Electrically Tunable Wafer-Sized Three-Dimensional Topological Insulator Thin Films Grown by Magnetron Sputtering

Three-dimensional(3 D) topological insulators(TIs) are candidate materials for various electronic and spintronic devices due to their strong spin-orbit coupling and unique surface electronic structure.Rapid,low-cost preparation of large-area TI thin films compatible with conventional semiconductor technology is the key to the practical applications of TIs.Here we show that wafer-sized Bi_2 Te_3 family TI and magnetic TI films with decent quality and well-controlled composition and properties can be prepared on amorphous SiO_2/Si substrates by magnetron cosputtering.The SiO_2/Si substrates enable us to electrically tune(Bi_(1-x)Sb_x)_2 Te_3 and Cr-doped(Bi_(1-x)Sb_x)_2 Te_3 TI films between p-type and n-type behavior and thus study the phenomena associated with topological surface states,such as the quantum anomalous Hall effect(QAHE).This work significantly facilitates the fabrication of TI-based devices for electronic and spintronic applications.     

From magnetically doped topological insulator to the quantum anomalous Hall effect

Quantum Hall effect （QHE）, as a class of quantum phenomena that occur in macroscopic scale, is one of the most important topics in condensed matter physics. It has long been expected that QHE may occur without Landau levels so that neither external magnetic field nor high sample mobility is required for its study and application, Such a QHE free of Landau levels, can appear in topological insulators （TIs） with ferromagnetism as the quantized version of the anomalous Hall effect, i.e., quantum anomalous Hall （QAH） effect. Here we review our recent work on experimental realization of the QAH effect in magnetically doped TIs. With molecular beam epitaxy, we prepare thin films of Cr-doped （Bi,Sb）2Te3 TIs with well- controlled chemical potential and long-range ferromagnetic order that can survive the insulating phase. In such thin films, we eventually observed the quantization of the Hall resistance at h/e2 at zero field, accompanied by a considerable drop in the longitudinal resistance. Under a strong magnetic field, the longitudinal resistance vanishes, whereas the Hall resistance remains at the quantized value. The realization of the QAH effect provides a foundation for many other novel quantum phenomena predicted in TIs, and opens a route to practical applications of quantum Hall physics in low-power-consumption electronics.     

Quantum Anomalous Hall Multilayers Grown by Molecular Beam Epitaxy

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 doped(Bi,Sb)_2Te_3 topological insulator and Cd Se normal insulator layers grown by molecular beam epitaxy. The obtained multilayer samples show quantized Hall resistance h/N_e~2, where h is Planck's constant, e is the elementary charge and N is the number of the magnetic topological insulator layers, resembling a high Chern number QAH insulator. The QAH multilayers provide an excellent platform to study various topological states of matter.     

Modification of the Hybridization Gap by Twisted Stacking of Quintuple Layers in a Three-Dimensional Topological Insulator Thin Film

Twisting the stacking of layered materials leads to rich new physics. A three-dimensional topological insulator film hosts two-dimensional gapless Dirac electrons on top and bottom surfaces, which, when the film is below some critical thickness, will hybridize and open a gap in the surface state structure. The hybridization gap can be tuned by various parameters such as film thickness and inversion symmetry, according to the literature. The three-dimensional strong topological insulator Bi(Sb)Se(Te) family has layered structures composed of quintuple layers(QLs) stacked together by van der Waals interaction. Here we successfully grow twistedly stacked Sb_2Te_3 QLs and investigate the effect of twist angels on the hybridization gaps below the thickness limit. It is found that the hybridization gap can be tuned for films of three QLs, which may lead to quantum spin Hall states.Signatures of gap-closing are found in 3-QL films. The successful in situ application of this approach opens a new route to search for exotic physics in topological insulators.     

Experimental Realization of an Intrinsic Magnetic Topological Insulator

An intrinsic magnetic topological insulator(TI) is a stoichiometric magnetic compound possessing both inherent magnetic order and topological electronic states. Such a material can provide a shortcut to various novel topological quantum effects but remained elusive experimentally for a long time. Here we report the experimental realization of thin films of an intrinsic magnetic TI, MnBi_2Te_4, by alternate growth of a Bi_2Te_3 quintuple layer and a MnTe bilayer with molecular beam epitaxy. The material shows the archetypical Dirac surface states in angle-resolved photoemission spectroscopy and is demonstrated to be an antiferromagnetic topological insulator with ferromagnetic surfaces by magnetic and transport measurements as well as first-principles calculations. The unique magnetic and topological electronic structures and their interplays enable the material to embody rich quantum phases such as quantum anomalous Hall insulators and axion insulators at higher temperature and in a well-controlled way.     

