Hidden Charge Order and Multiple Electronic Instabilities in EuTe4.

The rare-earth telluride compound EuTe4 exhibits a charge density wave (CDW) and an unconventional thermal hysteresis transition. Herein, we report a comprehensive study of the CDW states in EuTe4 by using low-temperature scanning tunneling microscopy. Two types of charge orders are observed at 4 K, including a newly discovered spindle-shaped pattern and a typical stripe-like pattern. As an exotic charge order, the spindle-shaped CDW is off-axis and barely visible at 77 K, indicating that it is a hidden order developed at low temperature. Based on our first-principles calculations, we reveal the origins of the observed electronic instabilities. The spindle-shaped charge order stems from a subsequent transition based on the stripe-like CDW phase. Our work demonstrates that the competition and cooperation between multiple charge orders can generate exotic quantum phases.

ARPES investigation of the electronic structure and its evolution in magnetic topological insulator MnBi2+2nTe4+3n family.

In the past 5 years, there has been significant research interest in the intrinsic magnetic topological insulator family compounds MnBi2+2nTe4+3n (where n = 0, 1, 2 …). In particular, exfoliated thin films of MnBi2Te4 have led to numerous experimental breakthroughs, such as the quantum anomalous Hall effect, axion insulator phase and high-Chern number quantum Hall effect without Landau levels. However, despite extensive efforts, the energy gap of the topological surface states due to exchange magnetic coupling, which is a key feature of the characteristic band structure of the system, remains experimentally elusive. The electronic structure measured by using angle-resolved photoemission (ARPES) shows significant deviation from ab initio prediction and scanning tunneling spectroscopy measurements, making it challenging to understand the transport results based on the electronic structure. This paper reviews the measurements of the band structure of MnBi2+2nTe4+3n magnetic topological insulators using ARPES, focusing on the evolution of their electronic structures with temperature, surface and bulk doping and film thickness. The aim of the review is to construct a unified picture of the electronic structure of MnBi2+2nTe4+3n compounds and explore possible control of their topological properties.

Observation of Anomalous Planar Hall Effect Induced by One-Dimensional Weak Antilocalization.

The confinement of electrons in one-dimensional (1D) space highlights the prominence of the role of electron interactions or correlations, leading to a variety of fascinating physical phenomena. The quasi-1D electron states can exhibit a unique spin texture under spin-orbit interaction (SOI) and thus could generate a robust spin current by forbidden electron backscattering. Direct detection of such 1D spin or SOI information, however, is challenging due to complicated techniques. Here, we identify an anomalous planar Hall effect (APHE) in the magnetotransport of quasi-1D van der Waals (vdW) topological materials as exemplified by Bi4Br4, which arises from the quantum interference correction of 1D weak antilocalization (WAL) to the ordinary planar Hall effect and demonstrates a deviation from the usual sine and cosine curves. The occurrence of 1D WAL is correlated to the line-shape Fermi surface and persistent spin texture of (100) topological surface states of Bi4Br4, as revealed by both our angle-resolved photoemission spectroscopy and first-principles calculations. By generalizing the observation of APHE to other non-vdW bulk materials, this work provides a possible characteristic of magnetotransport for identifying the spin/SOI information and quantum interference behavior of 1D states in 3D topological material.

Topological electronic structure and spin texture of quasi-one-dimensional higher-order topological insulator Bi4Br4.

The notion of topological insulators (TIs), characterized by an insulating bulk and conducting topological surface states, can be extended to higher-order topological insulators (HOTIs) hosting gapless modes localized at the boundaries of two or more dimensions lower than the insulating bulk. In this work, by performing high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements with submicron spatial and spin resolution, we systematically investigate the electronic structure and spin texture of quasi-one-dimensional (1D) HOTI candidate Bi4Br4. In contrast to the bulk-state-dominant spectra on the (001) surface, we observe gapped surface states on the (100) surface, whose dispersion and spin-polarization agree well with our ab-initio calculations. Moreover, we reveal in-gap states connecting the surface valence and conduction bands, which is a signature of the hinge states inside the (100) surface gap. Our findings provide compelling evidence for the HOTI phase of Bi4Br4. The identification of the higher-order topological phase promises applications based on 1D spin-momentum locked current in electronic and spintronic devices.

Bipolaronic Nature of the Pseudogap in Quasi-One-Dimensional (TaSe4)2I Revealed via Weak Photoexcitation.

