ABSTRACT
We have investigated the infrared spectra of the quarter-filled charge-ordered insulators δ-(EDT-TTF-CONMe2)2X (X= AsF6, Br) along all three crystallographic directions in the temperature range from 300 to 10 K. DFT-assisted normal mode analysis of the neutral and ionic EDT-TTF-CONMe2 molecule allows us to assign the experimentally observed intramolecular modes and to obtain relevant information on the charge ordering and intramolecular interactions. From frequencies of charge-sensitive vibrations we deduce that the charge-ordered state is already present at room temperature and does not change on cooling, in agreement with previous NMR measurements. The spectra taken along the stacking direction clearly show features of vibrational overtones excited due to the anharmonic electronic molecule potential caused by the large charge disproportionation between the molecular sites. The shift of certain vibrational modes indicates the onset of the structural transition below 200 K.
ABSTRACT
The layered organic compounds, kappa-(BEDT-TTF)2Cu[N(CN)2]X X=Cl, Br) are metals at ambient temperatures. At low temperatures, the Cl compound is a weakly ferromagnetic Mott insulator while the isostructural Br compound is a superconductor. We find by conduction electron spin resonance and antiferromagnetic resonance (AFMR) an extreme anisotropy of spin transport and magnetic interactions in these materials. In the metallic state spin diffusion is confined to single molecular layers within the spin lifetime of 10(-9) s. Electrons diffuse several hundreds of nm without interlayer hopping. In the magnetically ordered insulating phase of the Cl compound we observe and calculate the four AFMR modes of the weakly coupled single molecular layers. The interplane exchange field is comparable or less than the typically 1 mT dipolar field and almost 10(6) times less than the intralayer exchange field.
