We develop a cross-disciplinary approach to analytically compute optical response functions of open macromolecular systems by exploiting the mathematical formalism of quantum field theory (QFT). Indeed, the entries of the density matrix for the electronic excitations interacting with their open dissipative environment are mapped into vacuum-to-vacuum Green’s functions in a fictitious relativistic closed quantum system. We show that by re-summing appropriate self-energy diagrams in this dual QFT, it is possible to obtain analytic expressions for the response functions in Mukamel’s theory. This yields physical insight into the structure and dynamics of vibronic resonances, since their frequency and width is related to fundamental physical constants and microscopic model parameters. For illustration, we apply this scheme to compute the linear absorption spectrum of the Fenna-Matthews-Olson light harvesting complex, comparing analytic calculations, numerical Monte Carlo simulations, and experimental data.
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14 April 2019
Research Article|
April 08 2019
Microscopic calculation of absorption spectra of macromolecules: An analytic approach
Matteo Carli;
Matteo Carli
1
Physics Department of Trento University
, Via Sommarive 14, Povo, Trento 38123, Italy
2
Scuola Internazionale Superiore di Studi Avanzati (SISSA)
, via Bonomea 265, Trieste 34136, Italy
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Michele Turelli;
Michele Turelli
1
Physics Department of Trento University
, Via Sommarive 14, Povo, Trento 38123, Italy
3
Trento Institute for Fundamental Physics and Applications (INFN-TIFPA)
, Via Sommarive 23, Povo, Trento 38123, Italy
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Pietro Faccioli
Pietro Faccioli
a)
1
Physics Department of Trento University
, Via Sommarive 14, Povo, Trento 38123, Italy
3
Trento Institute for Fundamental Physics and Applications (INFN-TIFPA)
, Via Sommarive 23, Povo, Trento 38123, Italy
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J. Chem. Phys. 150, 144103 (2019)
Article history
Received:
December 04 2018
Accepted:
March 14 2019
Citation
Matteo Carli, Michele Turelli, Pietro Faccioli; Microscopic calculation of absorption spectra of macromolecules: An analytic approach. J. Chem. Phys. 14 April 2019; 150 (14): 144103. https://doi.org/10.1063/1.5084120
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