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It has long been an ultimate goal to introduce chemical doping at the atomiclevel to precisely tune properties of materials. Two-dimensional materials havenatural advantage because of its highly-exposed surface atoms, however, it isstill a grand challenge to achieve this goal experimentally. Here, wedemonstrate the ability to introduce chemical doping in graphene withatomic-level precision by controlling chemical adsorption of individual Seatoms, which are extracted from the underneath WSe2, at the interface ofgraphene-WSe2 heterostructures. Our scanning tunneling microscopy (STM)measurements, combined with first-principles calculations, reveal thatindividual Se atoms can chemisorbed on three possible positions in graphene,which generate distinct pseudospin-mediated atomic-scale vortices in graphene.We demonstrate that the chemisorbed positions of individual Se atoms can bemanipulated by STM tip, which enables us to achieve atomic-scale controllingquantum interference of the pseudospin-mediated vortices in graphene. Thisresult offers the promise of controlling properties of materials throughchemical doping with atomic-level precision.

Tunable interfacial chemisorption with atomic-level precision in a graphene WSe2 heterostructure