Microscopic calculation of absorption spectra of macromolecules: An analytic approach
| Autor: | Michele Turelli, Pietro Faccioli, Matteo Carli |
|---|---|
| Rok vydání: | 2019 |
| Předmět: |
Density matrix
Physics 010304 chemical physics Physical constant Monte Carlo method Structure (category theory) General Physics and Astronomy 010402 general chemistry 01 natural sciences 0104 chemical sciences Excited state 0103 physical sciences Dissipative system Quantum system Statistical physics Physical and Theoretical Chemistry Quantum field theory |
| Zdroj: | The Journal of Chemical Physics. 150:144103 |
| ISSN: | 1089-7690 0021-9606 |
| DOI: | 10.1063/1.5084120 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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