High-quality Epitaxial Growth Research Articles

Epitaxial Thin Film Growth on Recycled SrTiO3 Substrates Toward Sustainable Processing of Complex Oxides.

Complex oxide thin films cover a range of physical properties and multifunctionalities that are critical for logic, memory, and optical devices. Typically, the high-quality epitaxial growth of these complex oxide thin films requires single crystalline oxide substrates such as SrTiO3 (STO), MgO, LaAlO3, a-Al2O3, and many others. Recent successes in transferring these complex oxides as free-standing films not only offer great opportunities in integrating complex oxides on other devices, but also present enormous opportunities in recycling the deposited substrates after transfer for cost-effective and sustainable processing of complex oxide thin films. In this work, the surface modification effects introduced on the recycled STO are investigated, and their impacts on the microstructure and properties of subsequently grown epitaxial oxide thin films are assessed and compared with those grown on the pristine substrates. Detailed analyses using high-resolution scanning transmission electron microscopy and geometric phase analysis demonstrate distinct strain states on the surfaces of the recycled STO versus the pristine substrates, suggesting a pre-strain state in the recycled STO substrates due to the previous deposition layer. These findings offer opportunities in growing highly mismatched oxide films on the recycled STO substrates with enhanced physical properties. Specifically, yttrium iron garnet (Y3Fe5O12) films grown on recycled STO present different ferromagnetic responses compared to that on the pristine substrates, underscoring the effects of surface modification. The study demonstrates the feasibility of reuse and redeposition using recycled substrates. Via careful handling and preparation, high-quality epitaxial thin films can be grown on recycled substrates with comparable or even better structural and physical properties toward sustainable process of complex oxide devices.

Ultra-High-k Ferroelectric BaTiO3 Perovskite in the Gate Stack for Two-Dimensional WSe2 p-Type High-Performance Transistors.

The experimental demonstration of a p-type 2D WSe2 transistor with a ferroelectric perovskite BaTiO3 gate oxide is presented. The 30 nm thick BaTiO3 gate stack shows a robust ferroelectric hysteresis with a remanent polarization of 20 μC/cm2 and further enables a capacitance equivalent thickness of 0.5 nm in the hybrid WSe2/BaTiO3 stack due to its high dielectric constant of 323. We demonstrate one of the best ON currents for perovskite gate 2D transistors in the literature. This is enabled by high-quality epitaxial growth of BaTiO3 and a single 2D layer transfer based fabrication method that is shown to be amenable to silicon platforms. This demonstration is an important milestone toward the integration of crystalline complex oxides with 2D channel materials for scaled CMOS and low-voltage ferroelectric logic applications.

Oxygen-close-packed (310)-plane substrates of β-Ga2O3 grown by the casting method

The highly anisotropic crystal structure of β-Ga2O3 gives rise to a variety of crystal planes, among which the (310) plane is a potentially stable close-packed plane for the O sublattice. In this paper, we report the β-Ga2O3 single crystal and substrates with a (310) major plane grown by the spontaneous nucleation technique in the casting method. High-quality crystal growth and substrate processing were confirmed by the 25.67 arc sec full width at half maximum and the 0.25 nm surface roughness. The nanoindentation experiments revealed the (310) substrate's better elastic recovery than that of (100) substrate. The Young's modulus and hardness of (310) substrates were 200 and 7.6 GPa, respectively. The surface barrier height and the Schottky barrier height were 1.25 and 0.92 eV, respectively. First principles calculations identified the (310)-Ga-I plane as the most stable surface configuration of the (310) plane under oxygen-poor condition, with a surface energy density of 1.48 J/m2. The (310) twin boundary formation around the O sublattice has a high energy density of 0.55 J/m2, suggesting its unlikelihood of spontaneous formation. These properties of (310) plane facilitate a high-quality crystal processing and epitaxial growth, thus endowing potential applications in high-quality power devices. Furthermore, the growth and fabrication of the (310) plane provide a route toward understanding the properties of β-Ga2O3 and advancing the growth techniques of oxide crystals.

Advanced Mechanical Transfer of Micro-LEDs Enabled by Structurally Modified Wide Sapphire Nanomembranes through Thermal Reflow of Photoresist.

