Nearest-neighbor Kitaev exchange blocked by charge order in electron-doped α-RuCl3

A quantum spin liquid might be realized in α-RuCl3, a honeycomb-lattice magnetic material with substantial spin-orbit coupling. Moreover, α-RuCl3 is a Mott insulator, which implies the possibility that novel exotic phases occur upon doping. Here, we study the electronic structure of this material when intercalated with potassium by photoemission spectroscopy, electron energy loss spectroscopy, and density functional theory calculations. We obtain a stable stoichiometry at K0.5RuCl3. This gives rise to a peculiar charge is proportionation into formally Ru2+ (4d6) and Ru3+ (4d5). Every Ru 4d5 site with one hole in the t2g shell is surrounded by nearest neighbors of 4d6 character, where the t2g level is full and magnetically inert. Thus, each type of Ru site forms a triangular lattice, and nearest-neighbor interactions of the original honeycomb are blocked.