Visualizing the in-Gap States in Domain Boundaries of Ultra-Thin Topological Insulator Films

Ultra-thin topological insulators provide a platform for realizing many exotic phenomena such as the quantum spin Hall effect, and quantum anomalous Hall effect. These effects or states are characterized by quantized transport behavior of edge states. Experimentally, although these states have been realized in various systems,the temperature for the edge states to be the dominating channel in transport is extremely low, contrary to the fact that the bulk gap is usually in the order of a few tens of milli-electron volts. There must be other in-gap conduction channels that do not freeze out until a much lower temperature. Here we grow ultra-thin topological insulator Bi_2Te_3 and Sb_2Te_3 films by molecular beam epitaxy and investigate the structures of domain boundaries in these films. By scanning tunneling microscopy and spectroscopy we find that the domain boundaries with large rotation angles have pronounced in-gap bound states, through which one-dimensional conduction channels are suggested to form, as visualized by spatially resolved spectroscopy. Our work indicates the critical role played by domain boundaries in degrading the transport properties.     

高质量稀磁半导体(Ga,Mn)Sb单晶薄膜分子束外延生长

理论预言窄禁带稀磁半导体(Ga,Mn)Sb及其异质结构可能存在量子反常霍尔效应等新奇特性, 近年来受到了特别关注. 但是, 由于(Ga,Mn)Sb薄膜生长窗口窄, 纯相(Ga,Mn)Sb薄膜制备比较困难, 迄今关于这类材料的研究报道为数不多. 本文采用低温分子束外延的方法, 通过优化生长条件, 成功制备出厚度为10 nm, Mn含量在0.016至0.039之间的多组(Ga,Mn)Sb薄膜样品. 生长过程中反射式高能电子衍射原位监测和磁性测量都表明没有MnSb等杂相的偏析, 同时原子力显微镜图像表明其表面形貌平滑, 粗糙度小. 通过生长后退火处理, (Ga,Mn)Sb薄膜的最高居里温度达到30 K. 此外, 本文研究了霍尔电阻和薄膜电阻随磁场的变化关系, 在低温下观测到明显的反常霍尔效应.     

Raman spectra and XPS studies of phase changes in Ge2Sb2Te5 films

Ge_2Sb_2Te_5 film was deposited by RF magnetron sputtering on Si (100) substrate. The structure of amorphous and crystalline Ge_2Sb_2Te_5 thin films was investigated using XRD, Raman spectra and XPS. XRD measurements revealed the existence of two different crystalline phases, which has a FCC structure and a hexagonal structure, respectively. The broad peak in the Raman spectra of amorphous Ge_2Sb_2Te_5 film is due to the amorphous －Te－-Te－ stretching. As the annealing temperature increases, the broad peak separates into two peaks, which indicates that the heteropolar bond in GeTe_4 and the Sb－Sb bond are connected with four Te atoms, and other units such as (TeSb) Sb－Sb (Te_2) and (Sb_2) Sb－Sb (Te_2), where some of the four Te atoms in the above formula are replaced by Sb atoms, remain in crystalline Ge_2Sb_2Te_5 thin film. And from the results of Raman spectra and XPS, higher the annealing temperature, more Te atoms bond to Ge atoms and more Sb atoms substitute Te in (Te_2) Sb－Sb (Te_2).     

Anomalous Hall Effect in Layered Ferrimagnet MnSb_2Te_4

We report on low-temperature electron transport properties of MnSb_2Te_4,a candidate of ferrimagnetic Weyl semimetal.Long-range magnetic order is manifested as a nearly square-shaped hysteresis loop in the anomalous Hall resistance,as well as sharp jumps in the magnetoresistance.At temperatures below 4K,a lnT-type upturn appears in the temperature dependence of longitudinal resistance,which can be attributed to the electron-electron interaction(EEI),since the weak localization can be excluded by the temperature dependence of magnetoresistance.Although the anomalous Hall resistance exhibits a similar lnT-type upturn in the same temperature range,such correction is absent in the anomalous Hall conductivity.Our work demonstrates that MnSb_2Te_4 microflakes provide an ideal system to test the theory of EEI correction to the anomalous Hall effect.     

