Direct Imaging of Band Structure for Powdered Rhombohedral Boron Monosulfide by Microfocused ARPES.

Boron-based two-dimensional (2D) materials are an excellent platform for nanoelectronics applications. Rhombohedral boron monosulfide (r-BS) is attracting particular attention because of its unique layered crystal structure suitable for exploring various functional properties originating in the 2D nature. However, studies to elucidate its fundamental electronic states have been largely limited because only tiny powdered crystals were available, hindering a precise investigation by spectroscopy such as angle-resolved photoemission spectroscopy (ARPES). Here we report the direct mapping of the band structure with a tiny (∼20 × 20 µm2) r-BS powder crystal by utilizing microfocused ARPES. We found that r-BS is a p-type semiconductor with a band gap of >0.5 eV characterized by the anisotropic in-plane effective mass. The present results demonstrate the high applicability of micro-ARPES to tiny powder crystals and widen an opportunity to access the yet-unexplored electronic states of various novel materials.

Moiré-Assisted Realization of Octahedral MoTe2 Monolayer.

A current key challenge in 2D materials is the realization of emergent quantum phenomena in hetero structures via controlling the moiré potential created by the periodicity mismatch between adjacent layers, as highlighted by the discovery of superconductivity in twisted bilayer graphene. Generally, the lattice structure of the original host material remains unchanged even after the moiré superlattice is formed. However, much less attention is paid for the possibility that the moiré potential can also modify the original crystal structure itself. Here, it is demonstrated that octahedral MoTe2 which is unstable in bulk is stabilized in a commensurate MoTe2 /graphene hetero-bilayer due to the moiré potential created between the two layers. It is found that the reconstruction of electronic states via the moiré potential is responsible for this stabilization, as evidenced by the energy-gap opening at the Fermi level observed by angle-resolved photoemission and scanning tunneling spectroscopies. The present results provide a fresh approach to realize novel 2D quantum phases by utilizing the moiré potential.

Development of a versatile micro-focused angle-resolved photoemission spectroscopy system with Kirkpatrick-Baez mirror optics.

Angle-resolved photoemission spectroscopy using a micro-focused beam spot [micro-angle-resolved photoemission spectroscopy (ARPES)] is becoming a powerful tool to elucidate key electronic states of exotic quantum materials. We have developed a versatile micro-ARPES system based on the synchrotron radiation beam focused with a Kirkpatrick-Baez mirror optics. The mirrors are monolithically installed on a stage, which is driven with five-axis motion, and are vibrationally separated from the ARPES measurement system. Spatial mapping of the Au photolithography pattern on Si signifies the beam spot size of 10 µm (horizontal) × 12 µm (vertical) at the sample position, which is well suited to resolve the fine structure in local electronic states. Utilization of the micro-beam and the high precision sample motion system enables the accurate spatially resolved band-structure mapping, as demonstrated by the observation of a small band anomaly associated with tiny sample bending near the edge of a cleaved topological insulator single crystal.

Robust charge-density wave strengthened by electron correlations in monolayer 1T-TaSe2 and 1T-NbSe2.

Combination of low-dimensionality and electron correlation is vital for exotic quantum phenomena such as the Mott-insulating phase and high-temperature superconductivity. Transition-metal dichalcogenide (TMD) 1T-TaS2 has evoked great interest owing to its unique nonmagnetic Mott-insulator nature coupled with a charge-density-wave (CDW). To functionalize such a complex phase, it is essential to enhance the CDW-Mott transition temperature TCDW-Mott, whereas this was difficult for bulk TMDs with TCDW-Mott < 200 K. Here we report a strong-coupling 2D CDW-Mott phase with a transition temperature onset of ~530 K in monolayer 1T-TaSe2. Furthermore, the electron correlation derived lower Hubbard band survives under external perturbations such as carrier doping and photoexcitation, in contrast to the bulk counterpart. The enhanced Mott-Hubbard and CDW gaps for monolayer TaSe2 compared to NbSe2, originating in the lattice distortion assisted by strengthened correlations and disappearance of interlayer hopping, suggest stabilization of a likely nonmagnetic CDW-Mott insulator phase well above the room temperature. The present result lays the foundation for realizing monolayer CDW-Mott insulator based devices operating at room temperature.

Dirac semimetal phase and switching of band inversion in XMg2Bi2 (X = Ba and Sr).

Topological Dirac semimetals (TDSs) offer an excellent opportunity to realize outstanding physical properties distinct from those of topological insulators. Since TDSs verified so far have their own problems such as high reactivity in the atmosphere and difficulty in controlling topological phases via chemical substitution, it is highly desirable to find a new material platform of TDSs. By angle-resolved photoemission spectroscopy combined with first-principles band-structure calculations, we show that ternary compound BaMg2Bi2 is a TDS with a simple Dirac-band crossing around the Brillouin-zone center protected by the C3 symmetry of crystal. We also found that isostructural SrMg2Bi2 is an ordinary insulator characterized by the absence of band inversion due to the reduction of spin-orbit coupling. Thus, XMg2Bi2 (X = Sr, Ba, etc.) serves as a useful platform to study the interplay among crystal symmetry, spin-orbit coupling, and topological phase transition around the TDS phase.