The topology of pure Bi is controversial because of its very small ($sim$10 meV) band gap. Here we perform high-resolution angle-resolved photoelectron spectroscopy measurements systematically on 14$-$202 bilayers Bi films. Using high-quality films, we succeed in observing quantized bulk bands with energy separations down to $sim$10 meV. Detailed analyses on the phase shift of the confined wave functions precisely determine the surface and bulk electronic structures, which unambiguously show nontrivial topology. The present results not only prove the fundamental property of Bi but also introduce a capability of the quantum-confinement approach.
The mathematical field of topology has become a framework to describe the low-energy electronic structure of crystalline solids. A typical feature of a bulk insulating three-dimensional topological crystal are conducting two-dimensional surface states. This constitutes the topological bulk-boundary correspondence. Here, we establish that the electronic structure of bismuth, an element consistently described as bulk topologically trivial, is in fact topological and follows a generalized bulk-boundary correspondence of higher-order: not the surfaces of the crystal, but its hinges host topologically protected conducting modes. These hinge modes are protected against localization by time-reversal symmetry locally, and globally by the three-fold rotational symmetry and inversion symmetry of the bismuth crystal. We support our claim theoretically and experimentally. Our theoretical analysis is based on symmetry arguments, topological indices, first-principle calculations, and the recently introduced framework of topological quantum chemistry. We provide supporting evidence from two complementary experimental techniques. With scanning-tunneling spectroscopy, we probe the unique signatures of the rotational symmetry of the one-dimensional states located at step edges of the crystal surface. With Josephson interferometry, we demonstrate their universal topological contribution to the electronic transport. Our work establishes bismuth as a higher-order topological insulator.
Using high-resolution angle-resolved photoemission spectroscopy, the electronic structure near the Fermi level and the topological property of the Bi(111) films grown on the Bi$_2$Te$_3$(111) substrate were studied. Very different from the bulk Bi, we found another surface band near the $bar{M}$ point besides the two well-known surface bands on the Bi(111) surface. With this new surface band, the bulk valence band and the bulk conduction band of Bi can be connected by the surface states. Our band mapping revealed odd number of Fermi crossings of the surface bands, which provided a direct experimental signature that Bi(111) thin films of a certain thickness on the Bi$_2$Te$_3$(111) substrate can be topologically nontrivial in three dimension.
Bismuth has been the key element in the discovery and development of topological insulator materials. Previous theoretical studies indicated that Bi is topologically trivial and it can transform into the topological phase by alloying with Sb. However, recent high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements strongly suggested a topological band structure in pure Bi. To address this issue, we study the band structure of Bi and Sb films by ARPES and first-principles calculations. By tuning tight binding parameters, we show that Bi quantum films in topologically trivial and nontrivial phases response differently to surface perturbations. Therefore, we establish an experimental route for detecting the band topology of Bi by spectroscopic methods. In addition, our circular dichroic photoemission illuminates the rich surface states and complex spin texture of the Bi(111) surface.
The interface between a solid and vacuum can become electronically distinct from the bulk. This feature, encountered in the case of quantum Hall effect, has a manifestation in insulators with topologically protected metallic surface states. Non-trivial Berry curvature of the Bloch waves or periodically driven perturbation are known to generate it. Here, by studying the angle-dependent magnetoresistance in prismatic bismuth crystals of different shapes, we detect a robust surface contribution to electric conductivity when the magnetic field is aligned parallel to a two-dimensional boundary between the three-dimensional crystal and vacuum. The effect is absent in antimony, which has an identical crystal symmetry, a similar Fermi surface structure and equally ballistic carriers, but an inverted band symmetry and a topological invariant of opposite sign. Our observation points to the relevance of band symmetries to survival of metallicity at the boundary interrupting the cyclotron orbits.
We report the growth of self-assembled Bi2Se3 quantum dots (QDs) by molecular beam epitaxy on GaAs substrates using the droplet epitaxy technique. The QD formation occurs after anneal of Bismuth droplets under Selenium flux. Characterization by atomic force microscopy, scanning electron microscopy, X-ray diffraction, high-resolution transmission electron microscopy and X-ray reflectance spectroscopy is presented. The quantum dots are crystalline, with hexagonal shape, and have average dimensions of 12 nm height (12 quintuple layers) and 46 nm width, and a density of $8.5 cdot 10^9 cm^{-2}$. This droplet growth technique provides a means to produce topological insulator QDs in a reproducible and controllable way, providing convenient access to a promising quantum material with singular spin properties.