Advanced

Discrimination of Diverse Coherences Allows Identification of Electronic Transitions of a Molecular Nanoring

Butkus, Vytautas; Alster, Jan LU ; Basinskaite, Egle LU ; Augulis, Ramunas LU ; Neuhaus, Patrik; Valkunas, Leonas; Anderson, Harry L; Abramavicius, Darius and Zigmantas, Donatas LU (2017) In Journal of Physical Chemistry Letters 8(10). p.2344-2349
Abstract

The role of quantum coherence in photochemical functions of molecular systems such as photosynthetic complexes is a broadly debated topic. Coexistence and intermixing of electronic and vibrational coherences has been proposed to be responsible for the observed long-lived coherences and high energy transfer efficiency. However, clear experimental evidence of coherences with different origins operating at the same time has been elusive. In this work, multidimensional spectra obtained from a six-porphyrin nanoring system are analyzed in detail with support from theoretical modeling. We uncover a great diversity of separable electronic, vibrational, and mixed coherences and show their cooperation in shaping the spectroscopic response. The... (More)

The role of quantum coherence in photochemical functions of molecular systems such as photosynthetic complexes is a broadly debated topic. Coexistence and intermixing of electronic and vibrational coherences has been proposed to be responsible for the observed long-lived coherences and high energy transfer efficiency. However, clear experimental evidence of coherences with different origins operating at the same time has been elusive. In this work, multidimensional spectra obtained from a six-porphyrin nanoring system are analyzed in detail with support from theoretical modeling. We uncover a great diversity of separable electronic, vibrational, and mixed coherences and show their cooperation in shaping the spectroscopic response. The results permit direct assignment of electronic and vibronic states and characterization of the excitation dynamics. The clear disentanglement of coherences in molecules with extended π-conjugation opens up new avenues for exploring coherent phenomena and understanding their importance for the function of complex systems.

(Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Physical Chemistry Letters
volume
8
issue
10
pages
6 pages
publisher
The American Chemical Society
external identifiers
  • scopus:85019394990
  • wos:000402026500042
ISSN
1948-7185
DOI
10.1021/acs.jpclett.7b00612
language
English
LU publication?
yes
id
5f2cbd99-15db-4d37-a97d-fee074828aea
date added to LUP
2017-06-28 10:28:01
date last changed
2018-05-06 04:34:42
@article{5f2cbd99-15db-4d37-a97d-fee074828aea,
  abstract     = {<p>The role of quantum coherence in photochemical functions of molecular systems such as photosynthetic complexes is a broadly debated topic. Coexistence and intermixing of electronic and vibrational coherences has been proposed to be responsible for the observed long-lived coherences and high energy transfer efficiency. However, clear experimental evidence of coherences with different origins operating at the same time has been elusive. In this work, multidimensional spectra obtained from a six-porphyrin nanoring system are analyzed in detail with support from theoretical modeling. We uncover a great diversity of separable electronic, vibrational, and mixed coherences and show their cooperation in shaping the spectroscopic response. The results permit direct assignment of electronic and vibronic states and characterization of the excitation dynamics. The clear disentanglement of coherences in molecules with extended π-conjugation opens up new avenues for exploring coherent phenomena and understanding their importance for the function of complex systems.</p>},
  author       = {Butkus, Vytautas and Alster, Jan and Basinskaite, Egle and Augulis, Ramunas and Neuhaus, Patrik and Valkunas, Leonas and Anderson, Harry L and Abramavicius, Darius and Zigmantas, Donatas},
  issn         = {1948-7185},
  language     = {eng},
  month        = {05},
  number       = {10},
  pages        = {2344--2349},
  publisher    = {The American Chemical Society},
  series       = {Journal of Physical Chemistry Letters},
  title        = {Discrimination of Diverse Coherences Allows Identification of Electronic Transitions of a Molecular Nanoring},
  url          = {http://dx.doi.org/10.1021/acs.jpclett.7b00612},
  volume       = {8},
  year         = {2017},
}