2017 年 75 巻 10 号 p. 1045-1054
Molecular crystalline materials that comprise π-electron organic molecules exhibit various interesting physical properties and functionalities related to electrical conductivity and magnetic, dielectric, and optical properties. Their experimental and theoretical studies have extensively been performed by a wide range of researchers in the fields of organic chemistry, physical chemistry, solid-state physics, and so on. In particular, synthetic organic chemists have devoted continuous effort to the design and synthesis of new functional molecular crystals and component molecules, which led to numerous important discoveries in this interdisciplinary research field. Here we report the development of a new type of organic conductors based on catechol-fused tetrathiafulvalene (TTF) derivatives. Interestingly, dynamic properties of hydrogen bonds through the catechol moiety are coupled with π-electrons on the TTF skeleton, which allowed us to discover unprecedented phase transitions, physical properties, and functionalities. In this paper, the design, synthesis, structures, and properties of our new molecules and crystals are described from a molecular point of view.