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.; O’Connor, Michael; McIntosh-Smith, Simon; Johnson, Graham T.; Hohenstein, Edward G.; Manby, Fred R.; Glowacki, David R.; Martinez, Todd J.

doi:10.1039/c7cp00492c

Title: Atomistic non-adiabatic dynamics of the LH2 complex with a GPU-accelerated ab initio exciton model

Journal Article · Tue Mar 28 00:00:00 EDT 2017 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c7cp00492c· OSTI ID:1369335

Sisto, Aaron ^[1]; Stross, Clem ^[2];

^[3]; O’Connor, Michael ^[4]; McIntosh-Smith, Simon ^[5]; Johnson, Graham T. ^[6]; Hohenstein, Edward G. ^[7]; Manby, Fred R. ^[2];

^[4];

^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Stanford Univ., CA (United States)
Univ. of Bristol (United Kingdom). School of Chemistry
Univ. of Bristol (United Kingdom). School of Chemistry, School of Biochemistry
Univ. of Bristol (United Kingdom). School of Chemistry, Dept. of Computer Science
Univ. of Bristol (United Kingdom). Dept. of Computer Science
Univ. of California, San Francisco, CA (United States). California Inst. for Quantitative Biosciences (QB3), Dept. of Bioengineering and Therapeutic Sciences
City College of New York, NY (United States). Dept. of Chemistry and Biochemistry

We recently outlined an efficient multi-tiered parallel ab initio excitonic framework that utilizes time dependent density functional theory (TDDFT) to calculate ground and excited state energies and gradients of large supramolecular complexes in atomistic detail – enabling us to undertake non-adiabatic simulations which explicitly account for the coupled anharmonic vibrational motion of all the constituent atoms in a supramolecular system. Here we apply that framework to the 27 coupled bacterio-chlorophyll-a chromophores which make up the LH2 complex, using it to compute an on-the-fly nonadiabatic surface-hopping (SH) trajectory of electronically excited LH2. Part one of this article is focussed on calibrating our ab initio exciton Hamiltonian using two key parameters: a shift δ, which corrects for the error in TDDFT vertical excitation energies; and an effective dielectric constant ε, which describes the average screening of the transition-dipole coupling between chromophores. Using snapshots obtained from equilibrium molecular dynamics simulations (MD) of LH2, we tune the values of both δ and ε through fitting to the thermally broadened experimental absorption spectrum, giving a linear absorption spectrum that agrees reasonably well with experiment. In part two of this article, we construct a time-resolved picture of the coupled vibrational and excitation energy transfer (EET) dynamics in the sub-picosecond regime following photo-excitation. Assuming Franck–Condon excitation of a narrow eigenstate band centred at 800 nm, we use surface hopping to follow a single nonadiabatic dynamics trajectory within the full eigenstate manifold. Consistent with experimental data, this trajectory gives timescales for B800→B850 population transfer (τ_B800→B850) between 650–1050 fs, and B800 population decay (τ_800→) between 10–50 fs. The dynamical picture that emerges is one of rapidly fluctuating LH2 eigenstates that are delocalized over multiple chromophores and undergo frequent crossing on a femtosecond timescale as a result of the atomic vibrations of the constituent chromophores. The eigenstate fluctuations arise from disorder that is driven by vibrational dynamics with multiple characteristic timescales. The scalability of our ab initio excitonic computational framework across massively parallel architectures opens up the possibility of addressing a wide range of questions, including how specific dynamical motions impact both the pathways and efficiency of electronic energy-transfer within large supramolecular systems.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC02-76SF00515; ACI-1429830

OSTI ID:: 1369335

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Vol. 19, Issue 23; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 55 works

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Insights for Light-Driven Molecular Devices from ab initio Multiple Spawning Excited-State Dynamics of Organic and Biological Chromophores Martinez, Todd J. ChemInform, Vol. 37, Issue 18 https://doi.org/10.1002/chin.200618276	journal	May 2006
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Structure of a cyanobacterial photosystem I surrounded by octadecameric IsiA antenna proteins Akita, Fusamichi; Nagao, Ryo; Kato, Koji Communications Biology, Vol. 3, Issue 1 https://doi.org/10.1038/s42003-020-0949-6	journal	May 2020
Calculation of pigment transition energies in the FMO protein: From simplicity to complexity and back Adolphs, Julian; Müh, Frank; Madjet, Mohamed El-Amine Photosynthesis Research, Vol. 95, Issue 2-3 https://doi.org/10.1007/s11120-007-9276-8	journal	October 2007
Atomistic study of energy funneling in the light-harvesting complex of green sulfur bacteria Huh, Joonsuk; Saikin, Semion K.; Brookes, Jennifer C. arXiv https://doi.org/10.48550/arxiv.1307.0886	text	January 2013

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Double‐buffered, heterogeneous CPU + GPU integral digestion algorithm for single‐excitation calculations involving a large number of excited states Morrison, Adrian F.; Epifanovsky, Evgeny; Herbert, John M. Journal of Computational Chemistry, Vol. 39, Issue 26 https://doi.org/10.1002/jcc.25531	journal	October 2018
An efficient approximate algorithm for nonadiabatic molecular dynamics Hanasaki, Kota; Kanno, Manabu; Niehaus, Thomas A. The Journal of Chemical Physics, Vol. 149, Issue 24 https://doi.org/10.1063/1.5046757	journal	December 2018
Exciton transport in the PE545 complex: insight from atomistic QM/MM-based quantum master equations and elastic network models Pouyandeh, Sima; Iubini, Stefano; Jurinovich, Sandro Physical Biology, Vol. 14, Issue 6 https://doi.org/10.1088/1478-3975/aa90ea	journal	November 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
Exciton transport in the PE545 complex: insight from atomistic QM/MM-based quantum master equations and elastic network models Pouyandeh, Sima; Iubini, Stefano; Jurinovich, Sandro arXiv https://doi.org/10.48550/arxiv.1706.01306	text	January 2017
Delocalized excitons in natural light harvesting complexes Jang, Seogjoo J.; Mennucci, Benedetta arXiv https://doi.org/10.48550/arxiv.1804.09711	text	January 2018
Quantum Computation of Electronic Transitions using a Variational Quantum Eigensolver Parrish, Robert M.; Hohenstein, Edward G.; McMahon, Peter L. arXiv https://doi.org/10.48550/arxiv.1901.01234	text	January 2019
Simple Quantum Dynamics with Thermalization Jansen, Thomas L. C. The Journal of Physical Chemistry A, Vol. 122, Issue 1 https://doi.org/10.1021/acs.jpca.7b10380	journal	December 2017

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