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 ($μ$ = 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.
Epitaxial thin films of 1T-HfTe2 semimetal are grown by MBE on AlN(0001) substrates. The measured in-plane lattice parameter indicates an unstrained film which is also azimuthally aligned with the AlN substrate, albeit with an in-plane mosaic spread, as it would be expected for van der Waals epitaxy. Angle resolved photoemission spectroscopy combined with first principles electronic band structure calculations show steep linearly dispersing conduction and valence bands which cross near the Brillouin zone center, providing evidence that HfTe2 /AlN is an epitaxial topological Dirac semimetal.
Here, we report a detailed method of growing LaAlGe, a non-magnetic Weyl semimetal, thin film on silicon(100) substrates by molecular beam epitaxy and their structural and electrical characterizations. 50 nm thick LaAlGe films were deposited and annealed for 16 hours in situ at a temperature 793 K. As-grown high-quality films showed uniform surface topography and near ideal stoichiometry with a body-centered tetragonal crystal structure. Temperature-dependent longitudinal resistivity can be understood with dominant interband s-d electron-phonon scattering in the temperature range 5-40 K. Hall …
Rare earth compounds display diverse electronic, magnetic, and magneto-transport properties. Recently these compounds of the type RAlGe (R = La, Ce, Pr) have been shown to exhibit Weyl semimetallic behavior. In this work, we have investigated the crystal structure, electronic, and magneto-transport properties of the Weyl semimetal LaAlGe thin films grown by molecular beam epitaxy. The temperature dependence of longitudinal resistivity at different magnetic fields is discussed. Observations of magnetoresistances and Hall effect at different temperatures and their evolution with magnetic field u…
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 diff…
Thin crystalline layers of TaAs Weyl semimetal (9 and 18 nm thick) are grown by molecular beam epitaxy on GaAs(001) substrates. The (001) planes of the tetragonal TaAs lattice are parallel to the GaAs(001) substrate, but the corresponding in-plane crystallographic directions of the substrate and the layer are rotated by 45°. In spite of a substantial lattice mismatch (about 19%) between GaAs(001) substrate and TaAs epilayer no misfit dislocations are observed at the GaAs(001)/TaAs(001) interface. Only stacking fault defects in TaAs are detected with transmission electron microscopy. Thorough X…
We present a study on magnetotransport in films of the topological Dirac semimetal Cd$_{3}$As$_{2}$ doped with Sb grown by molecular beam epitaxy. In our weak antilocalization analysis, we find a significant enhancement of the spin-orbit scattering rate, indicating that Sb doping leads to a strong increase of the pristine band-inversion energy. We discuss possible origins of this large enhancement by comparing Sb-doped Cd$_{3}$As$_{2}$ with other compound semiconductors. Sb-doped Cd$_{3}$As$_{2}$ will be a suitable system for further investigations and functionalization of topological Dirac se…
(001)-oriented thin films of the three-dimensional Dirac semimetal cadmium arsenide can realize a quantum spin Hall insulator and other kinds of topological physics, all within the flexible architecture of epitaxial heterostructures. Here, we report a method for growing (001) cadmium arsenide films using molecular beam epitaxy. The introduction of a thin indium arsenide wetting layer improves surface morphology and structural characteristics, as measured by x-ray diffraction and reflectivity, atomic force microscopy, and scanning transmission electron microscopy. The electron mobility of 50-nm…
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 film…
Molecular beam epitaxy offers an exciting avenue for investigating the behavior of topological semimetal Cd3As2, by providing routes for doping, alloying, strain engineering, and heterostructure formation. To date, however, minimal exploration has been devoted to the impact of defects that are incorporated into epilayers due to contraints imposed by the substrate and narrow growth window. Here, we use a combination of lattice-matched ZnxCd1-xTe buffer layers, miscut substrates and broadband illumination to study how dislocations, twins and point defects influence the electron mobility of Cd3As…
Perovskite SrIrO3 has long been proposed as an exotic semimetal induced by the interplay between the spin-orbit coupling and electron correlations. However, its low-lying electronic structure is still lacking. We synthesize high-quality perovskite SrIrO3 (100) films by means of oxide molecular beam epitaxy, and then systemically investigate their low energy electronic structure using in-situ angle-resolved photoemission spectroscopy. We find that the hole-like bands around R and the electron-like bands around U(T) intersect the Fermi level simultaneously, providing the direct evidence of the s…
