Topological Insulator Bi2Se3 Thin Films Research Articles

Ion-Induced Lateral Damage in the Focused Ion Beam Patterning of Topological Insulator Bi2Se3 Thin Films

Focused Ion Beam patterning has become a widely applied technique in the last few decades in the micro- and nanofabrication of quantum materials, representing an important advantage in terms of resolution and versatility. However, ion irradiation can trigger undesired effects on the target material, most of them related to the damage created by the impinging ions that can severely affect the crystallinity of the sample, compromising the application of Focused Ion Beam to the fabrication of micro- and nanosized systems. We focus here on the case of Bi2Se3, a topological material whose unique properties rely on its crystallinity. In order to study the effects of ion irradiation on the structure of Bi2Se3, we irradiated with Ga+ ions the full width of Hall-bar devices made from thin films of this material, with the purpose of inducing changes in the electrical resistance and characterizing the damage created during the process. The results indicate that a relatively high ion dose is necessary to introduce significant changes in the conduction. This ion dose creates medium-range lateral damage in the structure, manifested through the formation of an amorphous region that can extend laterally up to few hundreds of nanometers beyond the irradiated area. This amorphous material is no longer expected to behave as intrinsic Bi2Se3, indicating a spatial limitation for the devices fabricated through this technique.

Signature of weak-antilocalization in sputtered topological insulator Bi2Se3 thin films with varying thickness

We report a low-temperature magneto transport study of Bi2Se3 thin films of different thicknesses (40, 80 and 160 nm), deposited on sapphire (0001) substrates, using radio frequency magnetron sputtering technique. The high-resolution x-ray diffraction measurements revealed the growth of rhombohedral c-axis {0003n} oriented Bi2Se3 films on sapphire (0001). Vibrational modes of Bi2Se3 thin films were obtained in the low wavenumber region using Raman spectroscopy. The surface roughness of sputtered Bi2Se3 thin films on sapphire (0001) substrates were obtained to be ~ 2.26–6.45 nm. The chemical and electronic state of the deposited Bi2Se3 was confirmed by X-ray photoelectron spectroscopy and it showed the formation of Bi2Se3 compound. Resistivity versus temperature measurements show the metallic nature of Bi2Se3 films and a slight up-turn transition in resistivity at lower temperatures < 25 K. The positive magneto-resistance value of Bi2Se3 films measured at low temperatures (2–100 K) confirmed the gapless topological surface states in Bi2Se3 thin films. The quantum correction to the magnetoconductivity of thin films in low magnetic field is done by employing Hikami–Larkin–Nagaoka theory and the calculated value of coefficient ‘α’ (defining number of conduction channels) was found to be 0.65, 0.83 and 1.56 for film thickness of 40, 80 and 160 nm, respectively. These observations indicate that the top and bottom surface states are coupled with the bulk states and the conduction mechanism in Bi2Se3 thin films varied with the film thicknesses.

Proximity-Induced Magnetism in a Topological Insulator/Half-Metallic Ferromagnetic Thin Film Heterostructure

Topological insulator (TI) Bi2Se3 thin films were prepared on half-metallic ferromagnetic La0.7Sr0.3MnO3 thin film by magnetron sputtering, forming a TI/FM heterostructure. The conductivity of Bi2Se3was modified by La0.7Sr0.3MnO3 at high- and low-temperature regions via different mechanisms, which could be explained by the short-range interactions and long-range interaction between ferromagnetic insulator and Bi2Se3 due to the proximity effect. Magnetic and transport measurements prove that the ferromagnetic phase and extra magnetic moment are induced in Bi2Se3 films. The weak anti-localized (WAL) effect was suppressed in Bi2Se3 films, accounting for the magnetism of La0.7Sr0.3MnO3 layers. This work clarifies the special behavior in Bi2Se3/La0.7Sr0.3MnO3 heterojunctions, which provides an effective way to study the magnetic proximity effect of the ferromagnetic phase in topological insulators.

