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Three dimensional (3D) topological insulators are quantum materials with aspin-orbit induced bulk insulating gap that exhibit quantum-Hall-like phenomenain the absence of applied magnetic fields. The proposed applications oftopological insulators in device geometries rely on the ability to tune thechemical potential on their surfaces in the vicinity of the Dirac node. Here,we demonstrate a suite of surface control methods based on a combination ofphoto-doping and molecular-doping to systematically tune the Dirac fermiondensity on the topological (111) surface of Bi2Te3. Their efficacy isdemonstrated via direct electronic structure topology measurements using highresolution angle-resolved photoemission spectroscopy (ARPES). These resultsopen up new opportunities for probing topological behavior of Dirac electronson the Bi2Te3 surface. At least one of the methods demonstrated here can besuccessfully applied to other topological insulators such as the Bi{1-x}Sb{x},Sb2Te3 and Bi2Se3 which will be shown elsewhere. More importantly, our methodsof topological surface state manipulation demonstrated here are highly suitablefor future spectroscopic studies of topological phenomena which will complementthe transport results gained from the traditional electrical gating techniques.

Topological Control: Systematic control of topological insulator Dirac fermion density on the surface of Bi2Te3