RESUMEN
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 Bi2Se3 films 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.
RESUMEN
Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.
RESUMEN
Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi6Te10. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi2Te4 termination. In contrast, antiferromagnetic MnBi6Te10 exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi6Te10. We provide a conceptual framework where a cooperative interplay of these defects drives a delicate change of overall magnetic ground state energies and leads to tunable magnetic topological orders. Our work provides a clear pathway for nanoscale defect-engineering toward the realization of topological quantum phases.
RESUMEN
We present the development of a multi-resolution photoemission spectroscopy (MRPES) setup, which probes quantum materials in energy, momentum, space, and time. This versatile setup integrates three light sources in one photoemission setup and can conveniently switch between traditional angle-resolved photoemission spectroscopy (ARPES), time-resolved ARPES (trARPES), and micrometer-scale spatially resolved ARPES. It provides a first-time all-in-one solution to achieve an energy resolution of <4 meV, a time resolution of <35 fs, and a spatial resolution of â¼10 µm in photoemission spectroscopy. Remarkably, we obtain the shortest time resolution among the trARPES setups using solid-state nonlinear crystals for frequency upconversion. Furthermore, this MRPES setup is integrated with a shadow-mask assisted molecular beam epitaxy system, which transforms the traditional photoemission spectroscopy into a quantum device characterization instrument. We demonstrate the functionalities of this novel quantum material testbed using FeSe/SrTiO3 thin films and MnBi4Te7 magnetic topological insulators.
RESUMEN
The observation of replica bands by angle-resolved photoemission spectroscopy has ignited interest in the study of electron-phonon coupling at low carrier densities, particularly in monolayer FeSe/SrTiO_{3}, where the appearance of replica bands has motivated theoretical work suggesting that the interfacial coupling of electrons in the FeSe layer to optical phonons in the SrTiO_{3} substrate might contribute to the enhanced superconducting pairing temperature. Alternatively, it has also been recently proposed that such replica bands might instead originate from extrinsic final state losses associated with the photoemission process. Here, we perform a quantitative examination of replica bands in monolayer FeSe/SrTiO_{3}, where we are able to conclusively demonstrate that the replica bands are indeed signatures of intrinsic electron-boson coupling, and not associated with final state effects. A detailed analysis of the energy splittings and relative peak intensities between the higher-order replicas, as well as other self-energy effects, allows us to determine that the interfacial electron-phonon coupling in the system corresponds to a value of λ=0.19±0.02, providing valuable insights into the enhancement of superconductivity in monolayer FeSe/SrTiO_{3}. The methodology employed here can also serve as a new and general approach for making more rigorous and quantitative comparisons to theoretical calculations of electron-phonon interactions and coupling constants.
RESUMEN
We developed a table-top vacuum ultraviolet (VUV) laser with 113.778 nm wavelength (10.897 eV) and demonstrated its viability as a photon source for high resolution angle-resolved photoemission spectroscopy (ARPES). This sub-nanosecond pulsed VUV laser operates at a repetition rate of 10 MHz, provides a flux of 2 × 10(12) photons/s, and enables photoemission with energy and momentum resolutions better than 2 meV and 0.012 Å(-1), respectively. Space-charge induced energy shifts and spectral broadenings can be reduced below 2 meV. The setup reaches electron momenta up to 1.2 Å(-1), granting full access to the first Brillouin zone of most materials. Control over the linear polarization, repetition rate, and photon flux of the VUV source facilitates ARPES investigations of a broad range of quantum materials, bridging the application gap between contemporary low energy laser-based ARPES and synchrotron-based ARPES. We describe the principles and operational characteristics of this source and showcase its performance for rare earth metal tritellurides, high temperature cuprate superconductors, and iron-based superconductors.
RESUMEN
Ultrathin FeSe films grown on SrTiO3 substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. By using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO3 films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump-probe delay for 1-unit-cell, 3-unit-cell, and 60-unit-cell thick FeSe films. The frequencies of the coherent intensity oscillations increase from 5.00 ± 0.02 to 5.25 ± 0.02 THz with increasing film thickness. By comparing with previous works, we attribute this mode to the Se A1g phonon. The dominant mechanism for the phonon softening in 1-unit-cell thick FeSe films is a substrate-induced lattice strain. Our results demonstrate an abrupt phonon renormalization due to a lattice mismatch between the ultrathin film and the substrate.