Quantum interference phenomena and electron – electron interaction in topological insulator Bi2Se3 thin polycrystalline films

The temperature (T = 2.0 - 300 K) and magnetic field (B = 0 - 14 T) dependences of the transport coefficients were obtained for the topological insulator (TI) polycrystalline Bi2Se3 films with thicknesses d = 40 and 200 nm grown on glass substrates by thermal evaporation in vacuum from a single source. In the region of weak magnetic fields, a sharp increase in magnetoresistance (MR) with increasing B was observed, indicating the presence of the weak antilocalization (WAL) effect, which is typical for 3D-TIs. However, the longitudinal resistance Rxx increases logarithmically with decreasing temperature below certain temperature Tc, which is not characteristic of the WAL effect in 2D-structures and indicates possible existence of the so-called “transport paradox”. In the temperature dependences of the Hall resistance, Hall coefficient and MR we also registered clearly pronounced kinks near Tc. The Rxx(T) dependence for a 40 nm film, with decreasing temperature in addition to the Rxx minimum near Tc, exhibits a maximum near 2.1 K. Estimates of the number of independent transport channels m and the dephasing length lφ show that as d increases from 40 nm to 200 nm, m increases from 1 to 3, while lφ changes insignificantly. The nonmonotonic behavior of the T- and B- dependences of the kinetic coefficients, the occurrence of the “transport paradox” are associated with a change in the contributions of WAL and electron-electron interaction effects when the nature and magnitude of the external influence and film thickness change. It follows from the data obtained that not only in very thin monocrystalline films, but also in rather thick polycrystalline Bi2Se3 films prepared by the simple method of the thermal evaporation in vacuum on amorphous substrates, quantum interference effects and “transport paradox” can be manifested.

Scalable fabrication of Bi2O2Se polycrystalline thin film for near-infrared optoelectronic devices applications* *Project supported by the Hunan Provincial Natural Science Foundation of China (Grant No. 2019JJ40032).

We present a controlled, stepwise formation of layered semiconductor Bi2O2Se thin films prepared via the vapour process by annealing topological insulator Bi2Se3 thin films in low oxygen atmosphere for different reactions. Photodetectors based on Bi2O2Se thin film show a responsivity of 1.7 × 104 A/W at a wavelength of 980 nm. Field-effect transistors based on Bi2O2Se thin film exhibit n-type behavior and present a high electron mobility of 17 cm2/V⋅s. In addition, the electrical properties of the devices after 4 months keeping in the air shows little change, implying outstanding air-stability of our Bi2O2Se thin films. From the obtained results, it is evident that low oxygen annealing is a surprisingly effective method to fabricate Bi2O2Se thin films for integrated optoelectronic applications.

Size effect in the kinetic properties in “sized” films of Bi2Se3 topological insulator

The Hall resistivity and magnetoresistivity of topological insulator Bi2Se3 thin films with a thickness from 30 nm to 75 nm in the temperature range from 4.2 to 80 K and magnetic fields of up to 10 T were measured. A size effect in the kinetic properties of bismuth selenide films was studied, i.e. a dependence of the Hall coefficient and magnetoconductivity of film dimensions. It was suggested that a similar size effect should be observed in other kinetic electronic properties, both of topological insulators and topological semimetals.

Anomalous Temperature Dependence of Quantum Correction to the Conductivity of Magnetic Topological Insulators.

Quantum transport in magnetic topological insulators reveals a strong interplay between magnetism and topology of electronic band structures. A recent experiment on magnetically doped topological insulator Bi_{2}Se_{3} thin films showed the anomalous temperature dependence of the magnetoconductivity while their field dependence presents a clear signature of weak antilocalization [Tkac etal., Phys. Rev. Lett. 123, 036406 (2019)PRLTAO0031-900710.1103/PhysRevLett.123.036406]. Here, we demonstrate that the tiny mass of the surface electrons induced by the bulk magnetization leads to a temperature-dependent correction to the π Berry phase and generates a decoherence mechanism to the phase coherence length of the surface electrons. As a consequence, the quantum correction to conductivity can exhibit nonmonotonic behavior by decreasing the temperature. This effect is attributed to the close relation of the Berry phase and quantum interference of the topological surface electrons in quantum topological materials.

Layer-dependent dielectric permittivity of topological insulator Bi2Se3 thin films

Dielectric properties and their evolutions are fundamental to reveal the optical responses of topological insulators and to guide the design of related devices. Here, we systematically investigate the layer-dependent dielectric permittivity of Bi2Se3 over an ultra-broad spectral range (0.73–6.43 eV) by combining the spectroscopic ellipsometry, energy-loss function (ELF), critical point (CP) analysis, and density function theory. Results demonstrate that the epsilon-near-zero point of the real permittivity and the ELF peak exhibit blue shifts, indicating the resonance frequencies of surface plasmon modes move towards the higher energy, due to the enhanced hybridization between the opposite surfaces. The joint density of states dominates the layer-dependent increase in imaginary permittivity as the thickness increases. We also find that the CP transition positions in band structures are layer-independent, and the CP center energies exhibit red shifts resulted by the reduced surface state gap with the thickness increasing.

First principles study of semihydrogenated graphene and topological insulator heterojunction

Based on first principles calculations, we study the electronic properties of heterostructures formed by a 2D ferromagnetic insulator semihydrogenated graphene (SG) and topological insulator Bi2Se3 thin films of a few quintuple layers (QLs). It is found that the unsaturated C atoms in SG form bonds with Se atoms in Bi2Se3 thin film and the top surface states (at the interface) are strongly hybridized with SG. Due to breaking of time-reversal symmetry, the surface states open gaps of 40 meV and 150 meV for SG/3QL-Bi2Se3 and SG/5QL-Bi2Se3 heterostructures, respectively. Furthermore, a giant Rashba spin splitting is found induced by the SG layer.

Electron–phonon coupling in topological insulator Bi2Se3 thin films with different substrates

Broadband transient reflectivity traces were measured for Bi2Se3 thin films with various substrates via a 400 nm pump–white-light-probe setup. We have verified the existence of a second Dirac surface state in Bi2Se3 and qualitatively located it by properly analyzing the traces acquired at different probe wavelengths. Referring to the band structure of Bi2Se3, the relaxation mechanisms for photo-excited electrons with different energies are also revealed and studied. Our results show a second rise of the transient reflection signal at the time scale of several picoseconds. The types of substrate can also significantly affect the dynamics of the rising signal. This phenomenon is attributed to the effect of lattice heating and coherent phonon processes. The mechanism study in this work will benefit the fabrication of high-performance photonic devices based on topological insulators.

Robustness of topological states in Bi2Se3 thin film grown by Pulsed Laser Deposition on (0 0 1)-oriented SrTiO3 perovskite

We report on the reproducible surface topological electron states in Bi2Se3 topological insulator thin films when epitaxially grown by Pulsed Laser Deposition (PLD) on (001)-oriented SrTiO3 (STO) perovskite substrates. Bi2Se3 has been reproducibly grown with single (001)-orientation and low surface roughness as controlled by ex-situ X-ray diffraction and in situ scanning tunnel microscopy and low-energy electron diffraction. Finally, in situ synchrotron radiation angle-resolved photo-emission spectroscopy measurements show a single Dirac cone and Dirac point at EB∼0.38 eV located in the center of the Brillouin zone likewise found from exfoliated single-crystals. These results demonstrate that the topological surface electron properties of PLD-grown Bi2Se3 thin films grown on (001)-oriented STO substrates open new perspectives for applications of multi-layered materials based on oxide perovskites.

Bulk transport properties of bismuth selenide thin films grown by magnetron sputtering approaching the two-dimensional limit

Transport properties of topological insulator Bi2Se3 thin films are investigated with an emphasis on understanding finite-size effects as the two-dimensional limit is approached. Ultra-smooth, (000l)-orientated Bi2Se3 thin-films fabricated using radio-frequency magnetron sputtering reveal disproportionately large changes in bulk resistivity and Hall mobility below six quintuple layers (QL). We correlate such changes to the bulk (other than surface) electronic structure where a bandgap enlargement is observed below six QL in optical absorption spectroscopy measurements. This effect is strongest at the three and two quintuple layers that show the largest changes in bandgap. Temperature dependent transport measurements reveal the effect of disorder from substrate and high carrier concentration. Films on sapphire substrate demonstrate better transport properties compared to amorphous quartz. While temperature dependence of bulk resistivity is both thickness and substrate sensitive, the temperature dependence of Hall coefficient is determined only by the carrier concentration in films. Our work highlights the influence of the bulk electronic structure on the transport properties of few-layer Bi2Se3 which is of interest in the applied areas of optoelectronics, nanoelectronics, and spintronics.

