Electron correlation in theκ-phase family of BEDT-TTF compounds studied byC13NMR, where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene

Abstract
A C13 NMR study on κ=(BEDTTTF)2X (X=Cu(NCS)2, Cu[N(CN)2]Br, and Cu[N(CN)2]Cl) is reported, where BEDT-TTF is bis(ethylenedithio)tetrathiafulvalene. The superconducting salts of X=Cu(NCS)2 and Cu[N(CN)2]Br show anamalous enhancement in nuclear spin-lattice relaxation rate T11 around 50 K, in spite of monotonic temperature dependence of the anisotropic Knight shift. On the other hand, the insulating salt of X=Cu[N(CN)2]Cl exhibits a divergent peak in (T1T)1 at 26-27 K, which is confirmed as a manifestation of an antiferromagnetic transition by broadening of the NMR line. Above 27 K, T11 shows a temperature dependence typical of critical magnetic fluctuations. The (T1T)1 and the line shape showed nearly the same profile for these three salts above 60 K, that gives experimental evidence for a correspondence between the anomalous enhancement of (T1T)1 in the superconducting salts and antiferromagnetic fluctuations established in the insulating salt of κ type. The present results demonstrate the presence of strong electron correlation in both superconducting and insulating salts. Analytical expressions of T1 and the Knight shift of the C13 NMR for κ(BEDTTTF)2X are given, which are general formulas applicable to other pπ electronic systems.