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.

Fermiology and Origin of T_{c} Enhancement in a Kagome Superconductor Cs(V_{1-x}Nb_{x})_{3}Sb_{5}.

Kagome metals AV_{3}Sb_{5} (A=K, Rb, and Cs) exhibit a characteristic superconducting ground state coexisting with a charge density wave (CDW), whereas the mechanisms of the superconductivity and CDW have yet to be clarified. Here we report a systematic angle-resolved photoemission spectroscopy (ARPES) study of Cs(V_{1-x}Nb_{x})_{3}Sb_{5} as a function of Nb content x, where isovalent Nb substitution causes an enhancement of superconducting transition temperature (T_{c}) and the reduction of CDW temperature (T_{CDW}). We found that the Nb substitution shifts the Sb-derived electron band at the Γ point downward and simultaneously moves the V-derived band around the M point upward to lift up the saddle point (SP) away from the Fermi level, leading to the reduction of the CDW-gap magnitude and T_{CDW}. This indicates a primary role of the SP density of states to stabilize the CDW. The present result also suggests that the enhancement of superconductivity by Nb substitution is caused by the cooperation between the expansion of the Sb-derived electron pocket and the recovery of the V-derived density of states at the Fermi level.

Dichotomy of superconductivity between monolayer FeS and FeSe.

The discovery of high-temperature (T c) superconductivity in monolayer FeSe on SrTiO3 raised a fundamental question: Whether high T c is commonly realized in monolayer iron-based superconductors. Tetragonal FeS is a key material to resolve this issue because bulk FeS is a superconductor with T c comparable to that of isostructural FeSe. However, difficulty in synthesizing tetragonal monolayer FeS due to its metastable nature has hindered further investigations. Here we report elucidation of band structure of monolayer FeS on SrTiO3, enabled by a unique combination of in situ topotactic reaction and molecular-beam epitaxy. Our angle-resolved photoemission spectroscopy on FeS and FeSe revealed marked similarities in the electronic structure, such as heavy electron doping and interfacial electron-phonon coupling, both of which have been regarded as possible sources of high T c in FeSe. However, surprisingly, high-T c superconductivity is absent in monolayer FeS. This is linked to the weak superconducting pairing in electron-doped multilayer FeS in which the interfacial effects are absent. Our results strongly suggest that the cross-interface electron-phonon coupling enhances T c only when it cooperates with the pairing interaction inherent to the superconducting layer. This finding provides a key insight to explore heterointerface high-T c superconductors.

Nanomosaic of Topological Dirac States on the Surface of Pb5Bi24Se41 Observed by Nano-ARPES.

We have performed scanning angle-resolved photoemission spectroscopy with a nanometer-sized beam spot (nano-ARPES) on the cleaved surface of Pb5Bi24Se41, which is a member of the (PbSe)5(Bi2Se3)3 m homologous series (PSBS) with m = 4 consisting of alternate stacking of the topologically trivial insulator PbSe bilayer and four quintuple layers (QLs) of the topological insulator Bi2Se3. This allows us to visualize a mosaic of topological Dirac states at a nanometer scale coming from the variable thickness of the Bi2Se3 nanoislands (1-3 QLs) that remain on top of the PbSe layer after cleaving the PSBS crystal, because the local band structure of topological origin changes drastically with the thickness of the Bi2Se3 nanoislands. A comparison of the local band structure with that in ultrathin Bi2Se3 films on Si(111) gives us further insights into the nature of the observed topological states. This result demonstrates that nano-ARPES is a very useful tool for characterizing topological heterostructures.

Observation of Chiral Fermions with a Large Topological Charge and Associated Fermi-Arc Surface States in CoSi.

