Molecular Doping Control at a Topological Insulator Surface: F4‑TCNQ on Bi2Se3

Recent electrical measurements have accessed transport in the topological surface state band of thin exfoliated samples of Bi2Se3 by removing the bulk n-type doping by contact with thin films of the molecular acceptor F4-TCNQ. Here we report on the film growth and interfacial electronic characterization of F4-TCNQ grown on Bi2Se3. Atomic force microscopy shows wetting layer formation followed by 3D island growth. X-ray photoelectron spectroscopy is consistent with this picture and also shows that charge transferred to the molecular layer is localized on nitrogen atoms. Ultraviolet photoelectron spectroscopy shows a work function increase and an upward shift of the valence band edge that suggest significant reduction in carrier density at the Bi2Se3 surface.