant nuclear modes in vibrationally assisted energy transport: The LHCII complex

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 153, Issue 4, Pages -

Publisher

AMER INST PHYSICS
DOI: 10.1063/5.0012420

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Funding

  1. U.S. Department of Energy, Office of Science, Chemical Sciences, Geosciences, and Biosciences Division
  2. U.S. Department of Energy, Office of Science User Facility [DE-AC02-05CH11231]

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In this paper, we discuss the explicit role of resonant nuclear/vibrational modes in mediating energy transport among chlorophylls in the Light-harvesting Complex II (LHCII), the major light-harvesting complex in green plants. The vibrational modes are considered to be resonant/quasi-resonant with the energy gap between electronic excitons. These resonant vibrations, along with the remaining nuclear degrees of freedom, constitute the environment/bath to the electronically excited system and contribute to two major phenomena: (a) decoherence and (b) incoherent phonon-mediated population relaxation. In this work, we explore the subtle interplay among the electronic excitation, the resonant vibrations, and the environment in dictating environment assisted quantum transport in light-harvesting complexes. We conclusively show that resonant vibrations are capable of boosting the incoherent population relaxation pathways and cause rapid decoherence.

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