Fulleride superconductivity tuned by elastic strain due to cation compositional disorder

Abstract

Dynamical fluctuations of the elastic strain in strongly correlated systems are known to affect the onset of metal-to-insulator or superconducting transitions. Here we report their effect on the properties of a family of bandwidth-controlled alkali-intercalated fullerene superconductors. We introduce elastic strain through static local structural disorder in a systematic and controllable way in the fcc-structured KxCs3-xC60 (with potassium content, 0.22 <= x(K) <= 2) series of compositions by utilizing the difference in size between the K+ and Cs+ co-dopants. The occurrence of the crossover from the Mott-Jahn-Teller insulating (MJTI) state into the strongly correlated Jahn-Teller metal (JTM) on cooling is evidenced for the compositions with x(K) < 1.28 by both synchrotron X-ray powder diffraction (SXRPD) - anomalous reduction of the unit cell volume - and Cs-133 NMR spectroscopy - sudden suppression in the Cs-133 spin-lattice relaxation rates. The emerging superconducting state with a maximum critical temperature, T-c = 30.9 K shows a characteristic dome-like dependence on the unit-cell volume or equivalently, on the ratio between the on-site Coulomb repulsion, U, and the bandwidth, W. However, compared to the parent Cs3C60 composition in which cation disorder effects are completely absent, the maximum T-c is lower by similar to 12%. The reduction in T-c displays a linear dependence on the variance of the tetrahedral-site cation size, sigma(2)(T), thus establishing a clear link between structural-disorder-induced attenuation of critical elastic strain fluctuations and the electronic ground state.