This document is confidential and is proprietary to the American Chemical Society and its authors. Do not copy or disclose without written permission. If you have received this item in error, notify the sender and delete all copies. Optical Excitations of Chlorophyll a and Chlorophyll b Monomers and Dimers Journal: Journal of Chemical Theory and Computation Manuscript ID Draft Manuscript Type: Article Date Submitted by the Author: n/a Complete List of Authors: Preciado-Rivas, María; Yachay Tech University, School of Physical Sciences and Nanotechnology Mowbray, Duncan; Yachay Tech University, School of Physical Sciences and Nanotechnology Larsen, Ask; Universidad del Pais Vasco, Nano-bio spectroscopy group, Departamento de Fisica de Materiales Milne, Bruce; University of Coimbra, Coimbra Chemistry Center, Department of Chemistry ACS Paragon Plus Environment Journal of Chemical Theory and Computation
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This document is confidential and is proprietary to the American Chemical Society and its authors. Do not copy or disclose without written permission. If you have received this item in error, notify the sender and delete all copies.
Optical Excitations of Chlorophyll a and Chlorophyll b
Monomers and Dimers
Journal: Journal of Chemical Theory and Computation
Manuscript ID Draft
Manuscript Type: Article
Date Submitted by the Author: n/a
Complete List of Authors: Preciado-Rivas, María; Yachay Tech University, School of Physical Sciences and Nanotechnology Mowbray, Duncan; Yachay Tech University, School of Physical Sciences and Nanotechnology Larsen, Ask; Universidad del Pais Vasco, Nano-bio spectroscopy group, Departamento de Fisica de Materiales Milne, Bruce; University of Coimbra, Coimbra Chemistry Center, Department of Chemistry
ACS Paragon Plus Environment
Journal of Chemical Theory and Computation
Optical Excitations of Chlorophyll a and Chlorophyll b
Monomers and Dimers
María Rosa Preciado-Rivas,† Duncan John Mowbray,∗,†,‡ Ask Hjorth Larsen,‡ and Bruce Forbes Milne¶,§,‡
† School of Physical Sciences and Nanotechnology, Yachay Tech University, Urcuquí 100119, Ecuador‡ Nano-Bio Spectroscopy Group and ETSF Scientific Development Centre, Departamento de Física de Materiales, Universidad del PaísVasco UPV/EHU, E-20018 San Sebastián, Spain¶ Coimbra Chemistry Center, Department of Chemistry, University of Coimbra, Rua Larga, 3004-535 Coimbra, Portugal§ CFisUC, Department of Physics, University of Coimbra, Rua Larga, 3004-516 Coimbra, Portugal
ABSTRACT: A necessary first step in the development of technologies such as artificial photosynthesis is understanding the photoexcitation
process within the basic building blocks of naturally-occuring light harvesting complexes (LHCs). The most important of these building
blocks in biological LHCs such as LHC II from green plants are the chlorophyll a (Chl a) and chlorophyll b (Chl b) chromophores dispersed
throughout the protein matrix. Efforts are still hampered by the lack of economical computational methods that are able to describe optical
absorption in large biomolecules with sufficient accuracy. In this work we employ a highly efficient localized basis set representation of
the Kohn–Sham (KS) wave functions at the density functional theory (DFT) level to perform time dependent density functional theory
(TDDFT) real time and frequency domain calculations of the optical absorption spectra of Chl a and Chl b monomers and dimers. We find
our TDDFT calculations using linear combinations of atomic orbitals (LCAO) reproduce results obtained with a plane wave (PW) and real
space (RS) representations of the KS wave functions, but with a significant reduction in computational effort. This work opens the path to
first principles calculations of optical excitations in macromolecular systems.
2020) and the Donostia International Physics Centre for financial
support. We acknowledge computational time from the Empresa
Pública Yachay on the “Supercomputador Quinde”.
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