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Kagome superconductors AV3Sb5 (A = K, Rb, Cs) exhibit a characteristic superconducting and charge-density wave (CDW) phase diagram upon carrier doping and chemical substitution. However, the key electronic states responsible for such a phase diagram have yet to be clarified. Here we report a systematic micro-focused angle-resolved photoemission spectroscopy (ARPES) study of Cs(V1-xCrx)3Sb5 as a function of Cr content x, where Cr substitution causes monotonic reduction of superconducting and CDW transition temperatures. We found that the V-derived bands forming saddle points at the M point and Dirac nodes along high-symmetry cuts show an energy shift due to electron doping by Cr substitution, whereas the Sb-derived electron band at the Gamma point remains almost unchanged, signifying an orbital-selective band shift. We also found that band doubling associated with the emergence of three-dimensional CDW identified at x = 0 vanishes at x = 0.25, in line with the disappearance of CDW. A comparison of band diagrams among Ti-, Nb-, and Cr-substituted Cs(V1-xCrx)3Sb5 suggests the importance to simultaneously take into account the two saddle points at the M point and their proximity to the Fermi energy, to understand the complex phase diagram against carrier doping and chemical pressure., Comment: 7 pages, 4 figures

Antiferromagnetic topological insulators (AF TIs) are predicted to exhibit exotic physical properties such as gigantic optical and topological magnetoelectric responses. While a key to achieving such phenomena relies on how to break the symmetry protecting the Dirac-cone surface state (SS) and acquire the mass of Dirac fermions, the mechanism has yet to be clarified. To address this issue, we carried out micro-focused angle-resolved photoemission spectroscopy for GdBi hosting the type-II AF order, and uncovered the stripe-type 2$\times$1 reconstruction of the Fermi surface associated with the AF band folding. Intriguingly, in contrast to NdBi with the type-I AF order displaying the surface-selective Dirac-fermion mass, GdBi shows massless behavior irrespective of AF domains due to the robust topological protection. These results strongly suggest a crucial role of the ThetaTD (time-reversal and translational) symmetry to create the Dirac-fermion mass in AF TIs., Comment: 18 pages, 5 figures

We study two related universal anomalies of the spectral function of cuprates, so called waterfall and high-energy kink features, by a combined cellular dynamical mean-field theory and angle-resolved photoemission study for the oxychloride Na$_x$Ca$_{2-x}$CuO$_2$Cl$_2$ (Na-CCOC). Tracing their origin back to an interplay of spin-polaron and local correlation effects both in undoped and hole-doped (Na-)CCOC, we establish them as a universal crossover between regions differing in the momentum dependence of the coupling and not necessarily in the related quasiparticles' energies. The proposed scenario extends to doping levels coinciding with the cuprate's superconducting dome and motivates further investigations of the fate of spin-polarons in the superconducting phase., Comment: Main text (8 pages, 4 figures) with supplemental information (7 pages, 8 figures, 1 table)

The spin-dependent band structure of CoS$_2$ which is a candidate for a half-metallic ferromagnet was investigated by both spin- and angle-resolved photoemission spectroscopy and theoretical calculations, in order to reappraise the half-metallicity and electronic correlations. We determined the three-dimensional Fermi surface and the spin-dependent band structure. As a result, we found that a part of the minority spin bands is on the occupied side in the vicinity of the Fermi level, providing spectroscopic evidence that CoS$_2$ is not but very close to a half-metal. Band calculations using density functional theory with generalized gradient approximation showed a good agreement with the observed majority spin $e_g$ bands, while it could not explain the observed band width of the minority-spin eg bands. On the other hand, theoretical calculations using dynamical mean field theory could better reproduce the strong mass renormalization in the minority-spin $e_g$ bands. All those results strongly suggest the presence of anomalously enhanced spin-dependent electron correlation effects on the electronic structure in the vicinity of the half-metallic state. We also report the temperature dependence of the electronic structure across the Curie temperature and discuss the mechanism of the thermal demagnetization. Our discovery of the anomalously large spin-dependent electronic correlations not only demonstrates a key factor in understanding the electronic structure of half-metals but also provides a motivation to improve theoretical calculations on spin-polarized strongly correlated systems., Comment: 53 pages, 25 figures, 1 table

We have performed micro-focused angle-resolved photoemission spectroscopy on NdSb which exhibits the type-I antiferromagnetism below TN = 16 K. We succeeded in selectively observing the band structure for all three types of single-q antiferromagnetic (AF) domains at the surface. We found that two of the three surfaces whose AF-ordering vector lies within the surface plane commonly show twofold symmetric surface states (SSs) around the bulk-band edges, whereas the other surface with an out-of-plane AF-ordering vector displays fourfold symmetric shallow electronlike SS at the Brillouin-zone center. We suggest that these SSs commonly originate from the combination of the PT (space-inversion and time-reversal) symmetry breaking at the surface and the band folding due to the AF order. The present results pave a pathway toward understanding the relationship between the symmetry and the surface electronic states in antiferromagnets., Comment: 23 pages, 7 figures