Topological semimetals materialize a new state of quantum matter where massless fermions protected by a specific crystal symmetry host exotic quantum phenomena. Distinct from well-known Dirac and Weyl fermions, structurally chiral topological semimetals are predicted to host new types of massless fermions characterized by a large topological charge, whereas such exotic fermions are yet to be experimentally established. Here, by using angle-resolved photoemission spectroscopy, we experimentally demonstrate that a transition-metal silicide CoSi hosts two types of chiral topological fermions, a spin-1 chiral fermion and a double Weyl fermion, in the center and corner of the bulk Brillouin zone, respectively. Intriguingly, we found that the bulk Fermi surfaces are purely composed of the energy bands related to these fermions. We also find the surface states connecting the Fermi surfaces associated with these fermions, suggesting the existence of the predicted Fermi-arc surface states. Our result provides the first experimental evidence for the chiral topological fermions beyond Dirac and Weyl fermions in condensed-matter systems, and paves the pathway toward realizing exotic electronic properties associated with unconventional chiral fermions.

Expression of recombinant organophosphorus hydrolase in the original producer of the enzyme, Sphingobium fuliginis ATCC 27551.

The plasmid encoding His-tagged organophosphorus hydrolase (OPH) cloned from Sphingobium fuliginis was modified to be transferred back to this bacterium. The replication function of S. amiense plasmid was inserted at downstream of OPH gene, and S. fuliginis was transformed with this plasmid. The transformant produced larger amount of active OPH with His-tag than E. coli.

Quasi-Homoepitaxial Growth of Highly Strained Alkali-Metal Ultrathin Films on Kagome Superconductors.

Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high-quality thin films, its application to studying strain-induced structural phases is limited. Contrary to this general belief, here the quasi-homoepitaxial growth of Cs and Rb thin films is reported with substantial in-plane compressive strain. This is achieved by utilizing the alkali-metal layer existing in bulk crystal of kagome metals AV3Sb5 (A = Cs and Rb) as a structural template. The angle-resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness-dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face-centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi-homoepitaxy, and pave the way for investigating many-body interactions in Fermi liquids with tunable dimensionality.

Development of Ar gas cluster ion beam system for surface preparation in angle-resolved photoemission spectroscopy.

Gas cluster ion beam (GCIB) sputtering has a high potential for obtaining clean and flat surfaces on materials without causing structural or compositional damage. We have developed an Ar cluster GCIB system for surface preparation in angle-resolved photoemission spectroscopy (ARPES). The constructed GCIB system is compatible with ultrahigh vacuum and achieves a beam current of 10 µA. We examined the usefulness of our GCIB system for high surface-sensitive ARPES measurements by applying it to several representative materials, e.g., Sb, GaAs, and Te. The results show that the constructed GCIB system is very useful for preparing a clean flat surface on crystals, widening opportunities for precise ARPES measurements for materials whose crystal surfaces or orientations are hardly obtained by a simple cleaving method.

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.

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.

Ultrathin Bismuth Film on High-Temperature Cuprate Superconductor Bi2Sr2CaCu2O8+δ as a Candidate of a Topological Superconductor.

One of the key challenges in condensed-matter physics is to establish a topological superconductor that hosts exotic Majorana fermions. Although various heterostructures consisting of conventional BCS (Bardeen-Cooper-Schrieffer) superconductors as well as doped topological insulators were intensively investigated, no conclusive evidence for Majorana fermions has been provided. This is mainly because of their very low superconducting transition temperatures ( Tc) and small superconducting-gap magnitude. Here, we report a possible realization of topological superconductivity at very high temperatures in a hybrid of Bi(110) ultrathin film and copper oxide superconductor Bi2Sr2CaCu2O8+δ (Bi2212). Using angle-resolved photoemission spectroscopy and scanning tunneling microscopy, we found that three-bilayer-thick Bi(110) on Bi2212 exhibits a proximity-effect-induced s-wave energy gap as large as 7.5 meV which persists up to Tc of Bi2212 (85 K). The small Fermi energy and strong spin-orbit coupling of Bi(110), together with the large pairing gap and high Tc, make this system a prime candidate for exploring stable Majorana fermions at very high temperatures.