Magnetotransport in antidot arrays of three-dimensional topological insulators

Three-dimensional topological insulators are a new kind of quantum matter featured with gapless Dirac-like energy-dispersive surface states in the insulating bulk band gaps. However, in experiment, it is difficult to study quantum interference effect of surface states due to considerable contribution from bulk carriers in thick bulk material. To suppress such a bulk state contribution, nanostructures, such as ultra-thin films, nanowires and nanoribbons, have been employed in the study of quantum interference effects of the surface states. Here, we report on a magnetotransport measurement study of nanoscaled antidot array devices made from three-dimensional topological insulator Bi2Se3 thin films. The antidot arrays with hundreds of nanometers in diameter and edge-to-edge distance are fabricated in the thin films by utilizing the focused-ion beam technique, and the magnetotransport properties of the fabricated devices are measured at low temperatures. The results of the magnetotransport measurements for three representative devices, denoted as Dev-1 (with no antidot array fabricated), Dev-2 (with an antidot array of a relatively large period), and Dev-3 (with an antidot array of a relatively small period), are reported in this work. Weak anti-localization indicated by a sharp peak of conductivity at zero magnetic field is observed in all the three devices. Through theoretical fitting to the measurement data, the transport parameters in the three devices, such as spin-orbit coupling length Lso, phase coherence length L, and the number of conduction channels , are extracted. The extracted Lso value is tens of nanometers, which is consistent with the presence of the strong spin-orbit interaction in the Bi2Se3 thin film. The extracted L value is hundreds of nanometers and increases exponentially with temperature decreasing. It is found that the magnetotransports in Dev-1 and Dev-2 are well characterized by the coherent transport through a single conduction channel. For Dev-3, the magnetotransport at low temperatures is described by the coherent transport through two independent conduction channels, while at elevated temperatures the magnetotransport is dominantly described by the transport through one single conduction channel. Unlike the case where the transport occurs dominantly through a single conduction channel, the transport through two independent conduction channels in Dev-3 implies that at least one surface channel is present in the device.

Disorder-dominated linear magnetoresistance in topological insulator Bi2Se3 thin films

The linear magnetoresistance (MR) effect is an interesting topic due to its potential applications. In topological insulator Bi2Se3, this effect has been reported to be dominated by the carrier mobility (μ) and hence has a classical origin. Here, we study the magnetotransport properties of Bi2Se3 thin films and observe the linear MR effect, which cannot be attributed to the quantum model. Unexpectedly, the linear MR does not show the linear dependence on μ, in conflict with the reported results. However, we find that the observed linear MR is dominated by the inverse disorder parameter 1/kFl, where kF and l are the Fermi wave vector and the mean free path, respectively. This suggests that its origin is also classical and that no μ-dominated linear MR effect is observed which may be due to the very small μ values in our samples.

Van der Waals epitaxy of topological insulator Bi2Se3 on single layer transition metal dichalcogenide MoS2

We report the growth of high quality topological insulator Bi2Se3 thin films on a single layer, transitional metal dichalcogenide MoS2 film via van der Waals epitaxy in a planar geometry. In stark contrast to the reported growth of using 3-D crystalline substrates such as Al2O3(0001), Bi2Se3 thin films grown on a 2-D template made of single layer MoS2 showed excellent crystallinity starting immediately from the growth of the first quintuple layer. Excellent crystallinity of Bi2Se3 thin films is attained, with the increased size of the triangular shaped Bi2Se3 domains and 2–3 times enhancement in mobility, along with the observation of Shubnikov–de Haas oscillations in the magnetoresistance. Our approach of adopting a van der Waals type template may be extended to the thin film growth of other low dimensional layered materials.