Tantalum ditelluride TaTe$_2$ belongs to the family of layered transition metal dichalcogenides but exhibits a unique structural phase transition at around 170 K that accompanies the rearrangement of the Ta atomic network from a "ribbon chain" to a "butterfly-like" pattern. While multiple mechanisms including Fermi surface nesting and chemical bonding instabilities have been intensively discussed, the origin of this transition remains elusive. Here we investigate the electronic structure of single-crystalline TaTe$_2$ with a particular focus on its modifications through the phase transition, by employing core-level and angle-resolved photoemission spectroscopy combined with first-principles calculations. Temperature-dependent core-level spectroscopy demonstrates a splitting of the Ta $4f$ core-level spectra through the phase transition indicative of the Ta-dominated electronic state reconstruction. Low-energy electronic state measurements further reveal an unusual kink-like band reconstruction occurring at the Brillouin zone boundary, which cannot be explained by Fermi surface nesting or band folding effects. On the basis of the orbital-projected band calculations, this band reconstruction is mainly attributed to the modifications of specific Ta $5d$ states, namely the $d_{XY}$ orbitals (the ones elongating along the ribbon chains) at the center Ta sites of the ribbon chains. The present results highlight the strong orbital-dependent electronic state reconstruction through the phase transition in this system and provide fundamental insights towards understanding complex electron-lattice-bond coupled phenomena., Comment: The final version is available in Phys. Rev. Res. (Open Acess)

The Kondo effect between localized $f$-electrons and conductive carriers leads to exotic physical phenomena. Among them, heavy-fermion (HF) systems, in which massive effective carriers appear due to the Kondo effect, have fascinated many researchers. Dimensionality is also an important characteristic of the HF system, especially because it is strongly related to quantum criticality [S. Sachdev, Science 288, 475 (2000)]. However, perfect two-dimensional (2D) HF materials have not been reported yet. Here, we report the surface electronic structure of the monoatomic-layer Kondo lattice YbCu$_2$ on a Cu(111) surface observed by synchrotron-based angle-resolved photoelectron spectroscopy. The 2D conducting band and the Yb 4$f$ state, located very close to the Fermi level, are observed. These bands are hybridized at low-temperature, forming the 2D HF state, with an evaluated coherent temperature of about 30 K. The effective mass of the 2D state is enhanced by a factor of 100 by the development of the HF state. Furthermore, clear evidence of the hybridization gap formation in the temperature dependence of the Kondo-resonance peak has been observed below the coherent temperature. Our study provides a new candidate as an ideal 2D HF material for understanding the Kondo effect at low dimensions., Comment: 24 pages, 10 figures

Recently discovered kagome superconductors AV3Sb5 (A = K, Rb, Cs) exhibit exotic bulk and surface physical properties such as charge-density wave (CDW) and chirality, whereas their origins remain unresolved. By using micro-focused angle-resolved photoemission spectroscopy, we discovered that AV3Sb5 commonly exhibits two distinct polar surfaces depending on the termination; electron- and hole-doped ones for the A- and Sb-termination, respectively. We observed that the kagome-derived band shows a clear splitting in the A-terminated surface while it is absent in the Sb-terminated counterpart, indicative of the polarity-dependent CDW at the surface. Close comparison of the band-dependent splitting reveals that the three-dimensional CDW structure of the K-terminated surface is different from that of the Rb- or Cs-terminated surface, suggesting the diversity of the CDW ground state. These results provide important insight into the origin of CDW in kagome superconductors AV3Sb5., Comment: 10 pages, 8 figures

We performed angle-resolved photoemission spectroscopy with micro-focused beam on a topological line-nodal compound CaSb2 which undergoes a superconducting transition at the onset Tc~1.8 K, to clarify the Fermi-surface topology relevant to the occurrence of superconductivity. We found that a three-dimensional hole pocket at the G point is commonly seen for two types of single-crystalline samples fabricated by different growth conditions. On the other hand, the carrier-doping level estimated from the position of the chemical potential was found to be sensitive to the sample fabrication condition. The cylindrical electron pocket at the Y(C) point predicted by the calculations is absent in one of the two samples, despite the fact that both samples commonly show superconductivity with similar Ts's. This suggests a key role of the three-dimensional hole pocket to the occurrence of superconductivity, and further points to an intriguing possibility to control the topological nature of superconductivity by carrier tuning in CaSb2., Comment: 7 pages, 3 figures

In intercalated transition metal dichalcogenides (I-TMDC), transition metal intercalation introduces magnetic phases which in some cases induce topological band crossing. However, evidence of the topological properties remains elusive in such materials. Here we employ angle-resolved photoemission spectroscopy to reveal the band structure of epitaxially grown ferromagnetic Cr1/3NbSe2. Experimental evidence of the Weyl crossing shows Cr1/3NbSe2 to be a topological ferromagnet. This work highlights I-TMDC as platform towards the interplay of magnetic and topological physics in low-dimensional systems., Comment: 18 pages (including references), 4 figures (placed at the end)