Micro light-emitting diodes (micro-LEDs) are pivotal in next-generation display technologies, driven by the need for high pixel density. This study introduces a novel methodology utilizing wide sapphire nanomembranes (W-SNM) as a dual-purpose template for high-quality epitaxial growth and the mechanical lift-off of individual micro-LEDs. Micro-LEDs grow individually on W-SNM, obviating the chip singulation process. By employing mechanical fracturing of the thin W-SNM, our method facilitates the transfer of micro-LEDs without the conventional laser lift-off (LLO) process. Previously introduced sapphire nanomembranes (SNM) have shown promise in enhancing epitaxial layer quality; however, they encountered challenges in managing micro-LED size variation and achieving efficient mechanical transfer. Here, we apply simple yet effective adjustments to the SNM structure, specifically, its elevation and widening. This strategic modification allows micro-LEDs to endure applied forces without incurring cracks or defects, ensuring that only the targeted W-SNM are selectively fractured. The mechanically transferred vertical 15 × 15 μm2 micro-LED device operates at an optimal turn-on voltage of 3.3 V. Finite element simulations validate the mechanical strain distribution between the W-SNM and GaN when pressure is applied, confirming the efficacy of our design approach. This pioneering methodology offers a streamlined, efficient pathway for the production and mechanical transfer of micro-LEDs, presenting new avenues for their integration into next-generation, high-performance displays.

Structural and interface band alignment properties of transparent p-type α-GaCrO3:Ni/α-Al2O3 heterojunction

Herein, we report epitaxial growth of p-type Ni doped gallium chromium oxide thin film on Al2O3 substrates and studied its band alignment properties with that of the substrate. Thin films are grown using the magnetron-sputtering technique. Synchrotron-based XRD measurements, performed in the coplanar and non-coplanar geometries, confirm high-quality single domain epitaxial growth of p-type α-GaCrO3:Ni. Pendellosung oscillations around the Bragg peak and transmission electron microscopy reveal the high interfacial quality of p-type α-GaCrO3:Ni films with the substrate. Thin film, thickness ∼200 nm, shows around 70% average transmission. The values of valence band and conduction band offsets are determined to be 2.79 ± 0.2 and 0.51 ± 0.2 eV, respectively, which confirm straddling gap band alignment at the heterojunction. This type of alignment creates a threshold barrier for the selective charge carriers and is useful in enhancing the performance of a wide range of devices, including UV photodetectors, metal oxide semiconductor high electron mobility transistors, and light emitters.

Current-Induced Magnetization Switching Behavior in Perpendicular Magnetized L10-MnAl/B2-CoGa Bilayer

Rare-earth-free Mn-based binary alloy L10-MnAl with bulk perpendicular magnetic anisotropy (PMA) holds promise for high-performance magnetic random access memory (MRAM) devices driven by spin-orbit torque (SOT). However, the lattice-mismatch issue makes it challenging to place conventional spin current sources, such as heavy metals, between L10-MnAl layers and substrates. In this work, we propose a solution by using the B2-CoGa alloy as the spin current source. The lattice-matching enables high-quality epitaxial growth of 2-nm-thick L10-MnAl on B2-CoGa, and the L10-MnAl exhibits a large PMA constant of 1.04 × 106 J/m3. Subsequently, the considerable spin Hall effect in B2-CoGa enables the achievement of SOT-induced deterministic magnetization switching. Moreover, we quantitatively determine the SOT efficiency in the bilayer. Furthermore, we design an L10-MnAl/B2-CoGa/Co2MnGa structure to achieve field-free magnetic switching. Our results provide valuable insights for achieving high-performance SOT-MRAM devices based on L10-MnAl alloy.

Progress in Gallium Oxide Field-Effect Transistors for High-Power and RF Applications.