We study the temperature dependence ($77$ K - $475$ K) of the longitudinal resistivity and Hall coefficient of thin films (thickness $20$ nm) of three dimensional topological Dirac semimetal Na$_3$Bi grown via molecular beam epitaxy (MBE). The temperature-dependent Hall coefficient is electron-like at low temperature, but transitions to hole-like transport around $200$ K. We develop a model of a Dirac band with electron-hole asymmetry in Fermi velocity and mobility (assumed proportional to the square of Fermi velocity) which explains well the magnitude and temperature dependence of the Hall re…
A quantum spin hall insulator(QSHI) is manifested by its conducting edge channels that originate from the nontrivial topology of the insulating bulk states. Monolayer 1T'-WTe2 exhibits this quantized edge conductance in transport measurements, but because of its semimetallic nature, the coherence length is restricted to around 100 nm. To overcome this restriction, we propose a strain engineering technique to tune the electronic structure, where either a compressive strain along a axis or a tensile strain along b axis can drive 1T'-WTe2 into an full gap insulating phase. A combined study of mol…
MX monopnictide compounds (M=Nb,Ta, X = As,P) are prototypical three-dimensional Weyl semimetals (WSMs) that have been shown in bulk single crystal form to have potential for a wide variety of novel devices due to topologically protected band structures and high mobilities. However, very little is known about thin film synthesis, which is essential to enable device applications. We synthesize TaAs(001) epilayers by molecular beam epitaxy on GaAs(001) and provide an experimental phase diagram illustrating conditions for single phase, single-crystal-like growth. We investigate the relationship b…
Quantum anomalous Hall (QAH) effect is a quantum Hall effect that occurs without the need of external magnetic field. A system composed of multiple parallel QAH layers is an effective high Chern number QAH insulator and the key to the applications of the dissipationless chiral edge channels in low energy consumption electronics. Such a QAH multilayer can also be engineered into other exotic topological phases such as a magnetic Weyl semimetal with only one pair of Weyl points. This work reports the first experimental realization of QAH multilayers in the superlattices composed of magnetically …
Thin films of the ferromagnet Fe$_2$Ge were grown via molecular beam epitaxy, and their electrical and magneto-transport properties measured for the first time. X-ray diffraction and vibrating sample magnetometry measurements confirmed the crystalline ferromagnetic Fe$_2$Ge phase. The observed high temperature maximum in the longitudinal resistivity, as well as the observed suppression of electron-magnon scattering at low temperatures, point to the presence of strong spin polarization in this material. Measurements of the Hall resistivity, $ρ_{xy}$, show contributions from both the ordinary Ha…
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 …
In-plane compressively strained $α$-Sn films have been theoretically predicted and experimentally proven to possess non-trivial electronic states of a 3D topological Dirac semimetal. The robustness of these states typically strongly depends on purity, homogeneity and stability of the grown material itself. By developing a reliable fabrication process, we were able to grow pure strained $α$-Sn films on InSb(100), without heating of the substrate during growth, nor using any dopants. The $α$-Sn films were grown by molecular beam epitaxy, followed by experimental verification of the achieved chem…
PtTe2 and PtSe2 with trigonal structure have attracted extensive research interests since the discovery of type-II Dirac fermions in the bulk crystals. The evolution of the electronic structure from bulk 3D topological semimetal to 2D atomic thin films is an important scientific question. While a transition from 3D type-II Dirac semimetal in the bulk to 2D semiconductor in monolayer (ML) film has been reported for PtSe2, so far the evolution of electronic structure of atomically thin PtTe2 films still remains unexplored. Here we report a systematic angle-resolved photoemission spectroscopy (AR…
Magnetic doping of topological quantum materials provides an attractive route for studying the effects of time-reversal symmetry breaking. Thus motivated, we explore the introduction of the transition metal Mn into thin films of the Dirac semimetal Cd3As2 during growth by molecular beam epitaxy. Scanning transmission electron microscopy measurements show the formation of a Mn-rich phase at the top surface of Mn-doped Cd3As2 thin films grown using both uniform doping and delta doping. This suggests that Mn acts as a surfactant during epitaxial growth of Cd3As2, resulting in phase separation. Ma…