Polar surface and interface play a pivotal role for realizing exotic properties of materials, and a search for such polar states is of crucial importance for expanding materials' functionality. Here we report micro-focused angle-resolved photoemission spectroscopy of CsV3Sb5, a member of recently discovered kagome superconductors AV3Sb5 (A = K, Rb, Cs), and show evidence for the polar nature of cleaved surface which is characterized by Cs- and Sb-terminated surfaces with markedly different fermiology. The Cs-terminated surface shows intriguing doubling of V-derived bands at low temperature associated with the band folding due to the three-dimensional charge-density wave (CDW), whereas the Sb-terminated one shows no band doubling or resultant CDW-gap opening indicative of the suppression of bulk-originated CDW due to polar charge. Such polar-surface-dependent band structure must be incorporated for understanding the origin of unconventional superconducting and charge order at the surface of AV3Sb5., Comment: 10 pages, 13 figures

In solids, strong repulsion between electrons can inhibit their movement and result in a "Mott" metal-to-insulator transition (MIT), a fundamental phenomenon whose understanding has remained a challenge for over 50 years. A key issue is how the wave-like itinerant electrons change into a localized-like state due to increased interactions. However, observing the MIT in terms of the energy- and momentum-resolved electronic structure of the system, the only direct way to probe both itinerant and localized states, has been elusive. Here we show, using angle-resolved photoemission spectroscopy (ARPES), that in V$_2$O$_3$ the temperature-induced MIT is characterized by the progressive disappearance of its itinerant conduction band, without any change in its energy-momentum dispersion, and the simultaneous shift to larger binding energies of a quasi-localized state initially located near the Fermi level., Comment: Main Text (4 figures) and Supplementary Information (12 figures)

The electronic structure changes of SmS surfaces under potassium (K) doping are elucidated using synchrotron-based core-level photoelectron spectroscopy and angle-resolved photoelectron spectroscopy (ARPES). The Sm core-level and ARPES spectra indicate that the Sm mean valence of the surface increased from the nearly divalent to trivalent states, with increasing K deposition. Carrier-induced valence transition (CIVT) from Sm$^{2+}$ to Sm$^{3+}$ exhibits a behavior opposite to that under conventional electron doping. Excess electrons are trapped by isolated excitons, which is inconsistent with the phase transition from the black insulator with Sm$^{2+}$ to the gold metal with Sm$^{3+}$ under pressure. This CIVT helps to clarify the pressure-induced black-to-golden phase transition in this material, which originates from the Mott transition of excitons., Comment: 7 pages, 6 figures

Ti2O3 exhibits a unique metal-insulator transition (MIT) at approximately 450 K over a wide temperature range of ~ 150 K. This broad MIT accompanied by lattice deformation differs from the sharp MITs observed in most other transition-metal oxides. A long-standing issue is determining the role of electron-electron correlation in the electronic structure and MIT of Ti2O3. However, the lack of information about the band structure of Ti2O3 has hindered investigating the origin of its unusual physical properties. Here, we report the electronic band structure of insulating Ti2O3 films with slight hole doping by angle-resolved photoemission spectroscopy (ARPES). ARPES showed clear band dispersion on the surface of single-crystalline epitaxial films. The experimentally obtained band structures were compared with band-structure calculation results based on density functional theory (DFT) with generalized gradient approximation + U correction. The obtained band structures are in good agreement with the DFT calculations at U = 2.2 eV, suggesting that electron-electron correlation plays an important role in the electronic structure of Ti2O3. Furthermore, the detailed analyses with varying U suggest that the origin of the characteristic MIT in Ti2O3 is a semimetal-semimetal or semimetal-semiconductor transition caused by changes in the Fermi surface due to lattice deformation., Comment: Main manuscript: 30 pages, 4 figures, Supplemental Material: 23 pages, 15 figures

Kagome metals AV3Sb5 (A = K, Rb, and Cs) exhibit a characteristic superconducting ground state coexisting with charge-density wave (CDW), whereas the mechanisms of the superconductivity and CDW have yet to be clarified. Here we report a systematic ARPES study of Cs(V1-xNbx)3Sb5 as a function of Nb content x, where isovalent Nb substitution causes an enhancement of superconducting transition temperature (Tc) and the reduction of CDW temperature (TCDW). We found that the Nb substitution shifts the Sb-derived electron band at the Gamma 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 CDW-gap magnitude and TCDW. This indicates a primary role of the SP density of states to stabilize 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., Comment: 6 pages, 3 figures

Angle-resolved photoemission spectroscopy using a micro-focused beam spot (micro-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 synchrotron radiation beam focused with a Kirkpatrick-Baez mirror optics. The mirrors are monolithically installed on a stage, which is driven with five-axes motion, and are vibrationally separated from the ARPES measurement system. Spatial mapping of the Auphotolithography pattern on Si signifies the beam spot size of 10 $\mu$m (horizontal) x 12 $\mu$m (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., Comment: 21 pages, 8 figures

