The symmetry of the superconducting order parameter in quasi-two-dimensional bis-ethylenedithio-tetrathiafulvalene (BEDT-TTF) organic superconductors is a subject of ongoing debate. We report ab initio density-functional-theory calculations for a number of organic superconductors containing κ-type layers. Using projective Wannier functions, we derive the parameters of a common low-energy Hamiltonian based on individual BEDT-TTF molecular orbitals. In a random-phase approximation spin-fluctuation approach, we investigate the evolution of the superconducting pairing symmetry within this model, and we point out a phase transition between extended s+dx2-y2 and dxy symmetry. We discuss the origin of the mixed order parameter and the relation between the realistic molecule description and the widely used dimer approximation. Based on our ab initio calculations, we position the investigated materials in the obtained molecule model phase diagram, and we simulate scanning tunneling spectroscopy experiments for selected cases. Our calculations show that many κ-type materials lie close to the phase-transition line between the two pairing symmetry types found in our calculation, possibly explaining the multitude of contradictory experiments in this field.
ASJC Scopus subject areas
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics