Cd3As2 Films Research Articles

Chiral anomaly and Weyl orbit in three-dimensional Dirac semimetal Cd3As2 grown on Si

Preparing Cd3As2, which is a three-dimensional (3D) Dirac semimetal in certain crystal orientation, on Si is highly desirable as such a sample may well be fully compatible with existing Si CMOS technology. However, there is a dearth of such a study regarding Cd3As2 films grown on Si showing the chiral anomaly. Here, for the first time, we report the novel preparation and fabrication technique of a Cd3As2 (112) film on a Si (111) substrate with a ZnTe (111) buffer layer which explicitly shows the chiral anomaly with a nontrivial Berry’s phase of π. Despite the Hall carrier density ( n3D≈ 9.42×1017 cm−3) of our Cd3As2 film, which is almost beyond the limit for the portents of a 3D Dirac semimetal to emerge, we observe large linear magnetoresistance in a perpendicular magnetic field and negative magnetoresistance in a parallel magnetic field. These results clearly demonstrate the chiral magnetic effect and 3D Dirac semimetallic behavior in our silicon-based Cd3As2 film. Our tailoring growth of Cd3As2 on a conventional substrate such as Si keeps the sample quality, while also achieving a low carrier concentration.

Circular Photogalvanic Current in Ni-Doped Cd3As2 Films Epitaxied on GaAs(111)B Substrate.

Magnetic element doped Cd3As2 Dirac semimetal has attracted great attention for revealing the novel quantum phenomena and infrared opto-electronic applications. In this work, the circular photogalvanic effect (CPGE) was investigated at various temperatures for the Ni-doped Cd3As2 films which were grown on GaAs(111)B substrate by molecular beam epitaxy. The CPGE current generation was found to originate from the structural symmetry breaking induced by the lattice strain and magnetic doping in the Ni-doped Cd3As2 films, similar to that in the undoped ones. However, the CPGE current generated in the Ni-doped Cd3As2 films was approximately two orders of magnitude smaller than that in the undoped one under the same experimental conditions and exhibited a complex temperature variation. While the CPGE current in the undoped film showed a general increase with rising temperature. The greatly reduced CPGE current generation efficiency and its complex variation with temperature in the Ni-doped Cd3As2 films was discussed to result from the efficient capture of photo-generated carriers by the deep-level magnetic impurity bands and enhanced momentum relaxation caused by additional strong impurity scattering when magnetic dopants were introduced.

Induced superconductivity in the two-dimensional topological insulator phase of cadmium arsenide

Hybrid structures between conventional, s-wave superconductors, and two-dimensional topological insulators (2D TIs) are a promising route to topological superconductivity. Here, we investigate planar Josephson junctions fabricated from hybrid structures that use thin films of cadmium arsenide (Cd3As2) as the 2D TI material. Measurements of superconducting interference patterns in a perpendicular magnetic field are used to extract information about the spatial distribution of the supercurrent. We show that the interference patterns are distinctly different in junctions with and without mesa-isolation. In mesa-defined junctions, the bulk of the 2D TI appears to be almost completely shunted by supercurrent flowing along the edges, whereas the supercurrent is much more uniform across the junction when the Cd3As2 film extends beyond the device. We discuss the possible origins of the observed behaviors.

Semi-Dirac and Dirac-node-arc phases in a (112) oriented Cd3As2 film

We investigate the electronic structure and spin-dependent densities of low-energy electron states in a (112) oriented Cd3As2 film. We find that the thick Cd3As2 film is a semi-Dirac material whose dispersion is linear (massless) in one direction and is quadratic (massive) in the orthogonal direction. Its spin-up and spin-down densities corresponding to linear dispersion, respectively, distribute at the top and bottom surface of the film, exhibiting the chirality of Dirac electrons, while the ones corresponding to quadratic dispersion overlap each other. In particular, an appropriate electric field vertical to the top surface of the film can result in anisotropic Rashba spin–orbit coupling and open a bandgap in the quadratic dispersions and its adjacent linear dispersions, driving a topological phase transition from a semi-Dirac-point phase to a Dirac-node-arc phase. Our findings predict a (112) oriented Cd3As2 film to be a candidate semi-Dirac material and provide a method to find Dirac-node-arc states for experiments.

Ultrafast Optical Probe of Coherent Acoustic Phonons in Dirac Semimetal Cd3As2 Film Epitaxied on GaAs(111)B Substrate.

Coherent longitudinal acoustic phonon (CAP) generation in epitaxial Dirac semimetal Cd3As2 films with different thicknesses was investigated by a time-resolved reflectance technique. The short-lived weak CAP oscillations can be observed only in the thicker Cd3As2 films, and their central frequency of 0.039 THz has no dependence on sample thickness, but is nearly inversely proportional to the probe wavelength. For the 20 nm thin film, the observed long-lived CAP with a central frequency of 0.049 THz is generated in the GaAs(111)B substrate underneath. A sound velocity of 3800 m/s for the Cd3As2 film and 5360 m/s for the GaAs(111)B substrate is thus deduced. In addition, the opposite CAP amplitude and lifetime dependence on temperature further confirms the electronic and thermal stress origination of CAP generated in GaAs(111)B and Cd3As2 film, respectively, based on the propagating strain pulse model. The central frequency of CAP is found to be stable with increasing pumping fluence and temperature, which makes Cd3As2 a potential material for thermoelectric device applications.

AC conductivity of amorphous and polycrystalline Cd3As2 films on single crystal substrates of Al2O3

In this work, we present first AC conductivity measurements of both amorphous and polycrystalline Cd3As2 thin films ( ∼50nm) in the frequency range 25–106Hz and temperature range 10–300 K. Cd3As2 thin films were grown by non-reactive AC magnetron sputtering. Both samples show a strong frequency dependence of the total conductivity in the order of 104Ω−1 cm−1. It was found that the DC conductivity, deduced from the total conductivity of Cd3As2 thin films, increases with increasing temperature. The experimental results indicate exponent values s>1 and s>2, which contradicts the universal dynamic response. In Cd3As2 films is observed a crossover of metal–semiconductor type at low temperatures, which is characteristic of topological materials. The results show a clearly frequency dependence of the mechanism of AC conductivity of Cd3As2 films in a wide range of temperatures.

Challenges to magnetic doping of thin films of the Dirac semimetal Cd3As2

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. Magnetometry measurements of such samples indicate a ferromagnetic phase with out-of-plane magnetic anisotropy. Electrical magneto-transport measurements of these films as a function of temperature, magnetic field, and chemical potential reveal a lower carrier density and higher electron mobility compared to pristine Cd3As2 films grown under similar conditions. This suggests that the surfactant effect might also serve to getter impurities. We observe robust quantum transport (Shubnikov-de Haas oscillations and an incipient integer quantum Hall effect) in very thin (7 nm) Cd3As2 films despite being in direct contact with a structurally disordered surface ferromagnetic overlayer.

Strain-induced circular photogalvanic current in Dirac semimetal Cd3As2 films epitaxied on a GaAs(111)B substrate.

Dirac semimetal (DSM) Cd3As2 has drawn great attention for exploring the novel quantum phenomena and high-speed optoelectronic applications. The circular photogalvanic effect (CPGE) current, resulting from the optically-excited spin orientation transport, was theoretically predicted to vanish in an ideal Dirac system due to the symmetric photoexcitation about the Dirac point. Here, we reported the observation of the CPGE photocurrent in epitaxial Cd3As2 thin films grown on a GaAs(111)B substrate. The signature of the CPGE is confirmed by its sign reversal upon switching the helicity of optical radiation, as well as its dependence on the excitation incident angle and power. By comparison of the CPGE response between the films with different thicknesses, it is suggested that the observed CPGE results from the reduced structure symmetry and substantially modified electronic band structure of the Cd3As2 thin film that undergoes large epitaxial strain. Our experimental findings provide a valuable reference for the band engineering and exotic helicity-dependent photocurrent phenomena in DSMs towards their potential opto-spintronic device applications.

Features in low-temperature electrical resistivity of amorphous Cd3As2 films due to hopping conductivity with changing activation energy

Amorphous Cd3As2 films were deposited on single-crystalline SrTiO3 substrate by high-frequency non-reactive magnetron sputtering. Electrical resistivity of the film, measured within 3-75 K range, increases at cooling. Below ∼70 K, negative transverse magnetoresistance observed. Features in electrical resistivity and magnertoresistance can be attributed to variable-range hopping conductivity of the Mott type with local activation energy, which is temperature-dependent. Two temperature ranges in the hopping conductivity observed. Appearing two ranges is in qualitative accordance with the Mott-Davis energy-band model developed for amorphous semiconductors. High temperature range of the hopping conductivity is attributed to electron hops between localized states, positioned inside band tails, whereas electron hops between localized states, positioned inside Fermi-peak, can be responsible for low-temperature range. At taking into account temperature dependences of local activation energy, universal expression for various mechanisms of the hopping conductivity could be successfully applied to analyze the experimental data.