Proximity-effect-induced Superconducting Gap in Topological Surface States \u2013 A Point Contact Spectroscopy Study of NbSe2/Bi2Se3 Superconductor-Topological Insulator Heterostructures

Proximity-effect-induced superconductivity was studied in epitaxial topological insulator Bi2Se3 thin films grown on superconducting NbSe2 single crystals. A point contact spectroscopy (PCS) method was used at low temperatures down to 40 mK. An induced superconducting gap in Bi2Se3 was observed in the spectra, which decreased with increasing Bi2Se3 layer thickness, consistent with the proximity effect in the bulk states of Bi2Se3 induced by NbSe2. At very low temperatures, an extra point contact feature which may correspond to a second energy gap appeared in the spectrum. For a 16 quintuple layer Bi2Se3 on NbSe2 sample, the bulk state gap value near the top surface is ~159 μeV, while the second gap value is ~120 μeV at 40 mK. The second gap value decreased with increasing Bi2Se3 layer thickness, but the ratio between the second gap and the bulk state gap remained about the same for different Bi2Se3 thicknesses. It is plausible that this is due to superconductivity in Bi2Se3 topological surface states induced through the bulk states. The two induced gaps in the PCS measurement are consistent with the three-dimensional bulk state and the two-dimensional surface state superconducting gaps observed in the angle-resolved photoemission spectroscopy (ARPES) measurement.

Optical evidence for blue shift in topological insulator bismuth selenide in the few-layer limit

Optical bandgap properties of high-quality few-layer topological insulator Bi2Se3 thin films are investigated using broadband absorption spectroscopy. We provide direct optical evidence for blue shift in the bulk bandgap of Bi2Se3 as it approaches the two-dimensional limit. The blue shift is robust and observed in both protected (capped) and exposed (uncapped) thin films. The behavior is strongest below six quintuple layers (QLs), particularly at the 2 and 3 QL level, where finite-size effects are known to be most significant in Bi2Se3. A further bandgap increase is observed in all films that we attribute to the Burstein-Moss effect. Our result provides additional insights into the scaling behavior of topological materials. The bandgap increase has a significant impact on the electronic and optoelectronic applications of topological insulators.

Structural and electronic properties of Bi2Se3 topological insulator thin films grown by pulsed laser deposition

We report on epitaxial growth of Bi2Se3 topological insulator thin films by Pulsed Laser Deposition (PLD). X-ray diffraction investigation confirms that Bi2Se3 with a single (001)-orientation can be obtained on several substrates in a narrow (i.e., 20 °C) range of deposition temperatures and at high deposition pressure (i.e., 0.1 mbar). However, only films grown on (001)-Al2O3 substrates show an almost-unique in-plane orientation. In-situ spin-resolved angular resolved photoemission spectroscopy experiments, performed at the NFFA-APE facility of IOM-CNR and Elettra (Trieste), show a single Dirac cone with the Dirac point at EB∼0.38 eV located in the center of the Brillouin zone and the spin polarization of the topological surface states. These results demonstrate that the topological surface state can be obtained in PLD-grown Bi2Se3 thin films.

Properties of topological insulator Bi2Se3 films prepared by thermal evaporation growth on different substrates

Topological insulator Bi2Se3 thin films were grown by the thermal evaporation deposition on different substrates and their phase structures and magneto-transport properties were discussed. The films growth is along the c-axis, and their surfaces exhibited terrace-like quintuple layers. Resistivity upturn as well as weak anti-localization was observed only in the film with Si and LAO substrates. The linear magneto-resistance (LMR) under high field was found, which was associated with the gapless topological surface states and the quantum origin. The results indicate that the films are highly uniform.

Molecular beam epitaxial growth and electronic transport properties of high quality topological insulator Bi2Se3 thin films on hexagonal boron nitride

We report the molecular beam epitaxial growth and characterization of high quality topological insulator Bi2Se3 thin films on hexagonal boron nitride (h-BN). A two-step growth was developed, enhancing both the surface coverage and crystallinity of the films on h-BN. High-resolution transmission electron microscopy study showed an atomically abrupt and epitaxial interface formation between the h-BN substrate and Bi2Se3. We performed gate tuned magnetotransport characterizations of the device fabricated on the thin film and confirmed a high mobility surface state at the Bi2Se3/h-BN interface. The Berry phase obtained from Shubnikov−de Haas oscillations suggested this interfacial electronic state is a topologically protected Dirac state.