Detection of Magnetic Gap in Topological Surface States of MnBi_2Te_4

Recently, intrinsic antiferromagnetic topological insulator MnBi_2Te_4 has drawn intense research interest and leads to plenty of significant progress in physics and materials science by hosting quantum anomalous Hall effect, axion insulator state, and other quantum phases. An essential ingredient to realize these quantum states is the magnetic gap in the topological surface states induced by the out-of-plane ferromagnetism on the surface of MnBi_2Te_4.However, the experimental observations of the surface gap remain controversial. Here, we report the observation of the surface gap via the point contact tunneling spectroscopy. In agreement with theoretical calculations, the gap size is around 50 me V, which vanishes as the sample becomes paramagnetic with increasing temperature.The magnetoresistance hysteresis is detected through the point contact junction on the sample surface with an out-of-plane magnetic field, substantiating the surface ferromagnetism. Furthermore, the non-zero transport spin polarization coming from the ferromagnetism is determined by the point contact Andreev reflection spectroscopy.Combining these results, the magnetism-induced gap in topological surface states of MnBi_2Te_4 is revealed.     

Sb_2Te_3热电薄膜的离子束溅射制备与表征

采用离子束溅射技术交替沉积Sb-Te-Sb多层薄膜后进行高真空热处理,直接制备Sb2Te3薄膜.利用X射线衍射(XRD)仪、霍尔系数测试仪、薄膜Seebeck系数测量系统对所制备的薄膜特性进行表征.XRD测量结果显示,薄膜的主要衍射峰与Sb2Te3标准衍射峰相同,在[101]/[012]晶向取向明显,存在较多的Te杂质峰;霍尔系数测试结果表明,薄膜为p型半导体薄膜,薄膜电阻率较低,其电导率接近于金属电导率,载流子浓度量级为1023cm-3,具有良好的电学性能;Seebeck系数测量结果显示,薄膜具有良好的热电性能,在不同条件下制备的薄膜的Seebeck系数在7.8—62μV/K范围;在所制备的薄膜中,退火时间为6h、退火温度为200℃的薄膜其Seebeck系数达到最大,约为62μV/K,且电阻率最小.     

Shubnikov-de Haas effect and semimetal-semiconductor transition in bismuth-antimony alloys in high magnetic fields

Shubnikov-de Haas effect is observed in Bi and BiSb alloys (containing 0.1?4.4 at.% Sb) in pulsed high magnetic fields up to 420 kG. It is found that the amplitude of the quantum oscillation remarkably increases by mixing a small amount of Sb in Bi, and that the magnitude of the Hall electric field in BiSb alloy (0.1 at.% Sb) is much larger than that in pure Bi. These observations demonstrate the difference in the scattering mechanism of carriers between Bi and BiSb alloys. The magnetic field induced semimetal to semiconductor transition is observed in BiSb alloy with 4.4 at.% Sb. From the analysis of the Shubnikov-de Haas oscillation in BiSb, the field at which the semimetal to semiconductor transition will occur in Bi is estimated as about 1 MG for the field direction parallel to the binary axis.     

Observation of ferromagnetism and anomalous Hall effect in laser-deposited chromium-doped indium tin oxide films

We report on the structural, magnetic, and magnetotransport characteristics of Cr-doped indium tin oxide (ITO) films grown on SiO₂/Si substrates by pulsed laser deposition. Structural analysis clearly indicates that homogeneous films of bixbyite structure are grown without any detectable formation of secondary phases up to 20 mol% Cr doping. The carrier concentration is found to decrease with Cr ion addition, displaying a change in the conduction type from n-type to p-type around 15 mol% Cr doping. Room temperature ferromagnetism is observed, with saturation magnetization of ∼0.7 emu/cm³, remnant magnetization of ∼0.2 emu/cm³ and coercive field of ∼30 Oe for 5 mol% Cr-doped ITO. Magnetotransport measurements reveal the unique feature of diluted magnetic semiconductors, in particular, an anomalous Hall effect governed by electron doping, which indicates the intrinsic nature of ferromagnetism in Cr-doped ITO. These results suggest that Cr-doped ITO could be promising for semiconductor spin electronics devices.     

Characteristics of Ti0.97Co0.03O2:Sb0.01 dilute magnetic semiconducting thin films deposited at 500 °C by pulsed laser deposition

Epitaxial Ti_0.97Co_0.03O₂:Sb_0.01(TCO:Sb) films were deposited on R-Al₂O₃ (1 1 0 2) substrates at 500 °C in various deposition pressures by pulsed laser deposition. The solubility of cobalt within the films increases with decreasing deposition pressure at a deposition temperature of 500 °C. The TCO:Sb films deposited at 5×10⁻⁶ Torr exhibit a p-type anomalous Hall effect having a hole concentration of 6.1×10²²/cm³ at 300 K. On the other hand, films deposited at 4×10⁻⁴ Torr exhibits an n-type anomalous Hall effect having an electron concentration of about 1.1×10²¹/cm³. p- or n-type DMS characteristics depends on the change of the structure of TCO:Sb films and the solubility of Co is possible by controlling the deposition pressure.     