Power electronics are becoming increasingly more important, as electrical energy constitutes 40% of the total primary energy usage in the USA and is expected to grow rapidly with the emergence of electric vehicles, renewable energy generation, and energy storage. New materials that are better suited for high-power applications are needed as the Si material limit is reached. Beta-phase gallium oxide (β-Ga2O3) is a promising ultra-wide-bandgap (UWBG) semiconductor for high-power and RF electronics due to its bandgap of 4.9 eV, large theoretical breakdown electric field of 8 MV cm-1, and Baliga figure of merit of 3300, 3-10 times larger than that of SiC and GaN. Moreover, β-Ga2O3 is the only WBG material that can be grown from melt, making large, high-quality, dopable substrates at low costs feasible. Significant efforts in the high-quality epitaxial growth of β-Ga2O3 and β-(AlxGa1-x)2O3 heterostructures has led to high-performance devices for high-power and RF applications. In this report, we provide a comprehensive summary of the progress in β-Ga2O3 field-effect transistors (FETs) including a variety of transistor designs, channel materials, ohmic contact formations and improvements, gate dielectrics, and fabrication processes. Additionally, novel structures proposed through simulations and not yet realized in β-Ga2O3 are presented. Main issues such as defect characterization methods and relevant material preparation, thermal studies and management, and the lack of p-type doping with investigated alternatives are also discussed. Finally, major strategies and outlooks for commercial use will be outlined.

A 1083 nm Narrow-Linewidth DFB Semiconductor Laser for Quantum Magnetometry

A 1083 nm laser, corresponding to a characteristic spectral line of 3He 23S1-23P, is the core light source for spin-exchange optical pumping-free technology, and thus has important developmental significance. In this paper, precise wavelength 1083.34 nm semiconductor lasers with 285 mW output power, −144.73 dBc/Hz RIN noise and 30.9952 kHz linewidth have been successfully achieved via reasonable chips design, high-quality epitaxial growth process and ultra-low reflectivity coating fabrication. All the results show the highest output power and ultra-narrow linewidth of the single-frequency 1083 nm DFB semiconductor laser achieved in this paper, which can fully satisfy the requirement of quantum magnetometers.

Theoretical adjustment of metalorganic chemical vapor deposition process parameters for high-quality gallium nitride epitaxial films

Semiconductor thin films for electronic devices are usually produced through processes such as chemical vapor deposition, which requires careful control of the gas flow, heat distribution, and concentration distribution over the substrate to ensure a uniform deposition rate and thickness. Herein, a systematic method is proposed for the theoretical adjustment of metalorganic chemical vapor deposition (MOCVD) process parameters. To this end, a GaN-MOCVD reactor with a vertical injection structure was simulated based on computational fluid dynamics to analyze the stable flow under a fixed flow rate. The orthogonal experimental design was used to analyze the influence of process conditions on film quality. A neural network and genetic algorithm were used to optimize the inlet flow under the stable flow state to render the coefficient of variation <3%. Under these conditions, the flow field in the reactor was stabilized to ensure a uniform thickness for the deposited film. This study provides not only an effective solution for high-quality epitaxial growth but also a theoretical basis for subsequent experiments and equipment improvement.

High Crystallinity Ge Growth on Si (111) and Si (110) by Using Reduced Pressure Chemical Vapor Deposition

A method for high quality epitaxial growth of Ge on Si (111) and Si (110) is investigated by reduced pressure chemical vapor deposition. Two step Ge epitaxy (low temperature Ge seed and high temperature main Ge growth) with several cycles of annealing by interrupting the Ge growth (cyclic annealing) is performed. In the case of Ge seed layer growth below 350 °C for (111) and 400 °C for (110) orientation, huge surface roughening due to too high dislocation density is observed after the following annealing step. For both crystal orientations, a high crystallinity Ge seed layer is realized by combination of 450 °C growth with 800 °C annealing. Once the high-quality Ge seed layer is deposited, high crystal quality Ge can be grown at 600 °C on the seed layer for both crystal orientations. For the 5 μm thick Ge layer deposited with the cyclic annealing process at 800 °C, a Si diffusion length of ∼400 nm from the interface, RMS roughness below 0.5 nm and threading dislocation density of 5 × 106 cm−2 are achieved for both (111) and (110) substrates.

