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The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi2Te4. Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but over-estimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi2Te4. Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics., Comment: 19 pages, 4 figures

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 topological insulator Bi$_2$Se$_3$, 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 Bi$_{2}$Se$_{3}$ films using angle-resolved photoemission spectroscopy. Leveraging the photon-energy-dependent surface sensitivity, the photoemission spectra taken with $6$ eV 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 wavefunction relocation of the topological surface states, our work paves the physics foundation crucial for the future fabrication of artificially stacked topological materials with single-layer precision., Comment: 4 figures

Layer-by-layer material engineering has enabled exotic quantum phenomena such as interfacial superconductivity and the quantum anomalous Hall effect. Meanwhile, deciphering electronic states layer-by-layer remains a fundamental scientific challenge. This is exemplified by the difficulty in understanding the layer origins of topological electronic states in magnetic topological insulators, which is key to understanding and controlling topological quantum phases. Here, we report a layer-encoded frequency-domain ARPES experiment on a magnetic topological insulator (MnBi2Te4)(Bi2Te3) to characterize the layer origins of electronic states. Infrared laser excitations launch coherent lattice vibrations with the layer index encoded by the vibration frequency; photoemission spectroscopy tracks the electron dynamics, where the layer information is decoded in the frequency domain. This layer-frequency correspondence reveals a surprising wavefunction relocation of the topological surface state from the top magnetic layer into the buried second layer, reconciling the controversy over the vanishing broken-symmetry energy gap in (MnBi2Te4)(Bi2Te3) and its related compounds. The layer-frequency correspondence can be harnessed to disentangle electronic states layer-by-layer in a broad class of van der Waals superlattices.

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 micron-scale spatially resolved ARPES ($\mu$ARPES). It provides a first-time all-in-one solution to achieve an energy resolution $< 4$ meV, a time resolution $< 35$ fs, and a spatial resolution $\sim 10$ $\mu$m 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/SrTiO$_3$ thin films and MnBi$_4$Te$_7$ magnetic topological insulators.

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 MnBi$_6$Te$_{10}$. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi$_2$Te$_4$ termination. In contrast, antiferromagnetic MnBi$_6$Te$_{10}$ exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi$_6$Te$_{10}$. 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 towards the realization of topological quantum phases., Comment: 22 pages, 3 figures

Despite the rapid progress in understanding the first intrinsic magnetic topological insulator MnBi$_2$Te$_4$, its electronic structure remains a topic under debates. Here we perform a thorough spectroscopic investigation into the electronic structure of MnBi$_2$Te$_4$ via laser-based angle-resolved photoemission spectroscopy. Through quantitative analysis, we estimate an upper bound of 3 meV for the gap size of the topological surface state. Furthermore, our circular dichroism measurements reveal band chiralities for both the topological surface state and quasi-2D bands, which can be well reproduced in a band hybridization model. A numerical simulation of energy-momentum dispersions based on a four-band model with an additional step potential near the surface provides a promising explanation for the origin of the quasi-2D bands. Our study represents a solid step forward in reconciling the existing controversies in the electronic structure of MnBi$_2$Te$_4$, and provides an important framework to understand the electronic structures of other relevant topological materials MnBi$_{2n}$Te$_{3n+1}$., Comment: 4 figures

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]Fe edges, yielding an extrapolation length of 8.0 nm. However, near specular [010]Fe edges 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]Fe edges, but not the [010]Fe edges. 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., Comment: 18 pages, 4 figures

Current generated spin polarization in topological insulator (TI) surface states due to spin-momentum locking has been detected recently using ferromagnet/tunnel barrier contacts, where the projection of the TI spin onto the magnetization of the ferromagnet is measured as a voltage. However, opposing signs of the spin voltage have been reported, which had been tentatively attributed to the coexistence of trivial two-dimensional electron gas states on the TI surface which may exhibit opposite current-induced polarization than that of the TI Dirac surface states. Models based on electrochemical potential have been presented to determine the sign of the spin voltage expected for the TI surface states. However, these models neglect critical experimental parameters which also affect the sign measured. Here we present a Mott two-spin current resistor model which takes into account these parameters such as spin-dependent interface resistances, and show that such inclusion can lead to a crossing of the voltage potential profiles for the spin-up and spin-down electrons within the channel, which can lead to measured spin voltages of either sign. These findings offer a resolution of the ongoing controversy regarding opposite signs of spin signal reported in the literature, and highlight the importance of including realistic experimental parameters in the model., Comment: 17 pages, 4 figures, Scientific Report, in press

The surface of a topological crystalline insulator (TCI) carries an even number of Dirac cones protected by crystalline symmetry. We epitaxially grew high quality Pb$_{1-x}$Sn$_x$Te(111) films and investigated the TCI phase by in-situ angle-resolved photoemission spectroscopy. Pb$_{1-x}$Sn$_x$Te(111) films undergo a topological phase transition from trivial insulator to TCI via increasing the Sn/Pb ratio, accompanied by a crossover from n-type to p-type doping. In addition, a hybridization gap is opened in the surface states when the thickness of film is reduced to the two-dimensional limit. The work demonstrates an approach to manipulating the topological properties of TCI, which is of importance for future fundamental research and applications based on TCI.