Charge-Separated States Determined Photoinduced Electron Transfer Efficiency in a D-D-A System in an External Electric Field
(2023) In Journal of Physical Chemistry C- Abstract
Focusing on the photoinduced electron transfer properties of the D-D-A molecule ((TPA-TT)-BODIPY-C60) in an external electric field (Fext), the excited-state properties in which the double-donor molecule is excited to form three charge-separated states were simulated. The charge-Transfer processes of these three charge-separated states were investigated by considering the two donors as a whole ((TPA-TT-BODIPY)·+-C60·-) as a comparison object. The electronic coupling (VDA), reorganization energy (λ), and free energy (δG) of the different charge-separated states in Fext were calculated and simulated. The calculated results show that the λ of (TPA-TT-BODIPY)·+-C60·- ranges from 0.576 to 0.51 eV, and the calculated δG of exciton... (More)
Focusing on the photoinduced electron transfer properties of the D-D-A molecule ((TPA-TT)-BODIPY-C60) in an external electric field (Fext), the excited-state properties in which the double-donor molecule is excited to form three charge-separated states were simulated. The charge-Transfer processes of these three charge-separated states were investigated by considering the two donors as a whole ((TPA-TT-BODIPY)·+-C60·-) as a comparison object. The electronic coupling (VDA), reorganization energy (λ), and free energy (δG) of the different charge-separated states in Fext were calculated and simulated. The calculated results show that the λ of (TPA-TT-BODIPY)·+-C60·- ranges from 0.576 to 0.51 eV, and the calculated δG of exciton dissociation ranges from-1.402 to-1.143 eV, indicating that exciton dissociation occurs in the Marcus inverted region. In the range of Fext =-10 × 10-5 to 10 × 10-5 au, the trend of the charge-Transfer rate is gradually increasing, and the rate increase is mainly from the VDA and δG changes. Moreover, the rapid formation of the (TPA-TT)-BODIPY·+-C60·- charge-separated state and the formation of the long-lived (TPA-TT)·+-BODIPY-C60·- are indicated by the exciton dissociation rate. By studying the charge-Transfer parameters under different electric field directions, it is found that the regulation of electric field strength on the charge-Transfer rate is consistent. These results provide a feasible method for the rational design of a new type of electron transfer process with high efficiency of the D-D-A system.
(Less)
- author
- Wang, Xinyue ; Wang, Hongxiang ; Zhang, Meixia ; Pullerits, Tõnu LU and Song, Peng
- organization
- publishing date
- 2023
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Physical Chemistry C
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- scopus:85147885824
- ISSN
- 1932-7447
- DOI
- 10.1021/acs.jpcc.2c07364
- language
- English
- LU publication?
- yes
- id
- 6496f8c1-fcbb-4707-b7ea-3926f0c4c72e
- date added to LUP
- 2023-02-20 14:12:34
- date last changed
- 2023-11-21 06:55:41
@article{6496f8c1-fcbb-4707-b7ea-3926f0c4c72e,
abstract = {{<p>Focusing on the photoinduced electron transfer properties of the D-D-A molecule ((TPA-TT)-BODIPY-C60) in an external electric field (Fext), the excited-state properties in which the double-donor molecule is excited to form three charge-separated states were simulated. The charge-Transfer processes of these three charge-separated states were investigated by considering the two donors as a whole ((TPA-TT-BODIPY)·+-C60·-) as a comparison object. The electronic coupling (VDA), reorganization energy (λ), and free energy (δG) of the different charge-separated states in Fext were calculated and simulated. The calculated results show that the λ of (TPA-TT-BODIPY)·+-C60·- ranges from 0.576 to 0.51 eV, and the calculated δG of exciton dissociation ranges from-1.402 to-1.143 eV, indicating that exciton dissociation occurs in the Marcus inverted region. In the range of Fext =-10 × 10-5 to 10 × 10-5 au, the trend of the charge-Transfer rate is gradually increasing, and the rate increase is mainly from the VDA and δG changes. Moreover, the rapid formation of the (TPA-TT)-BODIPY·+-C60·- charge-separated state and the formation of the long-lived (TPA-TT)·+-BODIPY-C60·- are indicated by the exciton dissociation rate. By studying the charge-Transfer parameters under different electric field directions, it is found that the regulation of electric field strength on the charge-Transfer rate is consistent. These results provide a feasible method for the rational design of a new type of electron transfer process with high efficiency of the D-D-A system.</p>}},
author = {{Wang, Xinyue and Wang, Hongxiang and Zhang, Meixia and Pullerits, Tõnu and Song, Peng}},
issn = {{1932-7447}},
language = {{eng}},
publisher = {{The American Chemical Society (ACS)}},
series = {{Journal of Physical Chemistry C}},
title = {{Charge-Separated States Determined Photoinduced Electron Transfer Efficiency in a D-D-A System in an External Electric Field}},
url = {{http://dx.doi.org/10.1021/acs.jpcc.2c07364}},
doi = {{10.1021/acs.jpcc.2c07364}},
year = {{2023}},
}