File
Authors
Fujita, Takatoshi Institute for Molecular Science
Noguchi, Yoshifumi Department of Applied Chemistry and Biochemical Engineering, Graduate School of Engineering, Shizuoka University
Hoshi, Takeo Department of Applied Mathematics and Physics, Tottori University Researchers DB KAKEN
Abstract
Predicting the charge-transfer (CT) excited states across the donor/acceptor (D/A) interface is essential for understanding the charge photogeneration process in an organic solar cell.Here, we present a fragment-based GW implementation that can be applied to a D/A interface structure and thus enables accurate determination of the CT states.The implementation is based on the fragmentation approximation of the polarization function and the combined GW and Coulomb-hole plus screened exchange approximations for self-energies.The fragmentbased GW is demonstrated by application to the pentacene/C60 interface structure containing more than 2000 atoms.The CT excitation energies were estimated from the quasiparticle energies and electron–hole screened Coulomb interactions; the computed energies are in reasonable agreement with experimental estimates from the external quantum efficiency measurements.We highlight the impact of the induced polarization effects on the electron–hole energetics.The proposed fragment-based GW method offers a first-principles tool to compute the quasiparticle energies and electronic excitation energies of organic materials.
Content Type
Journal Article
Link
ISSN
00219606
NCID
AA00694991
Journal Title
The Journal of Chemical Physics
Current Journal Title
The Journal of Chemical Physics
Volume
151
Issue
11
Start Page
114109
Published Date
2019-09-18
Publisher-DOI
Text Version
Publisher
Rights
© 2019 AIP Publishing
Citation
Fujita Takatoshi, Noguchi Yoshifumi, Hoshi Takeo. Charge-transfer excited states in the donor/acceptor interface from large-scale GW calculations. Journal of Chemical Physics. 2019;151(11):114109.
Department
Faculty of Engineering/Graduate School of Engineering
Language
English