Single-Component Conductors: A Sturdy Electronic Structure Generated by Bulky Substituents

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• 作者：Agathe Filatre-Furcate ; Nathalie Bellec ; Olivier Jeannin ; Pascale Auban-Senzier ; Marc Fourmigué ; Jorge Íñiguez ; Enric Canadell ; Benjamin Brière ; Vinh Ta Phuoc ; Dominique Lorcy
• 刊名：Inorganic Chemistry
• 出版年：2016
• 出版时间：June 20, 2016
• 年：2016
• 卷：55
• 期：12
• 页码：6036-6046
• 全文大小：612K
• 年卷期：0
• ISSN：1520-510X

文摘

While the introduction of large, bulky substituents such as tert-butyl, −SiMe₃, or −Si(isopropyl)₃ has been used recently to control the solid state structures and charge mobility of organic semiconductors, this crystal engineering strategy is usually avoided in molecular metals where a maximized overlap is sought. In order to investigate such steric effects in single component conductors, the ethyl group of the known [Au(Et-thiazdt)₂] radical complex has been replaced by an isopropyl one to give a novel single component molecular conductor denoted [Au(iPr-thiazdt)₂] (iPr-thiazdt: N-isopropyl-1,3-thiazoline-2-thione-4,5-dithiolate). It exhibits a very original stacked structure of crisscross molecules interacting laterally to give a truly three-dimensional network. This system is weakly conducting at ambient pressure (5 S·cm^–1), and both transport and optical measurements evidence a slowly decreasing energy gap under applied pressure with a regime change around 1.5 GPa. In contrast with other conducting systems amenable to a metallic state under physical or chemical pressure, the Mott insulating state is stable here up to 4 GPa, a consequence of its peculiar electronic structure.