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Utilizing the powerful combination of molecular-beam epitaxy (MBE) and angle-resolved photoemission spectroscopy (ARPES), we produce and study the effect of different terminating layers on the electronic structure of the metallic delafossite PdCoO 2 . Attempts to introduce unpaired electrons and synthesize new antiferromagnetic metals akin to the isostructural compound PdCrO 2 have been made by replacing cobalt with iron in PdCoO 2 films grown by MBE. Using ARPES, we observe similar bulk bands in these PdCoO 2 films with Pd-, CoO 2 -, and FeO 2 -termination. Nevertheless, Pd- and CoO 2 -terminated films show a reduced intensity of surface states. Additionally, we are able to epitaxially stabilize PdFe x Co 1− x O 2 films that show an anomaly in the derivative of the electrical resistance with respect to temperature at 20 K, but do not display pronounced magnetic order. 

Transition metal dichalcogenide heterostructures show strong interactions and can imprint a moiré potential to a separate layer. 

Tomographic spectroscopy reveals how the properties of topological materials can be engineered at interfaces. 

Topological materials are derived from the interplay between symmetry and topology. Advances in topological band theories have led to the prediction that the antiperovskite oxide Sr₃SnO is a topological crystalline insulator, a new electronic phase of matter where the conductivity in its (001) crystallographic planes is protected by crystallographic point group symmetries. Realization of this material, however, is challenging. Guided by thermodynamic calculations, a deposition approach is designed and implemented to achieve the adsorption‐controlled growth of epitaxial Sr₃SnO single‐crystal films by molecular‐beam epitaxy (MBE). In situ transport and angle‐resolved photoemission spectroscopy measurements reveal the metallic and electronic structure of the as‐grown samples. Compared with conventional MBE, the used synthesis route results in superior sample quality and is readily adapted to other topological systems with antiperovskite structures. The successful realization of thin films of Sr₃SnO opens opportunities to manipulate topological states by tuning symmetries via strain engineering and heterostructuring.