Recently, Cd3As2 has attracted intensive research interest as an archetypical Dirac semimetal, hosting three-dimensional linear-dispersive electronic bands near the Fermi level. Previous studies have shown that single-crystalline Cd3As2 has an anomalously low lattice thermal conductivity, ranging from 0.3 W/mK to 0.7 W/mK at 300 K, which has been attributed to point defects. In this work, we combine first-principles lattice dynamics calculations and temperature-dependent high-resolution Raman spectroscopy of high-quality single-crystal thin films grown by molecular beam epitaxy to reveal the e…
Toward Tunable Magnetic Dirac Semimetals: Mn Doping of Cd$_3$As$_2$
National Laboratory of the Rockies（落基山国家实验室）；King's College London（伦敦国王学院）；National High Magnetic Field Laboratory（国家高磁场实验室）；National Renewable Energy Laboratory（美国国家可再生能源实验室）；University of Colorado, Boulder（科罗拉多大学博尔德分校）
We investigate structural and transport properties of highly Ru-deficient SrRu0.7O3 thin films prepared by molecular beam epitaxy on (001) SrTiO3 substrates. To distinguish the influence of the two types of disorders in the films, Ru vacancies within lattices and disorders near the interface, SrRu0.7O3 thin films with various thicknesses (t = 1-60 nm) were prepared. It was found that the influence of the former dominates the electrical and magnetic properties when t > 5-10 nm, while that of the latter does when t < 5-10 nm. Structural characterizations revealed that the crystallinity, in terms…
Weyl Semimetals (WSMs), a recently discovered topological state of matter, exhibit an electronic structure governed by linear band dispersions and degeneracy (Weyl) points leading to rich physical phenomena, which are yet to be exploited in thin film devices. While WSMs were established in the monopnictide compound family several years ago, the growth of thin films has remained a challenge. Here, we report the growth of epitaxial thin films of NbP and TaP by means of molecular beam epitaxy. Single crystalline films are grown on MgO (001) substrates using thin Nb (Ta) buffer layers, and are fou…
Cadmium arsenide (Cd3As2) is one of the first materials to be discovered to belong to the class of three-dimensional topological semimetals. Reported room temperature crystal structures of Cd3As2 reported differ subtly in the way the Cd vacancies are arranged within its antifluorite-derived structure, which determines if an inversion center is present and if Cd3As2 is a Dirac or Weyl semimetal. Here, we apply convergent beam electron diffraction (CBED) to determine the point group of Cd3As2 thin films grown by molecular beam epitaxy. Using CBED patterns from multiple zone axes, high-angle annu…
Epitaxial thin films of (Sn$_{x}$Pb$_{1-x}$)$_{1-y}$In$_{y}$Te were successfully grown by molecular-beam-epitaxy (MBE) in a broad range of compositions (0 $\leq$ x $\leq$ 1, 0 $\leq$ y $\leq$ 0.23). We investigated electronic phases of the films by the measurements of electrical transport and optical second harmonic generation. In this system, one can control the inversion of band gap, the electric polarization that breaks the inversion symmetry, and the Fermi level position by tuning the Pb/Sn ratio and In composition. A plethora of topological electronic phases are expected to emerge, such a…
Thickness-Dependent Spintronic Terahertz Emission in MBE-Grown PtTe$_2$: From Semiconductor to Type-II Dirac Semimetal
Univ. Grenoble Alpes, CEA, CNRS, IRIG-SPINTEC（格勒诺布尔阿尔卑斯大学、法国原子能和替代能源委员会、法国国家科学研究中心、IRIG自旋技术中心）；Centre for Nanodiagnostics of Materials, Faculty of Materials Science and Technology, Slovak University of Technology（材料纳米诊断中心、材料与科技学院、斯洛伐克科技大学）
Realizing quantum materials in few atomic layer morphologies is a key to both observing and controlling a wide variety of exotic quantum phenomena. This includes topological electronic materials, where the tunability and dimensionality of few layer materials have enabled the detection of $Z_2$, Chern, and Majorana phases. Here, we report the development of a platform for thin film correlated, topological states in the magnetic rare-earth monopnictide ($RX$) system GdBi synthesized by molecular beam epitaxy. This material is known from bulk single crystal studies to be semimetallic antiferromag…
We report the measurement of efficient charge-to-spin conversion at room temperature in Weyl semimetal/ferromagnet heterostructures with both oxidized and pristine interfaces. Polycrystalline films of the Weyl semimetal, TaAs, are grown by molecular beam epitaxy on (001) GaAs and interfaced with a metallic ferromagnet (Ni$_{0.8}$Fe$_{0.2}$). Spin torque ferromagnetic resonance (ST-FMR) measurements in samples with an oxidized interface yield a spin torque efficiency as large as $ξ_{\mathrm{FMR}}=0.45\pm 0.25$ for a 8 nm Ni$_{0.8}$Fe$_{0.2}$ layer thickness. By studying ST-FMR in these samples …
Na3Bi has attracted significant interest in both bulk form as a three-dimensional topological Dirac semimetal and in ultra-thin form as a wide-bandgap two-dimensional topological insulator. Its extreme air sensitivity has limited experimental efforts on thin- and ultra-thin films grown via molecular beam epitaxy to ultra-high vacuum environments. Here we demonstrate air-stable Na3Bi thin films passivated with magnesium difluoride (MgF2) or silicon (Si) capping layers. Electrical measurements show that deposition of MgF2 or Si has minimal impact on the transport properties of Na3Bi whilst in ul…
