Although flakes of two-dimensional (2D) heterostructures at the micrometer scale can be formed with adhesive-tape exfoliation methods, isolation of 2D flakes into monolayers is extremely time consuming because it is a trial-and-error process. Controlling the number of 2D layers through direct growth also presents difficulty because of the high nucleation barrier on 2D materials. We demonstrate a layer-resolved 2D material splitting technique that permits high-throughput production of multiple monolayers of wafer-scale (5-centimeter diameter) 2D materials by splitting single stacks of thick 2D materials grown on a single wafer. Wafer-scale uniformity of hexagonal boron nitride, tungsten disulfide, tungsten diselenide, molybdenum disulfide, and molybdenum diselenide monolayers was verified by photoluminescence response and by substantial retention of electronic conductivity. We fabricated wafer-scale van der Waals heterostructures, including field-effect transistors, with single-atom thickness resolution.

Interface-enhanced high-temperature superconductivity in one unit-cell (UC) FeSe films on SrTiO3(001) (STO) substrate has recently attracted much attention in condensed matter physics and material science. By combined in-situ scanning tunneling microscopy/spectroscopy (STM/STS) and ex-situ scanning transmission electron microscopy (STEM) studies, we report on atomically resolved structure including both lattice constants and actual atomic positions of the FeSe/STO interface under both non-superconducting and superconducting states. We observed TiO2 double layers (DLs) and significant atomic displacements in the top two layers of STO, lattice compression of the Se-Fe-Se triple layer, and relative shift between bottom Se and topmost Ti atoms. By imaging the interface structures under various superconducting states, we unveil a close correlation between interface structure and superconductivity. Our atomic-scale identification of FeSe/STO interface structure provides useful information on investigating the pairing mechanism of this interfaceenhanced high-temperature superconducting system.

Interface charge transfer and electron–phonon coupling have been suggested to play a crucial role in the recently discovered high-temperature superconductivity of single unit-cell FeSe films on SrTiO3. However, their origin remains elusive. Here, using ultraviolet photoemission spectroscopy and element-sensitive X-ray photoemission spectroscopy, we identify the strengthened Ti–O bond that contributes to the interface enhanced electron–phonon coupling and unveil the band bending at the FeSe/SrTiO3 interface that leads to the charge transfer from SrTiO3 to FeSe films. We also observe band renormalization that accompanies the onset of superconductivity. Our results not only provide valuable insights into the mechanism of the interface-enhanced superconductivity, but also point out a promising route toward designing novel superconductors in heterostructures with band bending-induced charge transfer and interfacial enhanced electron–phonon coupling.

Alkali-metal (potassium) adsorption on FeSe thin films with thickness from two unit cells (UC) to 4-UC on SrTiO 3 grown by molecular beam epitaxy is investigated with a low-temperature scanning tunneling microscope. At appropriate potassium coverage (0.2−0.3 monolayer), the tunneling spectra of the films all exhibit a superconducting-like gap larger than 11 meV (five times the gap value of bulk FeSe), and two distinct features of characteristic phonon modes at ~11 meV and ~21 meV. The results reveal the critical role of the interface enhanced electron-phonon coupling for possible high temperature superconductivity in the system and is consistent with recent theories. Our study provides compelling evidence for the conventional pairing mechanism for this type of heterostructure superconducting systems.

We report the time-resolved excited state ultrafast dynamics of single unit cell (1 UC) thick FeSe films on SrTiO_{3} (STO), with FeTe capping layers. By measuring the photoexcited quasiparticles' density and lifetime, we unambiguously identify a superconducting (SC) phase transition, with a transition temperature T_{c} of 68 (-5/+2)  K and a SC gap of Δ(0)=20.2±1.5  meV. The obtained electron-phonon coupling strength λ is as large as 0.48, demonstrating the likely crucial role of electron-phonon coupling in the high temperature superconductivity of the 1 UC FeSe on STO systems. We further find a 0.05 THz coherent acoustic phonon branch in the capping layer, which provides an additional decay channel to the gluing bosons.