Singular crystalline beta'-layered topologies directed by ribbons of self-complementary amide...amide ring motifs in [EDT-TTF-(CONH(2))(2)](2)X (X = HSO(4)(-), ClO(4)(-), ReO(4)(-), AsF(6)(-)): coupled activation of ribbon curvature, electron interactions, and magnetic susceptibility

The deliberate design of a series of single crystals of conducting two-dimensional radical cation salts of o-bis(amide)-appended ethylenedithiotetrathiafulvalene, beta'-EDT-TTF-(CONH(2))(2)](2)X (X = HSO(4)(-), ClO(4)(-), ReO(4)(-), or AsF(6)(-)) and of their parent monocomponent solid EDT-TTF-(CONH(2))(2) is demonstrated and allows us to reach a level of prediction of the structure of molecular conductors. Their conductivity is activated with a gap of 1650 K and a sizable room-temperature conductivity of 0.15 S.cm(-)(1) (for X = ClO(4)(-)) and a singular spin susceptibility for a beta'-type salt that, in addition, changes very remarkably with the anion. The key design element is that of a recurrent, puckered ribbon constructed out of self-complementary, hydrogen-bonded amide...amide ring motifs whose minute modulations of curvature and shape throughout the series have been shown to correlate to very remarkable differences in the intrastack beta(HOMO)(-)(HOMO) interaction energies and changes in the density of states at the Fermi level and on to important differences of spin susceptibility behavior in a system where electron correlations are significant. The coupled activation of structure, electron interactions, and magnetic susceptibility discovered and discussed throughout the paper is unprecedented and is seen as a genuine expression of interfacial hydrogen-bond interactions onto the collective electronic properties.