Fe-doped III-V ferromagnetic semiconductors (FMSs) such as (In,Fe)As, (Ga,Fe)Sb, (In,Fe)Sb, and (Al,Fe)Sb are promising materials for spintronic device applications because of the availability of both n- and p-type materials and the high Curie temperatures. On the other hand, (Ga,Fe)As, which has the same zinc-blende crystal structure as the Fe-doped III-V FMSs, shows paramagnetism. The origin of the different magnetic properties in the Fe-doped III-V semiconductors remains to be elucidated. To address this issue, we use resonant photoemission spectroscopy (RPES) and x-ray magnetic circular dichroism (XMCD) to investigate the electronic and magnetic properties of the Fe ions in a paramagnetic (Ga$_{0.95}$,Fe$_{0.05}$)As thin film. The observed Fe 2$p$-3$d$ RPES spectra show that the Fe 3$d$ states are similar to those of ferromagnetic (Ga,Fe)Sb. The estimated Fermi level is located in the middle of the band gap in (Ga,Fe)As. The Fe $L_{2,3}$ XMCD spectra of (Ga$_{0.95}$,Fe$_{0.05}$)As show pre-edge structures, which are not observed in the Fe-doped FMSs, indicating that the minority-spin ($\downarrow$) $e_\downarrow$ states are vacant in (Ga$_{0.95}$,Fe$_{0.05}$)As. The XMCD results suggest that the carrier-induced ferromagnetic interaction in (Ga$_{0.95}$,Fe$_{0.05}$)As is short-ranged and weaker than that in the Fe-doped FMSs. The experimental findings suggest that the electron occupancy of the $e_\downarrow$ states contributes to the appearance of ferromagnetism in the Fe-doped III-V semiconductors, for p-type as well as n-type compounds.

This study investigated the electronic structure of SrTi$_{1-x}$V$_x$O$_3$ (STVO) thin films, which are solid solutions of strongly correlated transparent conductive oxide (TCO) SrVO$_3$ and oxide semiconductor SrTiO$_3$, using ${in situ}$ photoemission spectroscopy. STVO is one of the most promising candidates for correlated-metal TCO because it has the capability of optimizing the performance of transparent electrodes by varying ${x}$. Systematic and significant spectral changes were found near the Fermi level (${E_{\rm F}}$) as a function of ${x}$, while the overall electronic structure of STVO is in good agreement with the prediction of band structure calculations. As ${x}$ decreases from 1.0, spectral weight transfer occurs from the coherent band near ${E_{\rm F}}$ to the incoherent states (lower Hubbard band) around 1.0-1.5 eV. Simultaneously, a pseudogap is formed at ${E_{\rm F}}$, indicating a significant reduction in quasiparticle spectral weight within close vicinity of ${E_{\rm F}}$. This pseudogap seems to evolve into an energy gap at ${x}$ = 0.4, suggesting the occurrence of a composition-driven metal-insulator transition. From angle-resolved photoemission spectroscopic results, the carrier concentration ${n}$ changes proportionally as a function of ${x}$ in the metallic range of ${x}$ = 0.6-1.0. In contrast, the mass enhancement factor, which is proportional to the effective mass (${m^*}$), does not change significantly with varying ${x}$. These results suggest that the key factor of ${n/m^*}$ in optimizing the performance of correlated-metal TCO is tuned by ${x}$, highlighting the potential of STVO to achieve the desired TCO performance in the metallic region., Comment: 32 pages, 5 main figures, and 7 supplementary figures

The inside of the electrical double layer at perovskite oxide heterointerfaces is examined. Here, we report the local polarization and valence distribution in LaNiO$_3$/LaMnO$_3$ and LaMnO$_3$/LaNiO$_3$ bilayers on a SrTiO$_3$ (001) substrate. Simultaneous measurements of two aspects of the structure are realized by using Bayesian inference based on resonant- and nonresonant-surface X-ray diffraction data. The results show that the average Mn valences are Mn$^{3.12+}$ and Mn$^{3.19+}$ for the two samples. The intensity of their local electric field is $\sim$1~GV/m and the direction of the field points from LaMnO$_3$ to LaNiO$_3$., Comment: 19pages, 4 figures

The relationship between the magnetic interaction and photoinduced dynamics in antiferromagnetic perovskites is investigated in this study. In La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$ thin films, commensurate spin ordering is accompanied by charge disproportionation, whereas SrFeO${}_{3}$ thin films show incommensurate helical antiferromagnetic spin ordering due to increased ferromagnetic coupling compared to La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$. To understand the photoinduced spin dynamics in these materials, we investigate the spin ordering through time-resolved resonant soft X-ray scattering. In La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$, ultrafast quenching of the magnetic ordering within 130 fs through a nonthermal process is observed, triggered by charge transfer between the Fe atoms. We compare this to the photoinduced dynamics of the helical magnetic ordering of SrFeO${}_{3}$. We find that the change in the magnetic coupling through optically induced charge transfer can offer an even more efficient channel for spin-order manipulation., Comment: 7 pages, 5 figures

