Anion substitution in hydrogen-bonded organic conductors: the chemical pressure effect on hydrogen-bond-mediated phase transition
Anion substitution in hydrogen-bonded organic conductors: the chemical pressure effect on hydrogen-bond-mediated phase transition
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氢键有机导体中的阴离子取代：化学压力对氢键介导的相变的影响
作者：
J. Yoshida;A. Ueda;R. Kumai;Y. Murakami;H. Mori
本文合成了三种新型氢键有机导体β ′-[H3（Cat-EDO-TTF）2] X（X = ClO4，PF6，AsF6; Cat-EDO-TTF =邻苯二酚稠合的乙撑二氧四硫富瓦烯），作为母体BF 4盐（X = BF 4）的阴离子取代类似物。这些盐都是同构的，然而，只有BF 4盐显示相变，在此基础上的分子排列和物理性质急剧变化的合作与弯曲的H-键。通过对它们的晶体结构和电子结构的系统比较，发现阴离子取代产生了显著的化学压力，从而导致了它们的物理性质和相变性质的差异。有趣的是，这种化学压力是高度各向异性的，这专门改变了π堆叠层中Cat-EDO-TTF骨架之间的并排相互作用。因此，我们得出结论，这种独特的相变是由柱间的并排相互作用与π-π内二聚体相互作用和氢键弯曲的合作引起的。
We have synthesized three kinds of novel hydrogen-bonded (H-bonded) organic conductor, β′-[H3(Cat-EDO-TTF)2]X (X = ClO4, PF6, AsF6; Cat-EDO-TTF = catechol-fused ethylenedioxytetrathiafulvalene), as anion-substituted analogues of the parent BF4 salt (X = BF4). These salts are all isostructural, however, only the BF4 salt shows a phase transition, upon which the molecular arrangement and physical properties are drastically changed in cooperation with bending of the H-bond. A systematic comparison of their crystal and electronic structures disclosed that a significant chemical pressure is generated by the present anion substitution, causing differences in their physical properties and phase transition nature. Interestingly, this chemical pressure is highly anisotropic, which exclusively changes the side-by-side interactions between the Cat-EDO-TTF skeletons in the π-stacking layer. Therefore, we conclude that this unique phase transition is caused by a cooperation of the intercolumnar side-by-side interactions with the π–π intra-dimer interactions and H-bond bending.
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