Weyl semimetal in a topological insulator multilayer

We propose a simple realization of the three-dimensional (3D) Weyl semimetal phase, utilizing a multilayer structure, composed of identical thin films of a magnetically doped 3D topological insulator, separated by ordinary-insulator spacer layers. We show that the phase diagram of this system contains a Weyl semimetal phase of the simplest possible kind, with only two Dirac nodes of opposite chirality, separated in momentum space, in its band structure. This Weyl semimetal has a finite anomalous Hall conductivity and chiral edge states and occurs as an intermediate phase between an ordinary insulator and a 3D quantum anomalous Hall insulator. We find that the Weyl semimetal has a nonzero dc conductivity at zero temperature, but Drude weight vanishing as T(2), and is thus an unusual metallic phase, characterized by a finite anomalous Hall conductivity and topologically protected edge states.     

Effects of Thickness and Temperature on Thermoelectric Properties of Bi_2Te_3-Based Thin Films

Bi_2Te_3 thin films and GeTe/B_2Te_3 superlattices of different thicknesses are prepared on the silicon dioxide substrates by magnetron sputtering technique and thermally annealed at 573 K for 30 min. Thermoelectric(TE)measurements indicate that optimal thickness and thickness ratio improve the TE performance of Bi_2Te_3 thin films and GeTe/B_2Te_3 superlattices, respectively. High TE performances with figure-of-merit(ZT) values as high as 1.32 and 1.56 are achieved at 443 K for 30 nm and 50 nm Bi_2Te_3 thin films, respectively. These ZT values are higher than those of p-type Bi_2Te_3 alloys as reported. Relatively high ZT of the GeTe/B_2Te_3 superlattices at 300-380 K were 0.62-0.76. The achieved high ZT value may be attributed to the unique nano-and microstructures of the films,which increase phonon scattering and reduce thermal conductivity. The results indicate that Bi_2Te_3-based thin films can serve as high-performance materials for applications in TE devices.     

Quantum anomalous Hall effect and giant Rashba spin-orbit splitting in graphene system co-doped with boron and 5d transition-metal atoms

Quantum anomalous Hall effect (QAHE) is a fundamental quantum transport phenomenon in condensed matter physics. Until now, the QAHE has only been experimentally realized for Cr/V-doped (Bi, Sb)₂Te₃ but at an extremely low observational temperature, thereby limiting its potential application in dissipationless quantum electronics. By employing first-principles calculations, we study the electronic structures of graphene co-doped with 5d transition metal and boron atoms based on a compensated n–p co-doping scheme. Our findings are as follows: i) The electrostatic attraction between the n- and p-type dopants effectively enhances the adsorption of metal adatoms and suppresses their undesirable clustering. ii) Hf-B and Os-B co-doped graphene systems can establish long-range ferromagnetic order and open larger nontrivial band gaps because of the stronger spin-orbit coupling with the non-vanishing Berry curvatures to host the high-temperature QAHE. iii) The calculated Rashba splitting energies in Re–B and Pt–B co-doped graphene systems can reach up to 158 and 85 meV, respectively, which are several orders of magnitude higher than the reported intrinsic spin-orbit coupling strength.     

Control of topological phase transitions in Dirac semimetal films by exchange fields

The exchange field effects on topological Dirac semimetal(DSM) films are discussed in this article. A topological phase transition can be controlled by tuning the exchange field together with the quantum confinement effects. What is more interesting is that the system can transit into the quantum anomalous Hall(QAH) state from the topologically trivial state(Z_2 = 0) or from the topologically nontrivial state(Z_2 = 1), depending on the thickness of the DSM films. This provides a useful mechanism to realize the QAH state from the DSM.     

The anomalous strain resistor effect in Bi2−xSbxTe3 polycrystalline films

The structure, electrophysical and deformational properties of (Bi, Sb)₂Te₃ polycrystalline films with anomalous strain-sensitivity (K ～ 10⁴) were investigated. The presence of empty interleaves between conductive regions crossing current lines was established. An account of the peculiarities of temperature dependence of electrophysical parameters allowed us to come to a conclusion that charge carrier transfer in films occurred by tunneling across interleaves. The high films' strain-sensitivity was stipulated by modulation of thickness of empty interleaves (correspondingly to transparency of tunnel barrier) at uniaxial deformation.