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The recent discovery of the persistence of long-range magnetic order when vander Waals layered magnets are thinned towards the monolayer limit has provideda tunable platform for the engineering of novel magnetic structures anddevices. Here, we study the evolution of the electronic structure of CrGeTe$_3$as a function of electron doping in the surface layer. From angle-resolvedphotoemission spectroscopy, we observe spectroscopic fingerprints that thiselectron doping drives a marked increase in $T_\mathrm{C}$, reaching valuesmore than double that of the undoped material, in agreement with recent studiesusing electrostatic gating. Together with density functional theorycalculations and Monte Carlo simulations, we show that, surprisingly, theincreased $T_\mathrm{C}$ is mediated by the population of spin-minority Cr$t_{2g}$ states, forming a half-metallic 2D electron gas at the surface. Weshow how this promotes a novel variant of double exchange, and unlocks asignificant influence of the Ge -- which was previously thought to beelectronically inert in this system -- in mediating Cr-Cr exchange.

Charge doping into spin minority states mediates doubling of $T_\mathrm{C}$ in ferromagnetic CrGeTe$_3$