Abstract:We consider structural instabilities exhibited by the one-dimensional (1D) (arene) 2 X family of organic conductors in relation with their electronic and magnetic properties. With a charge transfer of one electron to each anion X, these salts exhibit a quarter-filled (hole) conduction band located on donor stacks. Compounds built with donors such as fluorenthene, perylene derivatives and anions X such as PF 6 or AsF 6 exhibit a high temperature (T P~1 70 K) conventional Peierls transition that is preceded by a sizeable regime of 1D 2k F charge density wave fluctuations (k F is the Fermi wave vector of the 1D electron gas located on Per stack). Surprisingly, and probably because of the presence of a multi-sheet warped Fermi surface, the critical temperature of the Peierls transition is considerably reduced in the perylene series α-(Per) 2 [M(mnt) 2 ] where X is the dithiolate molecule with M = Au, Cu, Co and Fe. Special attention will be devoted to physical properties of α-(Per) 2 [M(mnt) 2 ] salts with M = Pt, Pd and Ni which incorporate segregated S = 1/2 1D antiferromagnetic (AF) dithiolate stacks coexisting with 1D metallic Per stacks. We analyze conjointly the structural and magnetic properties of these salts in relation with the 1D spin-Peierls (SP) instability located on the dithiolate stacks. We show that the SP instability of Pd and Ni derivatives occurs in the classical (adiabatic) limit while the SP instability of the Pt derivative occurs in the quantum (anti-adiabatic) limit. Furthermore, we show that in Pd and Ni derivatives 1st neighbor direct and frustrated 2nd neighbor indirect (through a fine tuning with the mediated 2k F RKKY coupling interaction on Per stacks) AF interactions add their contribution to the SP instability to stabilize a singlet-triplet gap. Our analysis of the data show unambiguously that magnetic α-(Per) 2 [M(mnt) 2 ] salts exhibit the physics expected for a two chain Kondo lattice.