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It is known that within the interacting electron model Hamiltonian for theone-dimensional 1/4-filled band, the singlet ground state is a Wigner crystalonly if the nearest neighbor electron-electron repulsion is larger than acritical value. We show that this critical nearest neighbor Coulomb interactionis different for each spin subspace, with the critical value decreasing withincreasing spin. As a consequence, with the lowering of temperature, there canoccur a transition from a Wigner crystal charge-ordered state to a spin-Peierlsstate that is a Bond-Charge-Density Wave with charge occupancies different fromthe Wigner crystal. This transition is possible because spin excitations fromthe spin-Peierls state in the 1/4-filled band are necessarily accompanied bychanges in site charge densities. We apply our theory to the 1/4-filled bandquasi-one-dimensional organic charge-transfer solids in general and to 2:1tetramethyltetrathiafulvalene (TMTTF) and tetramethyltetraselenafulvalene(TMTSF) cationic salts in particular. We believe that many recent experimentsstrongly indicate the Wigner crystal to Bond-Charge-Density Wave transition inseveral members of the TMTTF family. We explain the occurrence of two differentantiferromagnetic phases but a single spin-Peierls state in the generic phasediagram for the 2:1 cationic solids. The antiferromagnetic phases can haveeither the Wigner crystal or the Bond-Charge-Spin-Density Wave chargeoccupancies. The spin-Peierls state is always a Bond-Charge-Density Wave.

Temperature-driven transition from the Wigner Crystal to the Bond-Charge-Density Wave in the Quasi-One-Dimensional Quarter-Filled band