Knight shift tensors and π-spin densities in the organic metals αt-(BEDT-TTF)2I3 and (BEDT-TTF)2Cu(NCS)2

Abstract

13C-MASS spectra of pure BEDT-TTF and of the organic metals αt-(BEDT-TTF) 2I 3 and (BEDT-TTF) 2Cu(NCS)2 were recorded at νL - 68 MHz. Isotropic shifts and the principal components of the shift tensors were determined, respectively, from the center and spinning side bands. For pure BEDT-TTF which is a diamagnetic insolator, the measured shifts are chemica/ shifts, while for the organic metals they are the sum of chemical and Knight shifts. In each of the compounds the shifts are assigned in groups to the inner, middle and outer carbons of the BEDT-TTF molecule. For the organic metals the separation of the experimental shifts into chemical and Knight shifts is discussed. From the anisotropic part of the Knight shift tensors the π-spin densities at the carbon and sulphur positions of the BEDT-TTF molecule are inferred. The result is that the π-spin density of the unpaired hole is concentrated on the center part of the BEDT-TTF molecuIe, i.e. on the inner and middle carbons, and on the inner sulphurs. It is argued that the current density is concentrated on this part of the BEDT-TTF molecule as well.