The origin of the pseudogap in many strongly correlated materials has been a longstanding puzzle. Here, we present experimental evidence that many-body interactions among small Holstein polarons, i.e., the formation of bipolarons, are primarily responsible for the pseudogap in (TaSe4)2I. After weak photoexcitation of the material, we observe the appearance of both dispersive (single-particle bare band) and flat bands (single-polaron sub-bands) in the gap by using time- and angle-resolved photoemission spectroscopy. Based on Monte Carlo simulations of the Holstein model, we propose that the melting of pseudogap and emergence of new bands originate from a bipolaron to single-polaron crossover. We also observe dramatically different relaxation times for the excited in-gap states in (TaSe4)2I (∼600 fs) compared with another 1D material Rb0.3MoO3 (∼60 fs), which provides a new method for distinguishing between pseudogaps induced by polaronic or Luttinger-liquid many-body interactions.

Towards layer-selective quantum spin hall channels in weak topological insulator Bi4Br2I2.

Weak topological insulators, constructed by stacking quantum spin Hall insulators with weak interlayer coupling, offer promising quantum electronic applications through topologically non-trivial edge channels. However, the currently available weak topological insulators are stacks of the same quantum spin Hall layer with translational symmetry in the out-of-plane direction-leading to the absence of the channel degree of freedom for edge states. Here, we study a candidate weak topological insulator, Bi4Br2I2, which is alternately stacked by three different quantum spin Hall insulators, each with tunable topologically non-trivial edge states. Our angle-resolved photoemission spectroscopy and first-principles calculations show that an energy gap opens at the crossing points of different Dirac cones correlated with different layers due to the interlayer interaction. This is essential to achieve the tunability of topological edge states as controlled by varying the chemical potential. Our work offers a perspective for the construction of tunable quantized conductance devices for future spintronic applications.

Observation of Mott instability at the valence transition of f-electron system.

Mott physics plays a critical role in materials with strong electronic correlations. Mott insulator-to-metal transition can be driven by chemical doping, external pressure, temperature and gate voltage, which is often seen in transition metal oxides with 3d electrons near the Fermi energy (e.g. cuprate superconductor). In 4f-electron systems, however, the insulator-to-metal transition is mostly driven by Kondo hybridization and the Mott physics has rarely been explored in experiments. Here, by combining the angle-resolved photoemission spectroscopy and strongly correlated band structure calculations, we show that an unusual Mott instability exists in YbInCu4 accompanying its mysterious first-order valence transition. This contrasts with the prevalent Kondo picture and demonstrates that YbInCu4 is a unique platform to explore the Mott physics in Kondo lattice systems. Our work provides important insight for the understanding and manipulation of correlated quantum phenomena in the f-electron system.

Topology Hierarchy of Transition Metal Dichalcogenides Built from Quantum Spin Hall Layers.

The evolution of the physical properties of 2D material from monolayer limit to the bulk reveals unique consequences from dimension confinement and provides a distinct tuning knob for applications. Monolayer 1T'-phase transition metal dichalcogenides (1T'-TMDs) with ubiquitous quantum spin Hall (QSH) states are ideal 2D building blocks of various 3D topological phases. However, the stacking geometry has been previously limited to the bulk 1T'-WTe2 type. Here, the novel 2M-TMDs consisting of translationally stacked 1T'-monolayers are introduced as promising material platforms with tunable inverted bandgaps and interlayer coupling. By performing advanced polarization-dependent angle-resolved photoemission spectroscopy as well as first-principles calculations on the electronic structure of 2M-TMDs, a topology hierarchy is revealed: 2M-WSe2 , MoS2, and MoSe2 are weak topological insulators (WTIs), whereas 2M-WS2 is a strong topological insulator (STI). Further demonstration of topological phase transitions by tunning interlayer distance indicates that band inversion amplitude and interlayer coupling jointly determine different topological states in 2M-TMDs. It is proposed that 2M-TMDs are parent compounds of various exotic phases including topological superconductors and promise great application potentials in quantum electronics due to their flexibility in patterning with 2D materials.

Carbon nanotube electron blackbody and its radiation spectra.

An optical blackbody is an ideal absorber for all incident optical radiation, and the theoretical study of its radiation spectra paved the way for quantum mechanics (Planck's law). Herein, we propose the concept of an electron blackbody, which is a perfect electron absorber as well as an electron emitter with standard energy spectra at different temperatures. Vertically aligned carbon nanotube arrays are electron blackbodies with an electron absorption coefficient of 0.95 for incident energy ranging from 1 keV to 20 keV and standard electron emission spectra that fit well with the free electron gas model. Such a concept might also be generalized to blackbodies for extreme ultraviolet, X-ray, and γ-ray photons as well as neutrons, protons, and other elementary particles.

The Giant Spin-to-Charge Conversion of the Layered Rashba Material BiTeI.

