Abstract: | Through replacement of cations with neutral molecules of similar shape and polarizability in a highly conducting “metal-like” change-transfer organic conductor, the deliberate control of the electronic structure from a quarter to a half-filled band is possible. This goal has been achieved with the N-methylphenazinium (NMP) salt of the tetracyanoquinodimethane (TCNQ) anion by partial replacement of the cation with phenazine. A detailed study of the optical, electrical, and magnetic properties of these conducting molecular solids has lead to the evolution of a broad understanding of the physics of one-dimensional organic conductors and a reinterpretation of the mechanism of electron transport in such solids. Phenomena such as switching from a low coulomb repulsion two-chain conductor to a high coulomb repulsion one-chain conductor as well as soliton-assisted electron transport are observed. |