期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 21, 期 42, 页码 15020-15028出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201502047
关键词
conducting materials; electron transfer; hydrogen bonds; hydrogen transfer; phase transitions
资金
- Japan Society for the Promotion of Science (JSPS), Japan [26810044, 24340074]
- Ministry of Education, Culture, Sports, Science and Technology, Japan
- Photon Factory Program Advisory Committee [2014S2-001]
- Grants-in-Aid for Scientific Research [15H00988, 26810044, 26610096] Funding Source: KAKEN
New important aspects of the hydrogen-bond (H-bond)-dynamics-based switching of electrical conductivity and magnetism in an H-bonded, purely organic conductor crystal have been discovered by modulating its tetrathiafulvalene (TTF)-based molecular p-electron system by means of partial sulfur/selenium substitution. The prepared selenium analogue also showed a similar type of phase transition, induced by H-bonded deuterium transfer followed by electron transfer between the H-bonded TTF skeletons, and the resulting switching of the physical properties; however, subtle but critical differences due to sulfur/selenium substitution were detected in the electronic structure, phase transition nature, and switching function. A molecular-level discussion based on the crystal structures shows that this chemical modification of the TTF skeleton influences not only its own p-electronic structure and pi-pi interactions within the conducting layer, but also the H-bond dynamics between the TTF pi skeletons in the neighboring layers, which enables modulation of the interplay between the H-bond and pi electrons to cause such differences.
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