LAUSR

The ability to assemble layers of two-dimensional (2D) materials to form permutations of van der Waals heterostructures provides significant opportunities in materials design and synthesis. Interlayer interactions can enable desired properties and functionality, and understanding such interactions is essential to that end. Here we report formation of interlayer exciton-phonon bound states in Bi2Se3/WS2 heterostructures, where the Bi2Se3 A1(3) surface phonon, a mode particularly susceptible to electron-phonon coupling, is imprinted onto the excitonic emission of the WS2. The exciton-phonon bound state (or exciton-phonon quasiparticle) presents itself as evenly separated peaks superposed on the WS2 excitonic photoluminescence spectrum, whose periodic spacing corresponds to the A1(3) surface phonon energy. Low-temperature polarized Raman spectroscopy of Bi2Se3 reveals intense surface phonons and local symmetry breaking that allows the A1(3) surface phonon to manifest in otherwise forbidden scattering geometries. Our work advances knowledge of the complex interlayer van der Waals interactions and facilitates technologies that combine the distinctive transport and optical properties from separate materials into one device for possible spintronics, valleytronics, and quantum computing applications.