Rashba spin-orbit coupling (SOC) could facilitate an efficient interconversion between spin and charge currents. Among various systems, BiTeI holds one of the largest Rashba-type spin splittings. Unlike other Rashba systems (e.g., Bi/Ag and Bi2Se3), an experimental investigation of the spin-to-charge interconversion in BiTeI remains to be explored. Through performing an angle-resolved photoemission spectroscopy (ARPES) measurement, such a large Rashba-type spin splitting with a Rashba parameter αR = 3.68 eV Å is directly identified. By studying the spin pumping effect in the BiTeI/NiFe bilayer, we reveal a very large inverse Rashba-Edelstein length λIREE ≈ 1.92 nm of BiTeI at room temperature. Furthermore, the λIREE monotonously increases to 5.00 nm at 60 K, indicating an enhanced Rashba SOC at low temperature. These results suggest that BiTeI films with the giant Rashba SOC are promising for achieving efficient spin-to-charge interconversion, which could be implemented for building low-power-consumption spin-orbitronic devices.

Observation of Coexisting Dirac Bands and Moiré Flat Bands in Magic-Angle Twisted Trilayer Graphene.

Moiré superlattices that consist of two or more layers of 2D materials stacked together with a small twist angle have emerged as a tunable platform to realize various correlated and topological phases, such as Mott insulators, unconventional superconductivity, and quantum anomalous Hall effect. Recently, magic-angle twisted trilayer graphene (MATTG) has shown both robust superconductivity similar to magic-angle twisted bilayer graphene and other unique properties, including the Pauli-limit violating and re-entrant superconductivity. These rich properties are deeply rooted in its electronic structure under the influence of distinct moiré potential and mirror symmetry. Here, combining nanometer-scale spatially resolved angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy, the as-yet unexplored band structure of MATTG near charge neutrality is systematically measured. These measurements reveal the coexistence of the distinct dispersive Dirac band with the emergent moiré flat band, showing nice agreement with the theoretical calculations. These results serve as a stepstone for further understanding of the unconventional superconductivity in MATTG.

Evolution of the Electronic Structure of Ultrathin MnBi2Te4 Films.

Ultrathin films of intrinsic magnetic topological insulator MnBi2Te4 exhibit fascinating quantum properties such as the quantum anomalous Hall effect and the axion insulator state. In this work, we systematically investigate the evolution of the electronic structure of MnBi2Te4 thin films. With increasing film thickness, the electronic structure changes from an insulator type with a large energy gap to one with in-gap topological surface states, which is, however, still in drastic contrast to the bulk material. By surface doping of alkali-metal atoms, a Rashba split band gradually emerges and hybridizes with topological surface states, which not only reconciles the puzzling difference between the electronic structures of the bulk and thin-film MnBi2Te4 but also provides an interesting platform to establish Rashba ferromagnet that is attractive for (quantum) anomalous Hall effect. Our results provide important insights into the understanding and engineering of the intriguing quantum properties of MnBi2Te4 thin films.

Approaching a Minimal Topological Electronic Structure in Antiferromagnetic Topological Insulator MnBi2Te4 via Surface Modification.

The topological electronic structure plays a central role in the nontrivial physical properties in topological quantum materials. A minimal, "hydrogen-atom-like" topological electronic structure is desired for research. In this work, we demonstrate an effort toward the realization of such a system in the intrinsic magnetic topological insulator MnBi2Te4, by manipulating the topological surface state (TSS) via surface modification. Using high resolution laser- and synchrotron-based angle-resolved photoemission spectroscopy (ARPES), we found the TSS in MnBi2Te4 is heavily hybridized with a trivial Rashba-type surface state (RSS), which could be efficiently removed by the in situ surface potassium (K) dosing. By employing multiple experimental methods to characterize K dosed surface, we attribute such a modification to the electrochemical reactions of K clusters on the surface. Our work not only gives a clear band assignment in MnBi2Te4 but also provides possible new routes in accentuating the topological behavior in the magnetic topological quantum materials.

Light-induced dimension crossover dictated by excitonic correlations.

In low-dimensional systems with strong electronic correlations, the application of an ultrashort laser pulse often yields novel phases that are otherwise inaccessible. The central challenge in understanding such phenomena is to determine how dimensionality and many-body correlations together govern the pathway of a non-adiabatic transition. To this end, we examine a layered compound, 1T-TiSe2, whose three-dimensional charge-density-wave (3D CDW) state also features exciton condensation due to strong electron-hole interactions. We find that photoexcitation suppresses the equilibrium 3D CDW while creating a nonequilibrium 2D CDW. Remarkably, the dimension reduction does not occur unless bound electron-hole pairs are broken. This relation suggests that excitonic correlations maintain the out-of-plane CDW coherence, settling a long-standing debate over their role in the CDW transition. Our findings demonstrate how optical manipulation of electronic interaction enables one to control the dimensionality of a broken-symmetry order, paving the way for realizing other emergent states in strongly correlated systems.