Controlling the symmetry of cadmium arsenide films by epitaxial strain

Epitaxial strains offer unique opportunities to obtain topological states in thin films and heterostructures that do not exist in their bulk counterparts. Here, we investigate the point group symmetries of coherently strained films of cadmium arsenide (Cd3As2), a prototype three-dimensional Dirac semimetal, by convergent beam electron diffraction. We report a loss of the fourfold rotational axis and adoption of the orthorhombic mmm point group in (112)-oriented films under biaxial compressive stress. (001)-oriented Cd3As2 films that are under a small biaxial tensile stress retain the fourfold rotational symmetry that protects the bulk nodes but adopt the non-centrosymmetric 4mm point group symmetry. This, in turn, suggests that (001) films adopt a different crystal structure in biaxial tension, one that differs in the arrangement of the ordered Cd vacancies that are an inherent feature of the crystal structure of Cd3As2 and that are key to its nodal electronic structure. Density functional theory calculations confirm the experimental findings of the stability of the non-centrosymmetric structure under biaxial tension, whereas the centrosymmetric structure is stable under biaxial compression. The results show that bulk Cd3As2 is already close to structural instability and showcase the extraordinary tunability of the topological states of Cd3As2.

Room-Temperature Spin Transport in Cd3As2.

As the need for ever greater transistor density increases, the commensurate decrease in device size approaches the atomic limit, leading to increased energy loss and leakage currents, reducing energy efficiencies. Alternative state variables, such as electronic spin rather than electronic charge, have the potential to enable more energy-efficient and higher performance devices. These spintronic devices require materials capable of efficiently harnessing the electron spin. Here we show robust spin transport in Cd3As2 films up to room temperature. We demonstrate a nonlocal spin valve switch from this material, as well as inverse spin Hall effect measurements yielding spin Hall angles as high as θSH = 1.5 and spin diffusion lengths of 10-40 μm. Long spin-coherence lengths with efficient charge-to-spin conversion rates and coherent spin transport up to room temperature, as we show here in Cd3As2, are enabling steps toward realizing actual spintronic devices.

Morphology and Optical Properties of Thin Cd3As2 Films of a Dirac Semimetal Compound

Using atomic-force microscopy (AFM) and wide-band (0.02–8.5 eV) spectroscopic ellipsometry techniques, we investigated the morphology and optical properties of Cd3As2 films grown by non-reactive RF magnetron sputtering on two types of oriented crystalline substrates (100)p-Si and (001) α-Al2O3. The AFM study revealed the grainy morphology of the films due to island incorporation during the film growth. The complex dielectric function spectra of the annealed Cd3As2/Al2O3 films manifest pronounced interband optical transitions at 1.2 and 3.0 eV, in excellent agreement with the theoretical calculations for the body centered tetragonal Cd3As2 crystal structure. We discovered that due to electronic excitations to the Cd(s) conical bands, the low-energy absorption edge of the annealed Cd3As2 films reveals a linear dependence. We found that for the annealed Cd3As2 films, the Cd(s) conical node may be shifted in energy by about 0.08–0.18 eV above the heavy-flat As(p) valence band, determining the optical gap value. The as-grown Cd3As2 films exhibit the pronounced changes of the electronic band structure due to the doping effect associated with Cd non-stoichiometry, where fine-tuning of the Cd concentration may result in the gapless electronic band structure of Dirac semimetals.

Effect of Cd/As flux ratio and annealing process on the transport properties of Cd3As2 films grown by molecular beam epitaxy

To study how the Cd/As flux ratio affects the microstructure and transport properties for Cd3As2 films, we used molecular beam epitaxy (MBE) to grow Cd3As2 (224) thin films on CdTe (111)/GaAs (001) virtual substrates. The effects of Cd/As flux ratio, during the grown process, on the electrical properties and surface morphology of the sample was studied. The films grown at lower Cd/As flux ratio have higher electron mobility and longer effective dephasing length. With decreasing Cd/As flux ratio, the magnetoresistance (MR) of the film changes from negative to positive. These results show that a lower beam ratio is beneficial to improve the crystal quality. In order to optimize the electrical properties of the films, the effect of annealing on the electron mobility and MR have been studied. After annealing, the MR changes from negative to positive, the electron mobility increase by 8 times, and the MR increase from 15% to 360% at 9 T. These results indicate that annealing is an effective method to optimize the electrical properties of Cd3As2 epitaxial films.

Third harmonic generation in Dirac semimetal Cd3As2

Cadmium arsenide (Cd3As2), an emerging three-dimensional Dirac semimetal, has recently generated significant interest in the area of ultrafast optics and optoelectronics. However, its nonlinear susceptibility has not been experimentally studied; thus, it is not yet possible to evaluate its potential in nonlinear optics. In this work, we investigate third harmonic generation (THG) in a 100 nm thick Cd3As2 film using broadband infrared femtosecond lasers (across 1500–2350 nm). The χ3 of Cd3As2 (2.30 × 10−19 m2 V−2) is obtained by comparing the THG spectra with a glass substrate, graphene, and monolayer MoS2. We further demonstrate a simple approach to enhance the THG signal by introducing an underlying planar micro-cavity. An enhancement of about 420 times in the THG signal was recorded at ≃1560 nm. Our results indicate that Cd3As2 thin films can provide a similar platform for nonlinear optics with respect to graphene and may offer unique potential in the mid-infrared due to its broadband light–matter interaction and excellent tunability.

