Hydrogen-Bond Architectures of Protonated 4,4′-Biimidazolium Derivatives and Oligo(imidazolium)s in Charge-Transfer Salts with Tetracyanoquinodimethane

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• 作者：Tsuyoshi Murata ; Yasushi Morita ; Yumi Yakiyama ; Yosuke Yamamoto ; Satoru Yamada ; Yoshie Nishimura ; Kazuhiro Nakasuji
• 刊名：Crystal Growth & Design
• 出版年：2008
• 出版时间：August 2008
• 年：2008
• 卷：8
• 期：8
• 页码：3058-3065
• 全文大小：492K
• 年卷期：v.8,no.8(August 2008)
• ISSN：1528-7505

文摘

Charge-transfer salts of protonated cations of 2,2′-disubstituted-4,4′-biimidazoles and oligo(imidazole)s with tetracyanoquinodimethane (TCNQ) were investigated to demonstrate the high potential of these systems for the regulation of molecular arrangement and electronic structure of charge-transfer salts. 4,4′-Biimidazole derivatives afforded six kinds of mixed-valent TCNQ salts exhibiting semiconducting behaviors. Structural analyses revealed that the protonated 4,4′-biimidazolium derivatives formed multidirectional and multidimensional hydrogen bonds with TCNQ, and constructed two kinds of self-assembled architectures: one-dimensional chainlike motifs involving TCNQ molecules and two-dimensional sheet structures composed of the alternation of segregated columns of 4,4′-biimidazolium and TCNQ. Furthermore, the hydrogen-bonding patterns regulated the electronic structures in TCNQ columns by strong cation−anion interaction, causing the nonuniform charge-distribution and semiconducting behaviors.