The Library
Importance and nature of short-range excitonic interactions in light harvesting complexes and organic semiconductors
Tools
Tools
Tools
Fornari, Rocco P., Rowe, Patrick, Padula, Daniele and Troisi, Alessandro (2017) Importance and nature of short-range excitonic interactions in light harvesting complexes and organic semiconductors. Journal of Chemical Theory and Computation, 13 (8). pp. 3754-3763. doi:10.1021/acs.jctc.7b00328 ISSN 1549-9618.
|
PDF
WRAP-importance-nature-short-range-excitonic-interactions-Fornari-2018.pdf - Accepted Version - Requires a PDF viewer. Download (1315Kb) | Preview |
Official URL: http://doi.org/10.1021/acs.jctc.7b00328
Abstract
The singlet excitonic coupling between many pairs of chromophores is evaluated in three different light harvesting complexes (LHCs) and two organic semiconductors (amorphous and crystalline). This large database of structures is used to assess the relative importance of short-range (exchange, overlap, orbital) and long-range (Coulombic) excitonic coupling. We find that Mulliken atomic transition charges can introduce systematic errors in the Coulombic coupling and that the dipole–dipole interaction fails to capture the true Coulombic coupling even at intermolecular distances of up to 50 Å. The non-Coulombic short-range contribution to the excitonic coupling is found to represent up to ∼70% of the total value for molecules in close contact, while, as expected, it is found to be negligible for dimers not in close contact. For the face-to-face dimers considered here, the sign of the short-range interaction is found to correlate with the sign of the Coulombic coupling, i.e. reinforcing it when it is already strong. We conclude that for molecules in van der Waals contact the inclusion of short-range effects is essential for a quantitative description of the exciton dynamics.
| Item Type: | Journal Article | ||||||||
|---|---|---|---|---|---|---|---|---|---|
| Subjects: | Q Science > QD Chemistry | ||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||
| Library of Congress Subject Headings (LCSH): | Excited state chemistry, Exciton theory, Organic semiconductors, Energy transfer | ||||||||
| Journal or Publication Title: | Journal of Chemical Theory and Computation | ||||||||
| Publisher: | American Chemical Society | ||||||||
| ISSN: | 1549-9618 | ||||||||
| Official Date: | August 2017 | ||||||||
| Dates: |
|
||||||||
| Volume: | 13 | ||||||||
| Number: | 8 | ||||||||
| Page Range: | pp. 3754-3763 | ||||||||
| DOI: | 10.1021/acs.jctc.7b00328 | ||||||||
| Status: | Peer Reviewed | ||||||||
| Publication Status: | Published | ||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||
| Copyright Holders: | American Chemical Society | ||||||||
| Date of first compliant deposit: | 8 February 2018 | ||||||||
| Date of first compliant Open Access: | 26 June 2018 | ||||||||
| RIOXX Funder/Project Grant: |
|
Request changes or add full text files to a record
Repository staff actions (login required)
 |
View Item |
Downloads
Downloads per month over past year
