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Abstract:

Alkali-doped fullerides are strongly correlated organic superconductors that exhibit high transition temperatures, exceptionally large critical magnetic fields, and a number of other unusual properties. The proximity to a Mott insulating phase is thought to be a crucial ingredient of the underlying physics and may also affect precursors of superconductivity in the normal state above T_C. We report on the observation of a sizable magneto-thermoelectric (Nernst) effect in the normal state of K₃C₆₀, which displays the characteristics of superconducting fluctuations. This nonquasiparticle Nernst effect emerges from an ordinary quasiparticle background below a temperature of 80 K, far above T_C = 20 K. At the lowest fields and close to T_C, the scaling of the effect is captured by a model based on Gaussian fluctuations. The behavior at higher magnetic fields displays a symmetry between the magnetic length and the correlation length of the system. The temperature up to which we observe fluctuations is exceptionally high for a three-dimensional isotropic system, where fluctuation effects are expected to be suppressed.

Abstract:

Owing to the unique chemical and electronic properties arising from 3d‐electrons, substitution with transition metal ions is one of the key routes for engineering new functionalities into materials. While this approach has been used extensively in complex metal oxide perovskites, metal halide perovskites have largely resisted facile isovalent substitution. In this work, it is demonstrated that the substitution of Co2+ into the lattice of methylammonium lead triiodide imparts magnetic behavior to the material while maintaining photovoltaic performance at low concentrations. In addition to comprehensively characterizing its magnetic properties, the Co2+ ions themselves are utilized as probes to sense the local electronic environment of Pb in the perovskite, thereby revealing the nature of their incorporation into the material. A comprehensive understanding of the effect of transition metal incorporation is provided, thereby opening the substitution gateway for developing novel functional perovskite materials and devices for future technologies.