Abstract

AbstractNew metallic triclinic (1) and monoclinic (2) crystals of the (BEDT‐TTF)4AI[MIII(C2O4)3]G family of organic molecular conductors have been prepared: α‐“pseudo‐κ”‐(BEDT‐TTF)4Kx(H3O)1–x[GaIII(C2O4)3]·1,2‐C6H4Br2 (x ≈ 0.45) (1) and β″‐(BEDT‐TTF)4Kx(H3O)1–x[GaIII(C2O4)3]·PhBr (x ≈ 0.33) (2). The triclinic crystals belong to a quite rare type of bilayered radical ion salts and contain alternating BEDT‐TTF layers with two distinct packing motifs (α‐ and “pseudo‐κ”). The monoclinic crystals contain one kind of BEDT‐TTF radical cation layers. The crystal structure, transport, and magnetotransport properties of 1 and 2 have been studied. The Shubnikov–de Haas (SdH) oscillations were found in both phases. The structure and properties of 1 and 2 are compared with another similar phase with M = FeIII.

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