Multireference Excitation Energies for Bacteriochlorophylls A within Light Harvesting System 2

Journal of Chemical Theory and Computation
André AndaLuca De Vico

Abstract

Light-harvesting system 2 (LH2) of purple bacteria is one of the most popular antenna complexes used to study Nature's way of collecting and channeling solar energy. The dynamics of the absorbed energy is probed by ultrafast spectroscopy. Simulation of these experiments relies on fitting a range of parameters to reproduce the spectra. Here, we present a method that can determine key parameters to chemical accuracy. These will eliminate free variables in the modeling, thus reducing the problem. Using MS-RASPT2/RASSCF calculations, we compute excitation energies and transition dipole moments of all bacteriochlorophylls in LH2. We find that the excitation energies vary among the bacteriochlorophyll monomers and that they are regulated by the curvature of the macrocycle ring and the dihedral angle of an acetyl moiety. Increasing the curvature lifts the ground state energy, which causes a red shift of the excitation energy. Increasing the torsion of the acetyl moiety raises the excited state energy, resulting in a blue shift of the excitation energy. The obtained results mark a giant leap for multiconfigurational multireference quantum chemical methods in the photochemistry of biological systems, which can prove instrumental in expo...Continue Reading

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Mar 10, 2016·Chemical Reviews·Carles Curutchet, Benedetta Mennucci
Jun 9, 2016·Journal of Chemical Theory and Computation·Dongxia MaLaura Gagliardi
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Jun 28, 2019·The Journal of Physical Chemistry. a·André AndaLuca De Vico
Nov 30, 2021·Physical Chemistry Chemical Physics : PCCP·Kwang Hyun Cho, Young Min Rhee

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