Inter-valence charge transfer (IVCT) is electron transfer between two metal $M$ sites differing in oxidation states through a bridging ligand: $M^{n+1} + M'^{m} \rightarrow M^{n} + M'^{m+1}$. It is considered that IVCT is related to the hopping probability of electron (or the electron mobility) in solids. Since controlling the conductivity of ferromagnetic semiconductors (FMSs) is a key subject for the development of spintronic device applications, the manipulation of the conductivity through IVCT may become a new approach of band engineering in FMSs. In Ru-doped cobalt ferrite CoFe$_2$O$_4$ (CFO) that shows ferrimagnetism and semiconducting transport properties, the reduction of the electric resistivity is attributed to both the carrier doping caused by the Ru substitution for Co and the increase of the carrier mobility due to hybridization between the wide Ru $4d$ and the Fe $3d$ orbitals. The latter is the so-called IVCT mechanism that is charge transfer between the mixed valence Fe$^{2+}$/Fe$^{3+}$ states facilitated by bridging Ru $4d$ orbital: Fe$^{2+}$ + Ru$^{4+}$ $\leftrightarrow$ Fe$^{3+}$ + Ru$^{3+}$. To elucidate the emergence of the IVCT state, we have conducted x-ray absorption spectroscopy (XAS) and resonant photoemission spectroscopy (RPES) measurements on non-doped CFO and Co$_{0.5}$Ru$_{0.5}$Fe$_2$O$_4$ (CRFO) thin films. The observations of the XAS and RPES spectra indicate that the presence of the mixed valence Fe$^{2+}$/Fe$^{3+}$ state and the hybridization between the Fe $3d$ and Ru $4d$ states in the valence band. These results provide experimental evidence for the IVCT state in CRFO, demonstrating a novel mechanism that controls the electron mobility through hybridization between the $3d$ transition-metal cations with intervening $4d$ states., Comment: 16 pages, 5 figures, 1 table

SrMoO$_3$ is a promising material for its excellent electrical conductivity, but growing high-quality thin films remains a challenge. Here we synthesized epitaxial films of SrMoO$_3$ using the molecular beam epitaxy (MBE) technique under a low oxygen-flow rate. Introduction of SrTiO$_3$ buffer layers of 4--8 unit cells between the film and the (001)-oriented SrTiO$_3$ or KTaO$_3$ substrate was crucial to remove impurities and/or roughness of the film surface. The obtained film shows improved electrical conductivities as compared with films obtained by other techniques. The high quality of the SrMoO$_3$ film is also verified by angle-resolved photoemission spectroscopy (ARPES) measurements showing clear Fermi surfaces., Comment: 6 pages, 5 figures

We have performed high-resolution angle-resolved photoemission spectroscopy of ternary pnictide CaAuAs which is predicted to be a three-dimensional topological Dirac semimetal (TDS). By accurately determining the bulk-band structure, we have revealed the coexistence of three-dimensional and quasi-two-dimensional Fermi surfaces with dominant hole carriers. The band structure around the Brillouin-zone center is characterized by an energy overlap between hole and electron pockets, in excellent agreement with first-principles band-structure calculations. This indicates the occurrence of bulk-band inversion, supporting the TDS state in CaAuAs. Because of the high tunability in the chemical composition besides the TDS nature, CaAuAs provides a precious opportunity for investigating the quantum phase transition from TDS to other exotic topological phases., Comment: 6 pages, 4 figures

Perovskite-type manganites, which are well-known for their intriguing physical properties such as colossal magnetoresistance (CMR) and half metalicity, have been considered as candidate materials for spintronics. However, their ferromagnetic (FM) properties are often suppressed in thin films when the thickness is reduced down to several monolayers (MLs). In order to investigate how the magnetic phases evolve near the paramagnetic (PM)-to-FM phase transition boundary, we have performed temperature-dependent x-ray magnetic circular dichroism (XMCD) experiments on a La$_{1-x}$Sr$_{x}$MnO$_3$ (LSMO, $x=0.4$) thin film, whose thickness (8 ML) is close to the boundary between the FM-metallic and the PM-insulating phases. By utilizing the element-selectiveness of XMCD, we have quantitatively estimated the fractions of the PM and superparamagnetic (SPM) phases as well as the FM one as a function of temperature. The results can be reasonably described based on a microscopic phase-separation model., Comment: 6 pages, 3 figures

SmO thin film is a new Kondo system showing a resistivity upturn around 10 K and was theoretically proposed to have a topologically nontrivial band structure. We have performed hard x-ray and soft x-ray photoemission spectroscopy to elucidate the electronic structure of SmO. From the Sm 3$d$ core-level spectra, we have estimated the valence of Sm to be $\sim$2.96, proving that the Sm has a mixed valence. The valence-band photoemission spectra exhibit a clear Fermi edge originating from the Sm 5$d$-derived band. The present finding is consistent with the theory suggesting a possible topological state in SmO and show that rare-earth monoxides or their heterostructures can be a new playground for the interplay of strong electron correlation and spin-orbit coupling.