Motivated by observations of extreme magnetoresistance (XMR) in bulk crystals of rare-earth monopnictide (RE-V) compounds and emerging applications in novel spintronic and plasmonic devices based on thin-film semimetals, we have investigated the electronic band structure and transport behavior of epitaxial GdSb thin films grown on III-V semiconductor surfaces. The Gd3+ ion in GdSb has a high spin S=7/2 and no orbital angular momentum, serving as a model system for studying the effects of antiferromagnetic order and strong exchange coupling on the resulting Fermi surface and magnetotransport pr…
In a Weyl orbit, the Fermi arc surface states on opposite surfaces of the topological semimetal are connected through the bulk Weyl or Dirac nodes. Having a real-space component, these orbits accumulate a sample-size-dependent phase. Following recent work on the three-dimensional Dirac semimetal cadmium arsenide (Cd3As2), we have sought evidence for this thickness-dependent effect in quantum oscillations and quantum Hall plateaus in (112)-oriented Cd3As2 thin films grown by molecular beam epitaxy. We compare quantum transport in films of varying thickness at apparently identical gate-tuned car…
Cd3As2 has long been known as a high-mobility semiconductor. The recent finding of a topological semimetal state in this compound has demanded growth of epitaxial films with high crystallinity and controlled thickness. Here we report the structural characterisation of Cd3As2 films grown on SrTiO3 substrates by solid-phase epitaxy at high temperatures up to 600 C by employing optimised capping layers and substrates. The As triangular lattice is epitaxially stacked on the Ti square lattice of the (001) SrTiO3 substrate, producing (112)-oriented Cd3As2 films exhibiting high crystallinity with a r…
Dirac nodal line semimetals (DNLSs) host relativistic quasiparticles in their one-dimensional (1D) Dirac nodal line (DNL) bands that are protected by certain crystalline symmetries. Their novel low-energy fermion quasiparticle excitations and transport properties invite studies of relativistic physics in the solid state where their linearly dispersing Dirac bands cross at continuous lines with four-fold degeneracy. In materials studied up to now, the four-fold degeneracy, however, has been vulnerable to suppression by the ubiquitous spin-orbit coupling (SOC). Despite the current effort to disc…
Electrostatic doping in materials can lead to various exciting electronic properties, such as metal-insulator transition and superconductivity, by altering the Fermi level position or introducing exotic phases. Cd3As2, a three-dimensional (3D) analog of graphene with extraordinary carrier mobility, was predicted to be a 3D Dirac semimetal, a feature confirmed by recent experiments. However, most research so far has been focused on metallic bulk materials that are known to possess ultra-high mobility and giant magnetoresistance but limited carrier transport tunability. Here, we report on the fi…
Magnetic Weyl fermions, which occur in magnets, have novel transport phenomena related to pairs of Weyl nodes, and they are, of both, scientific and technological interest, with the potential for use in high-performance electronics, spintronics and quantum computing. Although magnetic Weyl fermions have been predicted to exist in various oxides, evidence for their existence in oxide materials remains elusive. SrRuO3, a 4d ferromagnetic metal often used as an epitaxial conducting layer in oxide heterostructures, provides a promising opportunity to seek for the existence of magnetic Weyl fermion…
One of the basic assumptions in organic field-effect transistors, the most fundamental device unit in organic electronics, is that charge transport occurs two-dimensionally in the first few molecular layers near the dielectric interface. Although the mobility of bulk organic semiconductors has increased dramatically, direct probing of intrinsic charge transport in the two-dimensional limit has not been possible due to excessive disorders and traps in ultrathin organic thin films. Here, highly ordered mono- to tetra-layer pentacene crystals are realized by van der Waals (vdW) epitaxy on hexagon…
Recent observation of quantum transport phenomena of Weyl fermions has brought much attention to 4d ferromagnetic perovskite SrRuO3 as a magnetic Weyl semimetal. Besides, the hump-like Hall effect anomaly, which might have a topological origin, has also been reported for this material. Here, we show that the emergence of such phenomena is governed by the degree of scattering determined by the defect density (Ru-deficiency- and/or interface-driven-defect scattering) and measurement temperature (phonon scattering), where the former is controlled by varying the growth conditions of the SrRuO3 fil…
