Subtle Steric Differences Impact the Structural and Conducting Properties of Radical Gold Bis(dithiolene) Complexes

Abstract : Among single component molecular conductors, neutral radical gold dithiolene complexes [(R-thiazdt) 2 Au] • derived from the N-alkyl-1,3-thiazoline-2-thione-4,5-dithiolate (R-thiazdt) ligand provide an extensive series of conducting, non-dimerized, ½-filled band systems. Analogs of the known R = isopropyl derivative were investigated here with R = NMe 2 , cyclopropyl (cPr) and n-propyl (nPr), aiming at rationalizing the different solid state structures adopted by these compounds despite very closely related substituents on the heterocyclic nitrogen atom. An original crisscross organization within dimerized chains is observed with R = NMe 2 , differing however from the analogous iPr derivative by a 180° rotation of the heterocyclic nitrogen substituent. On the other hand, the cyclopropyl and n-propyl substituents lead to robust, uniform, non-dimerized chains with a strongly 1D electronic structure and a formal ½-filled electronic structure. The semiconducting behaviour of these two radical complexes is characteristic of a Mott insulator, whose sensitivity to external pressure has been evaluated up to 2.5 GPa.
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Chemistry - A European Journal, Wiley-VCH Verlag, 2017, 23 (63), pp.16004-16013. 〈10.1002/chem.201703172〉
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Agathe Filatre-Furcate, Thierry Roisnel, Marc Fourmigué, Olivier Jeannin, Nathalie Bellec, et al.. Subtle Steric Differences Impact the Structural and Conducting Properties of Radical Gold Bis(dithiolene) Complexes. Chemistry - A European Journal, Wiley-VCH Verlag, 2017, 23 (63), pp.16004-16013. 〈10.1002/chem.201703172〉. 〈hal-01636555〉

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