We have performed angle-resolved photoemission spectroscopy (ARPES) on CeBi which undergoes a two-step antiferromagnetic (AF) transition with temperature. Soft-x-ray ARPES has revealed the inverted band structure at the X point of bulk Brillouin zone for CeBi (and also for LaBi) as opposed to LaSb with non-inverted band structure. Low-energy ARPES on CeBi has revealed the Dirac-cone band at the Gamma point in the paramagnetic phase associated with the bulk band inversion. On the other hand, a double Dirac-cone band appears on entering the first AF phase at T = 25 K, whereas a single Dirac-cone band recovers below the second AF transition at T = 14 K. The present result suggests an intricate interplay between antiferromagnetism and topological surface states in CeBi., Comment: 8 pages, 6 figures

We have performed angle-resolved photoemission spectroscopy (ARPES) on layered ternary compounds ZrGeXc (Xc = S, Se, and Te) with square Ge lattices. ARPES measurements with bulk-sensitive soft-x-ray photons revealed a quasi-two-dimensional bulk-band structure with the bulk nodal loops protected by glide mirror symmetry of the crystal lattice. Moreover, high-resolution ARPES measurements near the Fermi level with vacuum-ultraviolet photons combined with first-principles band-structure calculations elucidated a Dirac-node-arc surface state traversing a tiny spin-orbit gap associated with the nodal loops. We found that this surface state commonly exists in ZrGeXc despite the difference in the shape of nodal loops. The present results suggest that the spin-orbit coupling and the multiple nodal loops cooperatively play a key role in creating the exotic Dirac-node-arc surface states in this class of topological line-node semimetals., Comment: 11 pages, 9 figures

Heterostructures having both magnetism and topology are promising materials for the realization of exotic topological quantum states while challenging in synthesis and engineering. Here, we report natural magnetic van der Waals heterostructures of (MnBi2Te4)m(Bi2Te3)n that exhibit controllable magnetic properties while maintaining their topological surface states. The interlayer antiferromagnetic exchange coupling is gradually weakened as the separation of magnetic layers increases, and an anomalous Hall effect that is well coupled with magnetization and shows ferromagnetic hysteresis was observed below 5 K. The obtained homogeneous heterostructure with atomically sharp interface and intrinsic magnetic properties will be an ideal platform for studying the quantum anomalous Hall effect, axion insulator states, and the topological magnetoelectric effect., Comment: 40 pages, 15 figures

To investigate the relationship between the charge redistribution and ferromagnetism at the heterointerface between perovskite transition-metal oxides LaNiO$_3$ (LNO) and LaMnO$_3$ (LMO), we performed x-ray absorption spectroscopy and x-ray magnetic circular dichroism (XMCD) measurements. In the LNO/LMO heterostructures with asymmetric charge redistribution, the electrons donated from Mn to Ni ions are confined within one monolayer (ML) of LNO at the interface, whereas holes are distributed over 3-4 ML on the LMO side. A detailed analysis of the Ni-$L_{2,3}$ and Mn-$L_{2,3}$ XMCD spectra reveals that Ni magnetization is induced only by the Ni$^{2+}$ ions in the 1 ML LNO adjacent to the interface, while the magnetization of Mn ions is increased in the 3-4 ML LMO of the interfacial region. The characteristic length scale of the emergent (increased) interfacial ferromagnetism of the LNO (LMO) layers is in good agreement with that of the charge distribution across the interface, indicating a close relationship between the charge redistribution due to the interfacial charge transfer and the ferromagnetism of the LNO/LMO interface. Furthermore, the XMCD spectra clearly demonstrate that the vectors of induced magnetization of both ions are aligned ferromagnetically, suggesting that the delicate balance between the exchange interactions occurring inside each layer and across the interface may induce the canted ferromagnetism of Ni$^{2+}$ ions, resulting in weak magnetization in the 1 ML LNO adjacent to the interface., Comment: 22 pages, 4 figures

Ce(O,F)Sb(S,Se)2 single crystals were successfully grown using a CsCl/KCl flux method. The obtained crystals have a plate-like shape with the typical size of 1-2 mm and well-developed ab-plane, which enables X-ray single crystal structural analysis. The Ce(O,F)Sb(S,Se)2 crystallizes in a monoclinic space group, P21/m, with lattice parameters of a = 4.121(7) A, b = 4.109(7) A, c = 13.233(15) A, beta = 97.94(7) deg. It is composed of alternate stacking of Ce-(O,F) and Sb-SSe layers, and the Sb-SSe layer includes selective occupation of Se atoms in its in-plane site. The valence state of Ce is estimated to be Ce3+ by X-ray absorption fine spectroscopy analysis. The single crystals show an insulating behavior, and a magnetic ordering around 6 K., Comment: 27 pages, 7 figures, 3 Tables

