期刊
JOURNAL OF PHYSICS-CONDENSED MATTER
卷 32, 期 18, 页码 -出版社
IOP PUBLISHING LTD
DOI: 10.1088/1361-648X/ab699e
关键词
molecular crystals; singlet fission; electronic structure; GW plus BSE; excitons
资金
- Charles E Kaufman Foundation [KA2017-91789]
- National Science Foundation (NSF) Division of Materials Research [DMR-1844484]
- DOE Office of Science User Facility [DE-AC02-06CH11357]
- Office of Science of the US Department of Energy [DE-AC02-05CH11231]
Singlet fission (SF) is a photophysical process considered as a possible scheme to bypass the Shockley-Queisser limit by generating two triplet-state excitons from one high-energy photon. Polyacene crystals, such as tetracene and pentacene, have shown outstanding SF performance both theoretically and experimentally. However, their instability prevents them from being utilized in SF-based photovoltaic devices. In search of practical SF chromophores, we use many-body perturbation theory within the GW approximation and Bethe-Salpeter equation to study the excitonic properties of a family of pyrene-stabilized acenes. We propose a criterion to define the convergence of exciton wave-functions with respect to the fine k-point grid used in the BerkeleyGW code. An open-source Python code is presented to perform exciton wavefunction convergence checks and streamline the double Bader analysis of exciton character. We find that the singlet excitons in pyrene-stabilized acenes have a higher degree of charge transfer character than in the corresponding acenes. The pyrene-fused tetracene and pentacene derivatives exhibit comparable excitation energies to their corresponding acenes, making them potential SF candidates. The pyrene-stabilized anthracene derivative is considered as a possible candidate for triplet-triplet annihilation because it yields a lower SF driving force than anthracene.
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