Rashba states have been actively revisited as a platform for advanced applications such as spintronics and topological quantum computation. Yet, access to the Rashba state is restricted to the specific material sets, and the methodology to control the Rashba state is not established. Here, we report the Rashba states on the (001) surface of KZnBi, a 3D Dirac semimetal. Using angle-resolved photoemission spectroscopy and first-principles calculations, we investigated the evolution of Rashba states under different surface conditions controlled by alkali metal deposition. We observed that restoring surface ordering enables a Rashba state, which is absent in freshly cleaved surfaces. Interestingly, we were able to modify the dispersion of the Rashba state from an ordinary parabolic dispersion to a linearly dispersing Dirac-like state by additional alkali-metal deposition. Our findings provide a methodology for engineering the properties of Rashba states for advanced applications and redefine topological systems as generic hosts of Rashba states.
In most charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-PdxTaSe2. Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, the estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields results closely resembling the known values of the superconducting dome. The results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights into the competing relationship not only for CDW but also for other competing orders.
In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole-like attribute of 2D single-crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single-crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.
Two-dimensional electrides can acquire topologically non-trivial phases due to intriguing interplay between the cationic atomic layers and anionic electron layers. However, experimental evidence of topological surface states has yet to be verified. Here, via angle-resolved photoemission spectroscopy (ARPES) and scanning tunnelling microscopy (STM), we probe the magnetic Weyl states of the ferromagnetic electride [Gd2C]2+·2e-. In particular, the presence of Weyl cones and Fermi-arc states is demonstrated through photon energy-dependent ARPES measurements, agreeing with theoretical band structure calculations. Notably, the STM measurements reveal that the Fermi-arc states exist underneath a floating quantum electron liquid on the top Gd layer, forming double-stacked surface states in a heterostructure. Our work thus not only unveils the non-trivial topology of the [Gd2C]2+·2e- electride but also realizes a surface heterostructure that can host phenomena distinct from the bulk.
The technical evolution of angle-resolved photoemission spectroscopy (ARPES) in the late 90s played a pivotal role in the exploration of electronic structures in condensed matter systems. ARPES achieved numerous successes during this period, notably capturing the first evidence of the unconventional d-wave symmetry of the superconducting gap in cuprate superconductors. It also elucidated the essential rules governing topological signatures in the electronic structures of topological materials, and played an essential role in demonstrating the engineered band structures of atomically thin materials. These early achievements spurred significant advancements in the technique. This topical review delves into four cutting-edge ARPES techniques that are currently at the forefront of development: time-resolved ARPES, nano ARPES, in-situ ARPES, and ARPES with novel control parameters. By examining the capabilities of these innovative approaches, we aim to illustrate their potential in unlocking new frontiers and providing unprecedented insights on the electronic structure of quantum materials.
We report the synthesis of ethylenediamine-intercalated NbSe2 and Li-ethylenediamine-intercalated MoSe2 single crystals with increased interlayer distances and their electronic structures measured by means of angle-resolved photoemission spectroscopy (ARPES). X-ray diffraction patterns and transmission electron microscopy images confirm the successful intercalation and an increase in the interlayer distance. ARPES measurement reveals that intercalated NbSe2 shows an electronic structure almost identical to that of monolayer NbSe2. Intercalated MoSe2 also returns the characteristic feature of the monolayer electronic structure, a direct band gap, which generates sizable photoluminescence even in the bulk form. Our results demonstrate that the properties and phenomena of the monolayer transition metal dichalcogenides can be achieved with large-scale bulk samples by blocking the interlayer interaction through intercalation.
Purely quantum electron systems exhibit intriguing correlated electronic phases by virtue of quantum fluctuations in addition to electron–electron interactions. To realize such quantum electron systems, a key ingredient is dense electrons decoupled from other degrees of freedom. Here, we report the discovery of a pure quantum electron liquid that spreads up to ~3 Å in a vacuum on the surface of an electride crystal. Its extremely high electron density and weak hybridization with buried atomic orbitals show the quantum and pure nature of the electrons, which exhibit a polarized liquid phase, as demonstrated by our spin-dependent measurement. Furthermore, upon enhancing the electron correlation strength, the dynamics of the quantum electrons change to that of a non-Fermi liquid along with an anomalous band deformation, suggestive of a transition to a hexatic liquid crystal phase. Our findings develop the frontier of quantum electron systems and serve as a platform for exploring correlated electronic phases in a pure fashion. A purely quantum electronic liquid on the surface of an electride crystal is reported.
We report the signature of a strain-controlled topological phase transition in the electronic structure of a quasione-dimensional superconductor TaSe3. Using angle-resolved photoemission spectroscopy and first-principles calculation, TaSe3 is identified to be in a weak topological insulator phase which has topologically nontrivial surface states only at the allowed planes. Under uniaxial tensile strain, a Dirac point and the topological surface state emerge on the originally forbidden (10 (1) over bar) plane, which demonstrates the transition to a strong topological insulator phase. Our results accomplish the experimental realization of possible topological insulating phases in TaSe3 and highlight the possibility of coupling the superconductivity with two distinct topological insulating phases in a controllable manner.
Transition metal dichalcogenide (TMD) semiconductors are attracting much attention in research regarding device physics based on their unique properties that can be utilized in spintronics and valleytronics. Although current studies concentrate on the monolayer form due to the explicitly broken inversion symmetry and the direct band gap, bulk materials also hold the capability of carrying spin and valley current. In this study, we report the methodology to continuously control the spin-orbit coupling (SOC) strength of bulk TMDs Mo1-xWxSe2 by changing the atomic ratio between Mo and W. The results show the size of band splitting at the K valley the measure of the coupling strength is linearly proportional to the atomic ratio of Mo and W. Our results thus demonstrate how to precisely tune the SOC coupling strength, and the collected information of which can serve as a reference for future applications of bulk TMDs.
A well-established way to find novel Majorana particles in a solid-state system is to have superconductivity arising from the topological electronic structure. To this end, the heterostructure systems that consist of normal superconductor and topological material have been actively explored in the past decade. However, a search for the single material system that simultaneously exhibits intrinsic superconductivity and topological phase has been largely limited, although such a system is far more favorable especially for the quantum device applications. Here, we report the electronic structure study of a quasi-one-dimensional (q1D) superconductor TaSe$_3$. Our results of angle-resolved photoemission spectroscopy (ARPES) and first-principles calculation clearly show that TaSe$_3$ is a topological superconductor. The characteristic bulk inversion gap, in-gap state and its shape of non-Dirac dispersion concurrently point to the topologically nontrivial nature of this material. The further investigations of the Z$_2$ indices and the topologically distinctive surface band crossings disclose that it belongs to the weak topological insulator (WTI) class. Hereby, TaSe$_3$ becomes the first verified example of an intrinsic 1D topological superconductor. It hopefully provides a promising platform for future applications utilizing Majorana bound states localized at the end of 1D intrinsic topological superconductors.