Molecular Conductors with Effectively Half‐Filled Electronic States Based on Tetrathiafulvalene Derivatives Condensed with a 2‐Isopropylidene‐1,3‐dithiole Ring

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<jats:title>Abstract</jats:title><jats:p>The electron donor 2‐isopropylidene‐1,3‐dithiolo[4,5‐<jats:italic>d</jats:italic>]‐4,5‐ethylenediselenotetrathiafulvalene (<jats:bold>3</jats:bold>) provides two new molecular conductors, (<jats:bold>3</jats:bold>)<jats:sub>2</jats:sub>[M(CN)<jats:sub>2</jats:sub>] (M = Ag and Au). These salts crystallize in the triclinic <jats:italic>P</jats:italic><jats:styled-content>$\bar {1}$<jats:inline-graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="graphic/tex2gif-ueqn-1.gif" xlink:title="equation image" /></jats:styled-content> space group. The donor sheet structure of these salts is the so‐called β‐type molecular array, in which the donor molecules form a head‐to‐tail dimer. The formation of considerable dimerization and the 2:1 donor–anion ratio result in an effectively half‐filled electronic nature. These salts show metallic conducting behavior from room temperature. The metallic conducting behavior of (<jats:bold>3</jats:bold>)<jats:sub>2</jats:sub>[Ag(CN)<jats:sub>2</jats:sub>] was retained down to 8 K; however, the resistivity of (<jats:bold>3</jats:bold>)<jats:sub>2</jats:sub>[Au(CN)<jats:sub>2</jats:sub>] increased at around 50 K. The magnetic susceptibility of (<jats:bold>3</jats:bold>)<jats:sub>2</jats:sub>[Au(CN)<jats:sub>2</jats:sub>] suggests that the strength of the electron correlation for this salt is enhanced below 50 K.</jats:p>

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