Direct Visualization and Manipulation of Tunable Quantum Well State in Semiconducting Nb2SiTe4.

Quantum well states (QWSs) can form at the surface or interfaces of materials with confinement potential. They have broad applications in electronic and optical devices such as high mobility electron transistor, photodetector, and quantum well laser. The properties of the QWSs are usually the key factors for the performance of the devices. However, direct visualization and manipulation of such states are, in general, challenging. In this work, by using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy/spectroscopy (STM/STS), we directly probe the QWSs generated on the vacuum interface of a narrow band gap semiconductor Nb2SiTe4. Interestingly, the position and splitting of QWSs could be easily manipulated via potassium (K) dosage onto the sample surface. Our results suggest Nb2SiTe4 to be an intriguing semiconductor system to study and engineer the QWSs, which has great potential in device applications.

Coexistence of resistance oscillations and the anomalous metal phase in a lithium intercalated TiSe2 superconductor.

Superconductivity and charge density wave (CDW) appear in the phase diagram of a variety of materials including the high-Tc cuprate family and many transition metal dichalcogenides (TMDs). Their interplay may give rise to exotic quantum phenomena. Here, we show that superconducting arrays can spontaneously form in TiSe2-a TMD with coexisting superconductivity and CDW-after lithium ion intercalation. We induce a superconducting dome in the phase diagram of LixTiSe2 by using the ionic solid-state gating technique. Around optimal doping, we observe magnetoresistance oscillations, indicating the emergence of periodically arranged domains. In the same temperature, magnetic field and carrier density regime where the resistance oscillations occur, we observe signatures for the anomalous metal-a state with a resistance plateau across a wide temperature range below the superconducting transition. Our study not only sheds further insight into the mechanism for the periodic electronic structure, but also reveals the interplay between the anomalous metal and superconducting fluctuations.

A vacuum ultraviolet laser with a submicrometer spot for spatially resolved photoemission spectroscopy.

Vacuum ultraviolet (VUV) lasers have demonstrated great potential as the light source for various spectroscopies, which, if they can be focused into a small beam spot, will not only allow investigation of mesoscopic materials and structures but also find application in the manufacture of nano-objects with excellent precision. In this work, we report the construction of a 177 nm VUV laser that can achieve a record-small (~0.76 µm) focal spot at a long focal length (~45 mm) by using a flat lens without spherical aberration. The size of the beam spot of this VUV laser was tested using a metal grating and exfoliated graphene flakes, and we demonstrated its application in a fluorescence spectroscopy study on pure and Tm3+-doped NaYF4 microcrystals, revealing a new emission band that cannot be observed in the traditional up-conversion process. In addition, this laser system would be an ideal light source for spatially and angle-resolved photoemission spectroscopy.

Mode-resolved reciprocal space mapping of electron-phonon interaction in the Weyl semimetal candidate Td-WTe2.

The excitation of coherent phonons provides unique capabilities to control fundamental properties of quantum materials on ultrafast time scales. Recently, it was predicted that a topologically protected Weyl semimetal phase in the transition metal dichalcogenide Td-WTe2 can be controlled and, ultimately, be destroyed upon the coherent excitation of an interlayer shear mode. By monitoring electronic structure changes with femtosecond resolution, we provide here direct experimental evidence that the shear mode acts on the electronic states near the phase-defining Weyl points. Furthermore, we observe a periodic reduction in the spin splitting of bands, a distinct electronic signature of the Weyl phase-stabilizing non-centrosymmetric Td ground state of WTe2. The comparison with higher-frequency coherent phonon modes finally proves the shear mode-selectivity of the observed changes in the electronic structure. Our real-time observations reveal direct experimental insights into electronic processes that are of vital importance for a coherent phonon-induced topological phase transition in Td-WTe2.

A combined laser-based angle-resolved photoemission spectroscopy and two-photon photoemission spectroscopy study of Td-WTe2.

Laser-based angle-resolved photoemission spectroscopy and two-photon photoemission spectroscopy are employed to study the valence electronic structure of the Weyl semimetal candidate Td-WTe2 along two high symmetry directions and for binding energies between ≈ -1 eV and 5 eV. The experimental data show a good agreement with band structure calculations. Polarization dependent measurements provide further information on initial and intermediate state symmetry properties with respect to the mirror plane of the Td structure of WTe2.