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Register a new userTopological Dirac Semimetal Na3Bi Films in the Ultrathin Limit via Alternating Layer Molecular Beam Epitaxy
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Ultrathin films of Na3Bi on insulating substrates are desired for opening a bulk band gap and generating the quantum spin Hall effect from a topological Dirac semimetal, though continuous films in the few nanometer regime have been difficult to realize. Here, we utilize alternating layer molecular beam epitaxy (MBE) to achieve uniform and continuous single crystal films of Na3Bi(0001) on insulating Al2O3(0001) substrates and demonstrate electrical transport on films with 3.8 nm thickness (4 unit cells). The high material quality is confirmed through in situ reflection high-energy electron diffraction (RHEED), scanning tunneling microscopy (STM), x-ray diffraction (XRD), and x-ray photoelectron spectroscopy (XPS). In addition, these films are employed as seed layers for subsequent growth by codeposition, leading to atomic layer-by-layer growth as indicated by RHEED intensity oscillations. These material advances facilitate the pursuit of quantum phenomena in thin films of Dirac semimetals.
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Rapid progress of quantum transport study in topological Dirac semimetal, including observations of quantum Hall effect in two-dimensional (2D) Cd$_{mathrm{3}}$As$_{mathrm{2}}$ samples, has uncovered even more interesting quantum transport properties in high-quality and three-dimensional (3D) samples. However, such 3D Cd$_{mathrm{3}}$As$_{mathrm{2}}$ films with low carrier density and high electron mobility have been hardly obtained. Here we report the growth and characterization of 3D thick Cd$_{mathrm{3}}$As$_{mathrm{2}}$ films adopting molecular beam epitaxy. The highest electron mobility ($mu$ = 3 $times$ 10$^{4}$ cm$^{2}$/Vs) among the reported film samples has been achieved at a low carrier density ($textit{n} = 5$ $times$ 10$^{16}$ cm$^{-3}$). In the magnetotransport measurement, Hall plateau-like structures are commonly observed in spite of the 3D thick films ($textit{t} = 120$ nm). On the other hand, field angle dependence of the plateau-like structures and corresponding Shubunikov-de Haas oscillations rather shows a 3D feature, suggesting the appearance of unconventional magnetic orbit, also distinct from the one described by the semiclassical Weyl-orbit equation.
Three-dimensional (3D) topological Dirac semimetal, when thinned down to 2D few layers, is expected to possess gapped Dirac nodes via quantum confinement effect and concomitantly display the intriguing quantum spin Hall (QSH) insulator phase. However, the 3D-to-2D crossover and the associated topological phase transition, which is valuable for understanding the topological quantum phases, remain unexplored. Here, we synthesize high-quality Na3Bi thin films with R3*R3 reconstruction on graphene, and systematically characterize their thickness-dependent electronic and topological properties by scanning tunneling microscopy/spectroscopy in combination with first-principles calculations. We demonstrate that Dirac gaps emerge in Na3Bi films, providing spectroscopic evidences of dimensional crossover from a 3D semimetal to a 2D topological insulator. Importantly, the Dirac gaps are revealed to be of sizable magnitudes on 3 and 4 monolayers (72 and 65 meV, respectively) with topologically nontrivial edge states. Moreover, the Fermi energy of a Na3Bi film can be tuned via certain growth process, thus offering a viable way for achieving charge neutrality in transport. The feasibility of controlling Dirac gap opening and charge neutrality enables realizing intrinsic high-temperature QSH effect in Na3Bi films and achieving potential applications in topological devices.
Three-dimensional (3D) topological Dirac semimetals (TDSs) represent a novel state of quantum matter that can be viewed as 3D graphene. In contrast to two-dimensional (2D) Dirac fermions in graphene or on the surface of 3D topological insulators, TDSs possess 3D Dirac fermions in the bulk. The TDS is also an important boundary state mediating numerous novel quantum states, such as topological insulators, Weyl semi-metals, Axion insulators and topological superconductors. By investigating the electronic structure of Na3Bi with angle resolved photoemission spectroscopy, we discovered 3D Dirac fermions with linear dispersions along all momentum directions for the first time. Furthermore, we demonstrated that the 3D Dirac fermions in Na3Bi were protected by the bulk crystal symmetry. Our results establish that Na3Bi is the first model system of 3D TDSs, which can also serve as an ideal platform for the systematic study of quantum phase transitions between rich novel topological quantum states.
We experimentally measure the band dispersions of topological Dirac semimetal Na3Bi using Fourier-transform scanning tunneling spectroscopy to image quasiparticle interference on the (001) surface of molecular-beam epitaxy-grown Na3Bi thin films. We find that the velocities for the lowest-lying conduction and valencebands are 1.6x10^6 m/s and 4.2x10^5 m/s respectively, significantly higher than previous theoreticalpredictions. We compare the experimental band dispersions to the theoretical band structures calculated usingan increasing hierarchy of approximations of self-energy corrections due to interactions: generalized gradientapproximation (GGA), meta-GGA, Heyd-Scuseria-Ernzerhof exchange-correlation functional (HSE06), and GW methods. We find that density functional theory methods generally underestimate the electron velocities. However, we find significantly improved agreement with an increasingly sophisticated description of the exchange and interaction potential, culminating in reasonable agreement with experiments obtained by the GW method. The results indicate that exchange-correlation effects are important in determining the electronicstructure of this Na3Bi, and are likely the origin of the high velocity. The electron velocity is consistent withrecent experiments on ultrathin Na3Bi and also may explain the ultrahigh carrier mobility observed in heavilyelectron-doped Na3Bi.
Type-II nodal line semimetal (NLS) is a new quantum state hosting one-dimensional closed loops formed by the crossing of two bands which have the same sign in their slopes along the radial direction of the loop. According to the theoretical prediction, Mg3Bi2 is an ideal candidate for studying the type-II NLS by tuning its spin-orbit coupling (SOC). In this paper, high quality Mg3Bi2 films are grown by molecular beam epitaxy (MBE). By in-situ angle resolved photoemission spectroscopy (ARPES), a pair of surface resonance bands (SRBs) around Gamma point is clearly seen. It shows that Mg3Bi2 films grown by MBE is Mg(1)-terminated by comparing the ARPES data with the first principles calculations results. And, the temperature dependent weak anti-localization (WAL) effect in Mg3Bi2 films is observed under low magnetic field, which shows a clear two dimensional (2D) e-e scattering characteristics by fitting with the Hikami-Larkin-Nagaoka (HLN) model. Combining with ARPES, magneto-transport measurements and the first principles calculations, this work proves that Mg3Bi2 is a semimetal with topological surface states TSSs, which paves the way for Mg3Bi2 as an ideal materials platform for studying the exotic features of type-II nodal line semimetals (NLSs) and the topological phase transition by tuning its SOC.
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