In order to study the origin of metallization of VO$_2$ induced by electron injection, we deposit K atoms onto the surface of VO$_2$ films grown on TiO$_2$ (001) substrates, and we investigate the change in the electronic and crystal structures using ${in~situ}$ photoemission spectroscopy and x-ray absorption spectroscopy (XAS). The deposition of K atoms onto a surface of insulating monoclinic VO$_2$ leads to a phase transition from insulator to metal. In this metallization state, the V-V dimerization characteristic to the monoclinic phase of VO$_2$ still exists, as revealed by the polarization dependence of the XAS spectra. Furthermore, the monoclinic metal undergoes a transition to a monoclinic insulator with decrease in temperature, and to a rutile metal with increase in temperature. These results indicate the existence of a metallic monoclinic phase around the boundary between the insulating monoclinic and metallic rutile phases in the case of electron-doped VO$_2$., Comment: 20 pages, 5 figures

Magnetic anisotropy of epitaxially grown thin films is affected by the strain from the substrates due to a combined effect of distorted electronic structure and spin-orbit interaction (SOI). As an inverse process, one expects an anisotropy of the electronic structure induced by magnetization in the presence of SOI. We have studied the charge-density anisotropy induced by magnetization in thin films of the ferromagnetic metal La$_{1-x}$Sr$_{x}$MnO$_3$ via x-ray magnetic linear dichroism (XMLD). XMLD measurements on thin films with various thicknesses have shown that the XMLD intensity is proportional to the square of the ferromagnetic moment. Using the XMLD sum rule and cluster-model calculation, it has been shown that more Mn 3$d$ electrons are distributed in orbitals elongated along the direction parallel to the spin polarization than in orbitals elongated in the direction perpendicular to it. The cluster-model calculation has shown that the effect of tensile strain from the SrTiO$_3$ substrate on the XMLD spectra is also consistent with the observed XMLD spectral line shapes., Comment: 12 pages, 4 figures

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, spin-1 chiral fermion and 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., Comment: 6 pages, 4 figures (paper proper) + 4 pages, 4 figures (supplemental material)

We have performed angle-resolved photoemission spectroscopy of AlB2 which is isostructural to high-temperature superconductor MgB2. Using soft-x-ray photons, we accurately determined the three-dimensional bulk band structure and found a highly anisotropic Dirac-cone band at the K point in the bulk hexagonal Brillouin zone. This band disperses downward on approaching the H point while keeping its degeneracy at the Dirac point, producing a characteristic Dirac nodal line along the KH line. We also found that the band structure of AlB2 is regarded as a heavily electron-doped version of MgB2 and is therefore well suited for fully visualizing the predicted Dirac nodal line. The present results suggest that (Al,Mg)B2 system is a promising platform for studying the interplay among Dirac nodal line, carrier doping, and possible topological superconducting properties., Comment: 6 pages, 3 figures

In CsW2O6, which undergoes a metal-insulator transition (MIT) at 213 K, the emergence of exotic properties associated with rattling motion of Cs is expected owing to its characteristic \beta-pyrochlore-type structure. However, a hurdle for crystal growth hampers elucidation of detailed properties and mechanisms of the MIT. Here we report on the epitaxial growth of \beta-pyrochlore-type CsW2O6 films and their electronic properties across the MIT. Using pulsed-laser deposi-tion technique, we grew single-crystalline CsW2O6 films exhibiting remarkably lower resistivity compared with a poly-crystalline bulk and sharp MIT around 200 K. Negative magnetoresistance and positive Hall coefficient were found, which became pronounced below 200 K. The valence-band and core-levels photoemission spectra indicated the drastic changes across the MIT. In the valence band photoemission spectrum, the finite density of states was observed at the Fermi level in the metallic phase. In contrast, an energy gap appeared in the insulating phase. The split of W 4f core-level spectrum suggested the charge disproportionation of W5+ and W6+ in the insulating phase. The change of spectral shape in the Cs 4d core levels reflected the rattling motion of Cs+ cations. These results strongly suggest that CsW2O6 is a novel material, in which MIT is driven by the charge disproportionation associated with the rattling motion., Comment: 8 pages, 6 figures

Engineering atomic-scale structures allows great manipulation of physical properties and chemical processes for advanced technology. We show that the B atoms deployed at the centers of honeycombs in boron sheets, borophene, behave as nearly perfect electron donors for filling the graphitic $\sigma$ bonding states without forming additional in-plane bonds by first-principles calculations. The dilute electron density distribution owing to the weak bonding surrounding the center atoms provides easier atomic-scale engineering and is highly tunable via in-plane strain, promising for practical applications, such as modulating the extraordinarily high thermal conductance that exceeds the reported value in graphene. The hidden honeycomb bonding structure suggests an unusual energy sequence of core electrons that has been verified by our high-resolution core-level photoelectron spectroscopy measurements. With the experimental and theoretical evidence, we demonstrate that borophene exhibits a peculiar bonding structure and is distinctive among two-dimensional materials., Comment: 5 pages, 3 figures, 1 table

We report the epitaxial growth of Ca3SnO antiperovskite oxide films on (001)-oriented cubic yttria-stabilized zirconia (YSZ) substrates by using a conventional pulsed laser deposition (PLD) technique. In this work, a sintered Ca3SnO pellet is used as the ablation target. X-ray diffraction measurements demonstrate the (001) growth of Ca3SnO films with the antiperovskite structure and a cube-on-cube orientation relationship to the YSZ substrate. The successful synthesis of the antiperovskite phase is further confirmed by x-ray photoemission spectroscopy. These results strongly suggest that antiperovskite-oxide films can be directly grown on substrates from the target material using a PLD technique.

