P{ 1 H} NMR), and DFT calculations (PDF) Coordinates of results of the theoretical calculations (XYZ) Accession CodesCCDC 1999367−1999369 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk

No abstract

No abstract

Thermodynamic measurements on the organic system of (DI-DCNQI)(2)(Ag(1-x)Cu(x)) (x = 0,0.05, 0.71, 0.90) were performed to study the change from the charge-ordered (CO) insulating state to the π-d hybridized metallic state. A thermal anomaly associated with the antiferromagnetic transition that occurred in the charge-ordered lattice was observed at 6.2 K from the temperature dependence of the heat capacity of (DI-DCNQI)(2)Ag. We have found that the magnetic entropy around the peak is only 1.5% of Rln2, corresponding to the full entropy expected for the formula unit of (DI-DCNQI)(2)Ag. This anomaly is suppressed down to about 3 K in the x = 0.05 sample owing to the disorders induced in the CO lattice. In the metallic concentration of x = 0.90, the low-temperature electronic heat capacity coefficient, γ was found to be enhanced by up to about 63.6 mJ K(-2) mol(-1) probably owing to the cooperative effect of π-d hybridization and intersite Coulomb interaction (V).