The emergence of quantization at the nanoscale, the quantum size effect (QSE), allows flexible control of matter and is a rich source of advanced functionalities. A QSE-induced transition into an insulating phase in semimetallic nanofilms was predicted for bismuth a halfcentury ago and has regained new interest with regard to its surface states exhibiting nontrivial electronic topology. Here, we reveal an unexpected mechanism of the transition by high-resolution angle-resolved photoelectron spectroscopy combined with theoretical calculations. Anomalous evolution and degeneracy of quantized energy levels indicate that increased Coulomb repulsion from the surface states deforms a quantum confinement potential with decreasing thickness. The potential deformation strongly modulates spatial distributions of quantized wave functions, which leads to acceleration of the transition beyond the original QSE picture. This discovery establishes a complete picture of the long-discussed transition and highlights a new class of size effects dominating nanoscale transport in systems with metallic surface states.
Teaser (127 characters)Increased Coulomb repulsion from surface states significantly modulates quantum confinement in topological semimetal nanofilms.
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IntroductionQuantized electronic states generated by the quantum size effect (QSE) in nano-confined systems enable unique tunability for a wide range of phenomena such as superconductivity (1), light-matter interaction (2), and non-equilibrium carrier dynamics (3). Modulations of the band gap and the density of states further improve functionalities in catalysts (4) and information devices (5). From a technological point of view, quantization inevitably affects any electronic system fabricated at the nanoscale. One of the most well-known examples is a QSE-induced metal-insulator transition, whose essence is illustrated for a film geometry in Figs. 1 (A and B). When semimetallic bulk bands are quantized, the valence-band top and the conduction-band bottom no longer cross the Fermi level ( ), and the system enters an insulating phase. In the case of a system possessing metallic surface states as typically observed in topological materials, the transition is marked by the disappearance of conducting channels in the film interior, and thereafter electric current flows only through the surfaces. The transition was first predicted a half-century ago on bismuth (Bi) (6). A Bi single crystal is a typical semimetal with small carrier pockets and three-dimensional (3D) Dirac dispersions (7), which generate unusual magneto-transport responses (8-10). Moreover, due to the large spin-orbit coupling, Bi surfaces host spin-polarized metallic states (Figs. 1, A, B, and E) that have been intensively examined in the context of electronic topology (11-16). Although theoretical calculations tended to predict trivial band topology (11, 12), angle-resolved photoelectron spectroscopy (ARPES) experiments have detected electronic band structures exhibiting nontrivial topology (13,14). A...