Structural Variations in β-(BDA-TTP)₂FeCl₄ at Low Temperature and under Pressure : Charge-Ordered State with a Two-Fold Crystal Structure
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概要
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The pressure-induced organic superconductor \beta-(BDA-TTP)<inf>2</inf>FeCl<inf>4</inf>[BDA-TTP = 2,5-bis(1,3-dithian-2-ylidene)-1,3,4,6-tetrathiapentalene], which shows a metal--insulator (MI) transition at T_{\text{MI}} = 113 K under ambient pressure, has been found by X-ray study to have a two-fold crystal structure along the c-axis in the insulating state at 10 K. In the donor layer, there are four independent BDA-TTP molecules, which are divided into two charge-poor ones and two charge-rich ones on the basis of the folding dihedral angles around the intramolecular sulfur-to-sulfur axes of two outer dithiane rings in BDA-TTP. The charge separation leads to the formation of two types of dimers: a dimer consisting of two charge-poor donors and a dimer consisting of two charge-rich ones. The tight-binding band calculation revealed a band gap of 5.3 meV in the energy dispersion. The MI transition can be therefore accounted for by the charge separation. In addition, we investigated the crystal and electronic structures of \beta-(BDA-TTP)<inf>2</inf>FeCl<inf>4</inf>at different pressures up to 21 kbar, and found that the application of pressures causes variations in both the conformation of donor molecule and the donor arrangement, which are responsible for almost uniform interaction in the donor stacking and for an increase in bandwidth (W). As a result, the suppression of MI transition and subsequent occurrence of superconductivity in \beta-(BDA-TTP)<inf>2</inf>FeCl<inf>4</inf>would be observed with increasing pressure.
- 2013-05-15
著者
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Kikuchi Koichi
Department Of Chemistry Tokyo Metropolitan University
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Yamada Jun-ichi
Department Of Electronics Faculty Of Engineering Kobe University:(present Address) The Musashino Ele
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Fujita Wataru
Department Of Applied Chemistry School Of Engineering Nagoya University
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Kodama Takeshi
Department Of Applied Physics Waseda University
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Takahashi Kazuyuki
Department Of Chemical Pharmacology Faculty Of Pharmaceutical Sciences Meijo University
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SASAMORI Kota
Department of Chemistry, Tokyo Metropolitan University, Hachioji, Tokyo 192-0397, Japan
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