Chemistry of Materials
Chemistry of Materials
5 years ago

Molecular Assembly-Induced Charge Transfer for Programmable Functionalities

Molecular Assembly-Induced Charge Transfer for Programmable Functionalities
Shenqiang Ren, Zheng Li, Ziyao Zhou, Shuquan Chang, Jeffrey C. Grossman, Zhipu Luo, Huashan Li, Ming Liu, Zhuolei Zhang, Mengmeng Guan
The donor–acceptor interface within molecular charge transfer (CT) solids plays a vital role in the hybridization of molecular orbitals to determine their carrier transport and electronic delocalization. In this study, we demonstrate molecular assembly-driven bilayer and crystalline solids, consisting of electron donor dibenzotetrathiafulvalene (DBTTF) and acceptor C60, in which interfacial engineering-induced CT degree control is a key parameter for tuning its optical, electronic, and magnetic performance. Compared to the DBTTF/C60 bilayer structure, the DBTTFC60 cocrystalline solids show a stronger degree of charge transfer for broad CT absorption and a large dielectric constant. In addition, the DBTTFC60 cocrystals exhibit distinct CT arrangement-driven anisotropic electron mobility and spin characteristics, which further enables the development of high-penetration and high-energy γ-ray photodetectors. The results presented in this paper provide a basis for the design and control of molecular charge transfer solids, which facilitates the integration of such materials into molecular electronics.

Publisher URL: http://dx.doi.org/10.1021/acs.chemmater.7b04357

DOI: 10.1021/acs.chemmater.7b04357

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