Excitonic Energy Landscape of the Y16F Mutant of the Chlorobium tepidum Fenna–Matthews–Olson (FMO) Complex: High Resolution Spectroscopic and Modeling Studies

Khmelnitskiy, Anton; Saer, Rafael G.; Blankenship, Robert E.; Jankowiak, Ryszard

doi:10.1021/acs.jpcb.7b11763

Title: Excitonic Energy Landscape of the Y16F Mutant of the Chlorobium tepidum Fenna–Matthews–Olson (FMO) Complex: High Resolution Spectroscopic and Modeling Studies

Journal Article · Mon Mar 19 00:00:00 EDT 2018 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.7b11763· OSTI ID:1470597

Khmelnitskiy, Anton ^[1]; Saer, Rafael G. ^[2]; Blankenship, Robert E. ^[2];

^[3]

Kansas State Univ., Manhattan, KS (United States). Dept. of Chemistry
Washington Univ., St. Louis, MO (United States). Dept. of Biology and Chemistry
Kansas State Univ., Manhattan, KS (United States). Dept. of Chemistry, and Dept. of Physics

We report high-resolution (low-temperature) absorption, emission, and nonresonant/resonant hole-burned (HB) spectra and results of excitonic calculations using a non-Markovian reduced density matrix theory (with an improved algorithm for parameter optimization in heterogeneous samples) obtained for the Y16F mutant of the Fenna–Matthews–Olson (FMO) trimer from the green sulfur bacterium Chlorobium tepidum. We show that the Y16F mutant is a mixture of FMO complexes with three independent low-energy traps (located near 817, 821, and 826 nm), in agreement with measured composite emission and HB spectra. Two of these traps belong to mutated FMO subpopulations characterized by significantly modified low-energy excitonic states. Hamiltonians for the two major subpopulations (Sub₈₂₁ and Sub₈₁₇) provide new insight into extensive changes induced by the single-point mutation in the vicinity of BChl 3 (where tyrosine Y16 was replaced with phenylalanine F16). The average decay time(s) from the higher exciton state(s) in the Y16F mutant depends on frequency and occurs on a picosecond time scale.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001035

OSTI ID:: 1470597

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 122, Issue 14; Related Information: PARC partners with Washington University in St. Louis (lead); University of California, Riverside; University of Glasgow, UK; Los Alamos National Laboratory; University of New Mexico; New Mexico Corsortium; North Carolina State University; Northwestern University; Oak Ridge National Laboratory; University of Pennsylvania; Sandia National Laboratories; University of Sheffield, UK; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 8 works

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Title: Excitonic Energy Landscape of the Y16F Mutant of the Chlorobium tepidum Fenna–Matthews–Olson (FMO) Complex: High Resolution Spectroscopic and Modeling Studies

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