Electron Doping of Proposed Kagome Quantum Spin Liquid Produces Localized States in the Band Gap

Carrier doping of quantum spin liquids is a long-proposed route to the emergence of high-temperature superconductivity. Electrochemical intercalation in kagome hydroxyl halide materials shows that samples remain insulating across a wide range of electron counts. Here we demonstrate through first-principles density-functional calculations, corrected for self-interaction, the mechanism by which electrons remain localized in various Zn-Cu hydroxyl halides, independent of the chemical identity of the dopant-the formation of polaronic states with attendant lattice displacements and a dramatic narrowing of bandwidth upon electron addition. The same theoretical method applied to electron doping in cuprate Nd2CuO4 correctly produces a metallic state when the initially formed polaron dissolves into an extended state. Our general findings explain the insulating behavior in a wide range of "doped" quantum magnets and demonstrate that new quantum spin liquid host materials are needed to realize metallicity borne of a spin liquid.