Mn doping effects on the gate-tunable transport properties of Cd3As2 films epitaxied on GaAs

The Mn doping effects on the gate-tunable transport properties of topological Dirac semimetal Cd3As2 films have been investigated. Mn-doped Cd3As2 films are directly grown on GaAs(111)B substrates by molecular-beam epitaxy, during which the single crystal phase can be obtained with Mn concentration less than 2%. Shubnikov-de Haas oscillation and quantum Hall effect are observed at low temperatures, and electrons are found to be the dominant carrier in the whole temperature range. Higher Mn content results in smaller lattice constant, lower electron mobility and larger effective band gap, while the carrier density seems to be unaffected by Mn-doping. Gating experiments show that Shubnikov-de Haas oscillation and quantum Hall effect are slightly modulated by electric field, which can be explained by the variation of electron density. Our results provide useful information for understanding the magnetic element doping effects on the transport properties of Cd3As2 films.

Carrier mobilities of (001) cadmium arsenide films

We investigate (001)-oriented films of the topological semimetal cadmium arsenide (Cd3As2) grown by molecular beam epitaxy on lattice-matched III–V AlxIn1−xSb buffer layers. Magnetotransport studies and analysis of thin film microstructures are used to determine the influence of dislocations on their carrier mobilities. We show that only a minority of the threading dislocations present in the buffer layers extend into the Cd3As2 films. Threading dislocations are shown to reduce the mobilities of carriers residing in the topological surface states, while bulk transport was unaffected by a change in the dislocation density across an order of magnitude. Thick (001) Cd3As2 films exhibit electron mobilities of up to 41 000 cm2 V−1 s−1 at 2 K. The results provide insights into the influence of extended defects on the transport properties of a prototype topological semimetal.

Superconductivity and Shubnikov - de Haas effect in polycrystalline Cd3As2 thin films

In this study we observed the reproducible superconducting state in Cd3As2 thin films without any external stimuli. Comparison with our previous results reveals similar qualitative behavior for films synthesized by different methods, while the difference in the values of the critical parameters clearly shows the possibility to control this state. The X-ray diffraction measurements demonstrate the presence of the tetragonal Cd3As2 crystal phase in studied films. Measurements of high-field magnetoresistance reveal pronounced Shubnikov - de Haas oscillations. The analysis of these oscillations suggests that, due to high carrier concentration in studied Cd3As2 films, the initial Dirac semimetal phase may be partially suppressed, which, however, does not contradict with possible topological nature of the observed superconductivity.

Superconductivity in Thin Films of the Dirac Semimetal Cd3As2

Thin films of Dirac semimetal Cd3As2 about 100 nm thick made of single crystals of cadmium arsenide, prepared by direct fusion of the elements by vacuum–ampoule method, by vacuum–thermal sputtering/depostion have been studied. Temperature and magnetic field dependences of electrical resistance have been measured, which indicate the presence of a superconducting transition at a temperature from 0.2 to 0.6 K.

Hopping Conductivity Mechanism in Cd3As2 Films Prepared by Magnetron Sputtering

Hopping Conductivity Mechanism in Cd3As2 Films Prepared by Magnetron Sputtering

Molecular beam epitaxy of three-dimensionally thick Dirac semimetal Cd3As2 films

Rapid progress of quantum transport study in topological Dirac semimetal, including observations of quantum Hall effect in two-dimensional (2D) Cd3As2 samples, has uncovered even more interesting quantum transport properties in high-quality and three-dimensional (3D) samples. However, such 3D Cd3As2 films with low carrier density and high electron mobility have been hardly obtained. Here, we report the growth and characterization of 3D thick Cd3As2 films adopting molecular beam epitaxy. The highest electron mobility (μ = 3 × 104 cm2/Vs) among the reported film samples has been achieved at a low carrier density (n = 5 × 1016 cm−3). In the magnetotransport measurement, Hall plateau-like structures are commonly observed despite the 3D thick films (t = 120 nm). On the other hand, the field angle dependence of the plateau-like structures and corresponding Shubunikov-de Haas oscillations rather shows a 3D feature, suggesting the appearance of an unconventional magnetic orbit, also distinct from the one described by the semiclassical Weyl-orbit equation.