Millimeter-Scale, Atomically Controlled 2D Topological Insulators Revealed by Multimodal Spectroscopy

Quantum spin Hall insulators, also known as 2D topological insulators, are crucial 2D systems hosting topologically protected edge states. The working temperature of this topological quantum phase is dictated by the inverted bandgap. However, the previously identified large-gap 2D topological insulators are either extremely chemically unstable or cannot be made with atomistic precision over macroscopic scales. Here, we establish two-quintuple-layer Bi2Te3 and MnBi2Te4/Bi2Te3 heterostructures as atomically controlled, millimeter-scale 2D topological insulators, enabled by precision layer-by-layer growth that yields a carpet-like morphology extending coherently over macroscopic distances. This carpet-like growth mode renders the films amenable to mechanical exfoliation and subsequent wet or dry transfer. Multimodal spectroscopies and microscopies reveal the integer-layer-tuned electronic structure of (Bi2Te3)n in excellent agreement with theory. Photon-energy-dependent photoemission and time-resolved photoemission identify band inversion and band dynamics, respectively, while scanning tunneling spectroscopy resolves topological edge states that are characteristic of the 2D topological insulator phase. Thickness- and photon-energy-dependent photoemission further validate MnBi2Te4/Bi2Te3 as a robust 2D topological insulator. The large inverted gaps of ∼100 meV in (Bi2Te3)2 and ∼150 meV in MnBi2Te4/Bi2Te3 suggest operation near ambient temperature. These results define a scalable materials platform for next-generation, low-loss quantum and energy-efficient devices.