The van der Waals (vdW) materials with low dimensions have been extensively studied as a platform to generate exotic quantum properties [1][2][3][4][5][6]. Advancing this view, a great deal of attention is currently paid to topological quantum materials with vdW structures, which give new concepts in designing the functionality of materials. Here, we present the first experimental realization of a higher-order topological insulator by investigating a quasi-one-dimensional (quasi-1D) bismuth bromide Bi 4 Br 4 [7][8][9][10][11] built from a vdW stacking of quantum spin Hall insulators (QSHI) [12] with angle-resolved photoemission spectroscopy (ARPES). The quasi-1D bismuth halides can select various topological phases by different stacking procedures of vdW chains, offering a fascinating playground for engineering topologically non-trivial edge-states toward future spintronics applications.The Z 2 weak topological insulator (WTI) phases have been confirmed in the materials with stacked QSHI layers, where the side-surface becomes topologically non-trivial by accumulating helical edge states of QSHI layers [13,14]. Similarly, higher-order topological insulators (HOTIs) are expected to be built from stacking QSHIs, which, however, accumulate the 1D edge-states to develop 1D helical hinge-states in a 3D crystal [15,16]. Such HOTI phases have been theoretically predicted recently in materials previously regarded as trivial insulators under the Z 2 criterion by extending the topological classification to the Z 4 topological index [17][18][19][20][21][22]. To date, only one material has been experimentally confirmed to be in the higher-order topological phase, which is bulk bismuth [23]. However, bulk bismuth is a semimetal, which cannot become insulating even by carrier doping. Materials science is, therefore, awaiting the first experimental realization of a HOTI, which enables one to explore various quantum phenomena including spin currents around hinges and quantized conductance under the external fields.A quasi-1D bismuth bromide, Bi 4 Br 4 , with a bilayer structure of chains (Fig. 1b) is theoretically predicted to be a topological crystalline insulator of Z 2,2,2,4 = {0, 0, 0, 2}, protected by the C 2 -rotation symmetry [10,11,[19][20][21]. This state should develop 2D topological surface states in the cross-section (010) of the chains [24,25]. Significantly, theory also categorizes this system as a HOTI, and expects that 1D helical hinge-states emerge between the top-surface (001) and the side-surface (100) of a crystal due to the second-order bulk-boundary correspondence [10,11]. Nevertheless, the topological phase of Bi 4 Br 4 has

Experimental determinations of bulk band topology in the solid states have been so far restricted to only indirect investigation through the probing of surface states predicted by electronic structure calculations. We here present an alternative approach to determine the band topology by means of bulk-sensitive soft x-ray angle-resolved photoemission spectroscopy. We investigate the bulk electronic structures of the series materials, Ce monopnictides (CeP, CeAs, CeSb, and CeBi). By performing a paradigmatic study of the band structures as a function of their spin-orbit coupling, we draw the topological phase diagram and unambiguously reveal the topological phase transition from a trivial to a nontrivial regime in going from CeP to CeBi induced by the band inversion. The underlying mechanism of the phase transition is elucidated in terms of spin-orbit coupling in concert with their semimetallic band structures. Our comprehensive observations provide a new insight into the band topology hidden in the bulk states.

In cuprate superconductors with high critical transition temperature (Tc), light hole-doping to the parent compound, which is an antiferromagnetic Mott insulator, has been predicted to lead to the formation of small Fermi pockets. These pockets, however, have not been observed. Here, we investigate the electronic structure of the five-layered Ba2Ca4Cu5O10(F,O)2, which has inner copper oxide (CuO2) planes with extremely low disorder, and find small Fermi pockets centered at (π/2, π/2) of the Brillouin zone by angle-resolved photoemission spectroscopy and quantum oscillation measurements. The d-wave superconducting gap opens along the pocket, revealing the coexistence between superconductivity and antiferromagnetic ordering in the same CuO2 sheet. These data further indicate that superconductivity can occur without contribution from the antinodal region around (π, 0), which is shared by other competing excitations.

Using a laser-excited angle-resolved photoemission spectroscopy capable of bulk sensitive and high-energy resolution measurements, we reveal a new phenomenon of superconductors in the optimally doped trilayer Bi_{2}Sr_{2}Ca_{2}Cu_{3}O_{10+δ}. We observe a hybridization of the Bogoliubov bands derived from the inner and outer CuO_{2} planes with different magnitudes of energy gaps. Our data clearly exhibit the splitting of coherent peaks and the consequent enhancement of spectral gaps. These features are reproduced by model calculations, which indicate that the gap enhancement extends over a wide range of Fermi surface up to the antinode. The significant modulation of electron pairing uncovered here might be a crucial factor to achieve the highest critical temperature in the trilayer cuprates.

Solids with competing interactions often undergo complex phase transitions with a variety of long-periodic modulations. Among such transition, devil's staircase is the most complex phenomenon, and for it, CeSb is the most famous material, where a number of the distinct phases with long-periodic magnetostructures sequentially appear below the Néel temperature. An evolution of the low-energy electronic structure going through the devil's staircase is of special interest, which has, however, been elusive so far despite 40 years of intense research. Here, we use bulk-sensitive angle-resolved photoemission spectroscopy and reveal the devil's staircase transition of the electronic structures. The magnetic reconstruction dramatically alters the band dispersions at each transition. Moreover, we find that the well-defined band picture largely collapses around the Fermi energy under the long-periodic modulation of the transitional phase, while it recovers at the transition into the lowesttemperature ground state. Our data provide the first direct evidence for a significant reorganization of the electronic structures and spectral functions occurring during the devil's staircase.

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