Controlling quantum critical phenomena in strongly correlated electron systems, which emerge in the neighborhood of a quantum phase transition, is a major challenge in modern condensed matter physics. Quantum critical phenomena are generated from the delicate balance between long-range order and its quantum fluctuation. So far, the nature of quantum phase transitions has been investigated by changing a limited number of external parameters such as pressure and magnetic field. We propose a new approach for investigating quantum criticality by changing the strength of quantum fluctuation that is controlled by the dimensional crossover in metallic quantum well (QW) structures of strongly correlated oxides. With reducing layer thickness to the critical thickness of metal-insulator transition, crossover from a Fermi liquid to a non-Fermi liquid has clearly been observed in the metallic QW of SrVO$_3$ by \textit{in situ} angle-resolved photoemission spectroscopy. Non-Fermi liquid behavior with the critical exponent ${\alpha} = 1$ is found to emerge in the two-dimensional limit of the metallic QW states, indicating that a quantum critical point exists in the neighborhood of the thickness-dependent Mott transition. These results suggest that artificial QW structures provide a unique platform for investigating novel quantum phenomena in strongly correlated oxides in a controllable fashion., Comment: 6 pages, 3 figures

We investigate the thickness effects on charge and magnetic orderings in Fe perovskite oxide La1/3Sr2/3FeO3/SrTiO3 thin films by hard x-ray and resonant soft x-ray scattering (RSXS) with changing thin film thickness systematically. We found that the correlation lengths of the magnetic ordering along the in-plane and out-of-plane directions are comparable and proportional to the thickness, and shows stronger thickness dependence than those of charge orderg. %the thickness dependence of correlation length of charge ordering is smaller than that of magnetic orderings. The magnetic ordered states disappear when the correlation length of magnetic ordering decreases to that of charge ordering through the intrinsic thickness effects. Surface sensitive grazing-incident RSXS revealed that the orderings exist even in the surface region, which indicates that the observed orderings is not affected by surface effect like oxygen vacancies. Critical thickness is in 5-15 nm, which corresponds to 4-11 antiferromagnetic ordering period. This critical value seems to be common to other ferromagnetic oxide thin films.

Honeycomb structures of group IV elements can host massless Dirac fermions with non-trivial Berry phases. Their potential for electronic applications has attracted great interest and spurred a broad search for new Dirac materials especially in monolayer structures. We present a detailed investigation of the \beta 12 boron sheet, which is a borophene structure that can form spontaneously on a Ag(111) surface. Our tight-binding analysis revealed that the lattice of the \beta 12-sheet could be decomposed into two triangular sublattices in a way similar to that for a honeycomb lattice, thereby hosting Dirac cones. Furthermore, each Dirac cone could be split by introducing periodic perturbations representing overlayer-substrate interactions. These unusual electronic structures were confirmed by angle-resolved photoemission spectroscopy and validated by first-principles calculations. Our results suggest monolayer boron as a new platform for realizing novel high-speed low-dissipation devices., Comment: accepted for publication in Physical Review Letters

Two-dimensional (2D) electrides are a new concept material in which anionic electrons are confined in the interlayer space between positively charged layers. We have performed angle-resolved photoemission spectroscopy measurements on Y$_2$C, which is a possible 2D electride, in order to verify the formation of 2D electride states in Y$_2$C. We clearly observe the existence of semimetallic "electride bands" near the Fermi level, as predicted by ${ab}$ ${initio}$ calculations, conclusively demonstrating that Y$_2$C is a quasi-2D electride with electride bands derived from interlayer anionic electrons., Comment: 5 pages, 4 figures

A synergistic effect between strong electron correlation and spin-orbit interaction (SOI) has been theoretically predicted to result in a new topological state of quantum matter on Kondo insulators (KIs), so-called topological Kondo insulators (TKIs). One TKI candidate has been experimentally observed on the KI SmB6(001), and the origin of the surface states (SS) and the topological order of SmB6 has been actively discussed. Here, we show a metallic SS on the clean surface of another TKI candidate YbB12(001), using angle-resolved photoelectron spectroscopy. The SS showed temperature-dependent reconstruction corresponding with the Kondo effect observed for bulk states. Despite the low-temperature insulating bulk, the reconstructed SS with c-f hybridization was metallic, forming a closed Fermi contour surrounding $\bar{\Gamma}$ on the surface Brillouin zone and agreeing with the theoretically expected behavior for SS on TKIs. These results demonstrate the temperature-dependent holistic reconstruction of two-dimensional states localized on KIs surface driven by the Kondo effect., Comment: 15 pages, 4 figures