Molecular cocrystal odyssey to unconventional electronics and photonics

Cocrystal has been discovered and studied for more than 170 years since 1844, while the applications to optoelectronics only begin in the last decade. Several general questions that chemists and materials scientists currently seek to answer are: can we design and control the molecular self-assembly and cocrystal growth, what's the packing-property correlations, as well as how can we improve device parameters for real applications in industry. In this contribution, we review our and other groups' recent advances in the cocrystal research field sequentially including: (1) nucleation and growth mechanisms for selective preparation of cocrystals with different donor/acceptor ratio and morphology; (2) charge transport and electronic devices, particularly field-effect transistor (FET) and photo-response device. We discuss the in-situ single crystal device fabrication method, ambipolar charge transport, and molecular packing-charge separation correlation; (3) photonic and optical property, focusing on optical waveguide, photonic logic computation, and nonlinear optics (NLO). We present unusual optical properties revealed by advanced instruments and general structure-function relations for future study. Importantly, the extensive investigations described herein yield in-depth and detailed understandings of molecular cocrystals, and show that such bi-component material systems together with the developed instrument measurement methodologies have the potential to initiate unconventional electronic and photonic science and technology.