Molecular Level Design Principle behind Optimal Sizes of Photosynthetic LH2 Complex: Taming Disorder through Cooperation of Hydrogen Bonding and Quantum Delocalization

Jang, Seogjoo; Rivera, Eva; Montemayor, Daniel

doi:10.1021/acs.jpclett.5b00078

Molecular Level Design Principle behind Optimal Sizes of Photosynthetic LH2 Complex: Taming Disorder through Cooperation of Hydrogen Bonding and Quantum Delocalization

Journal Article · Fri Feb 27 00:00:00 EST 2015 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.5b00078· OSTI ID:1753985

Jang, Seogjoo ^[1]; Rivera, Eva ^[2]; Montemayor, Daniel ^[2]

City Univ. of New York (CUNY), NY (United States); Queens College, City University of New York
City Univ. of New York (CUNY), NY (United States)

Here we discuss the light harvesting 2 (LH2) antenna complex from purple photosynthetic bacteria is an efficient natural excitation energy carrier with well-known symmetric structure, but the molecular level design principle governing its structure-function relationship is unknown. Our all-atomistic simulations of nonnatural analogues of LH2 as well as those of a natural LH2 suggest that nonnatural sizes of LH2-like complexes could be built. However, stable and consistent hydrogen bonding (HB) between bacteriochlorophyll and the protein is shown to be possible only near naturally occurring sizes, leading to significantly smaller disorder than for nonnatural ones. Extensive quantum calculations of intercomplex exciton transfer dynamics, sampled for a large set of disorder, reveal that taming the negative effect of disorder through a reliable HB as well as quantum delocalization of the exciton is a critical mechanism that makes LH2 highly functional, which also explains why the natural sizes of LH2 are indeed optimal.

View Accepted Manuscript (DOE)

Research Organization:: City Univ. of New York (CUNY), NY (United States)

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

Grant/Contract Number:: SC0001393

OSTI ID:: 1753985

Report Number(s):: DOE-Queens-1393-14

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 6 Vol. 6; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Atomistic non-adiabatic dynamics of the LH2 complex with a GPU-accelerated ab initio exciton model Sisto, Aaron; Stross, Clem; van der Kamp, Marc W. Physical Chemistry Chemical Physics, Vol. 19, Issue 23 https://doi.org/10.1039/c7cp00492c	journal	January 2017
Delocalized excitons in natural light-harvesting complexes Jang, Seogjoo J.; Mennucci, Benedetta Reviews of Modern Physics, Vol. 90, Issue 3 https://doi.org/10.1103/revmodphys.90.035003	journal	August 2018
Delocalized excitons in natural light harvesting complexes Jang, Seogjoo J.; Mennucci, Benedetta arXiv https://doi.org/10.48550/arxiv.1804.09711	text	January 2018

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Molecular Level Design Principle behind Optimal Sizes of Photosynthetic LH2 Complex: Taming Disorder through Cooperation of Hydrogen Bonding and Quantum Delocalization

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