Organic single crystals of charge-transfer complexes: model systems for the study of donor/acceptor interactions

Abstract

The charge-transfer (CT) state arising as a hybrid electronic state at the interface between charge donor and charge acceptor molecular units is important to a wide variety of physical processes in organic semiconductor devices. The exact nature of this state depends heavily on the nature and co-facial overlap between the donor and acceptor; however, altering this overlap is usually accompanied by extensive confounding variations in properties due to extrinsic factors, such as microstructure. As a consequence, establishing reliable relationships between donor/acceptor molecular structures, their molecular overlap, degree of charge transfer and physical properties, is challenging. Herein, we examine the electronic structure of a polymorphic system based on the donor dibenzotetrathiafulvalene (DBTTF) and the acceptor 7,7,8,8-tetracyanoquinodimethane (TCNQ) in the form of high-quality single crystals varying in the donor–acceptor overlap. Using angle-resolved photoemission spectroscopy, we resolve the highest occupied molecular orbital states of the CT crystals. Analysis based on field-effect transistors allows us to probe the sub-gap states impacting hole and electron transport. Our results expand the understanding on the impact of donor and acceptor interactions on electronic structure and charge transport.

Graphical abstract: Organic single crystals of charge-transfer complexes: model systems for the study of donor/acceptor interactions

Supplementary files

Article information

Article type
Communication
Submitted
31 Jul 2021
Accepted
15 Oct 2021
First published
15 Oct 2021

Mater. Horiz., 2022, Advance Article

Organic single crystals of charge-transfer complexes: model systems for the study of donor/acceptor interactions

K. P. Goetz, H. F. Iqbal, E. G. Bittle, C. A. Hacker, S. Pookpanratana and O. D. Jurchescu, Mater. Horiz., 2022, Advance Article , DOI: 10.1039/D1MH01214B

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