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Ultrathin topological insulator membranes are building blocks of exotic quantum matter. However, traditional epitaxy of these materials does not facilitate stacking in arbitrary orders, while mechanical exfoliation from bulk crystals is also challenging due to the non-negligible interlayer coupling therein. Here we liberate millimeter-scale films of the topological insulator Bi2Se3, grown by molecular beam epitaxy, down to 3 quintuple layers. We characterize the preservation of the topological surface states and quantum well states in transferred Bi2Se3films using angle-resolved photoemission spectroscopy. Leveraging the photon-energy-dependent surface sensitivity, the photoemission spectra taken with 6 and 21.2 eV photons reveal a transfer-induced migration of the topological surface states from the top to the inner layers. By establishing clear electronic structures of the transferred films and unveiling the wave function relocation of the topological surface states, our work lays the physics foundation crucial for the future fabrication of artificially stacked topological materials with single-layer precision.

The de Gennes extrapolation length is a direction dependent measure of the spatial evolution of the pairing gap near the boundary of a superconductor and thus provides a viable means to probe its symmetry. It is expected to be infinite and isotropic for plain s-wave pairing, and finite and anisotropic for d-wave. Here, we synthesize single-layer FeSe films on SrTiO3(001) (STO) substrates by molecular beam epitaxy and measure the de Gennes extrapolation length by scanning tunneling microscopy/spectroscopy. We find a 40% reduction of the superconducting gap near specular [110]Feedges, yielding an extrapolation length of 8.0 nm. However, near specular [010]Feedges, the extrapolation length is nearly infinite. These findings are consistent with a phase changing pairing with 2-fold symmetry, indicating d-wave superconductivity. This is further supported by the presence of in-gap states near the specular [110]Feedges, but not the [010]Feedges. This work provides direct experimental evidence for d-wave superconductivity in single-layer FeSe/STO and demonstrates quasiparticle scattering at boundaries to be a viable phase sensitive probe of pairing symmetry in Fe-based superconductors.