2D materials-assisted heterogeneous integration of semiconductor membranes toward functional devices

Heterogeneous integration techniques allow the coupling of highly lattice-mismatched solid-state membranes, including semiconductors, oxides, and two-dimensional materials, to synergistically fuse the functionalities. The formation of heterostructures generally requires two processes: the combination of crystalline growth and a non-destructive lift-off/transfer process enables the formation of high-quality heterostructures. Although direct atomic interaction between the substrate and the target membrane ensures high-quality growth, the strong atomic bonds at the substrate/epitaxial film interface hinder the non-destructive separation of the target membrane from the substrate. Alternatively, a 2D material-coated compound semiconductor substrate can transfer the weakened (but still effective) surface potential field of the surface through the 2D material, allowing both high-quality epitaxial growth and non-destructive lift-off of the grown film. This Perspective reviews 2D/3D heterogeneous integration techniques, along with applications of III–V compound semiconductors and oxides. The advanced heterogeneous integration methods offer an effective method to produce various freestanding membranes for stackable heterostructures with unique functionalities that can be applied to novel electrical, optoelectronic, neuromorphic, and bioelectronic systems.

High Quality Ge Growth on Si (111) and Si (110) by Using Reduced Pressure Chemical Vapor Deposition

A method for high quality epitaxial growth of Ge on Si (111) and Si (110) is investigated by reduced pressure chemical vapor deposition. Two step Ge epitaxy (low temperature Ge seed and high temperature main Ge growth) with several cycles of annealing by interrupting the Ge growth (cyclic annealing) is performed. In the case of Ge seed layer growth below 350 °C for (111) and 400 °C for (110) orientation, huge surface roughening due to too high dislocation density is observed after the following annealing step. For both crystal orientations, a high crystallinity Ge seed layer is realized by combination of 450 °C growth with 800 °C annealing. Once the high-quality Ge seed layer is deposited, high crystal quality Ge can be grown at 600 °C on the seed layer for both crystal orientations. For the 5 µm thick Ge layer deposited with the cyclic annealing process at 800 °C, a Si diffusion length of ~400 nm from the interface, RMS roughness below 0.5 nm and threading dislocation density of 5×106 cm-2 are achieved for both (111) and (110) substrates.

Molecular beam epitaxy growth of MoTe2 on hexagonal boron nitride

Hexagonal boron nitride has already been proven to serve as a decent substrate for high quality epitaxial growth of several 2D materials, such as graphene, MoSe2, MoS2 or WSe2. Here, we present for the first time the molecular beam epitaxy growth of MoTe2 on atomically smooth hexagonal boron nitride (hBN) substrate. Occurrence of MoTe2 in various crystalline phases such as distorted octahedral 1T’ phase with semimetal properties or hexagonal 2H phase with semiconducting properties opens a possibility of realization of crystal-phase homostructures with tunable properties. Atomic force microscopy studies of MoTe2 grown in a single monolayer regime enable us to observe impact of growth conditions on formation of various structures: flat grains, net of one-dimensional structures, quasi continuous monolayers with bilayer contribution. Comparison of the distribution of the thickness with Poisson distribution shows that tested growth conditions favorite formation of grains with monolayer thickness. The diffusion constant of MoTe2 grown on hBN can reach order of 10−6 cm2/s for typical growth conditions. Raman spectroscopy results suggest a coexistence of various phases with domination of 2H MoTe2 for samples grown at lower temperatures. XPS measurements confirm the stoichiometry of MoTe2.

Band offsets at metalorganic chemical vapor deposited β-(AlxGa1−x)2O3/β-Ga2O3 interfaces—Crystalline orientation dependence

The β-(AlxGa1−x)2O3 alloy represents an emerging ultrawide bandgap semiconductor material for applications in high-power electronics and deep ultraviolet optoelectronics. The recent demonstrations of orientation-dependent epitaxial growth of high quality β-(AlxGa1−x)2O3 films have unlocked prospects for the development of ultrahigh frequency β-(AlxGa1−x)2O3/Ga2O3 based transistors with high-power tolerance. To control the electronic and optical properties of β-(AlxGa1−x)2O3/Ga2O3 heterostructure-based devices, an understanding of the band offsets between β-(AlxGa1−x)2O3 and β-Ga2O3 is crucial. However, there have been no systematic experimental studies on the evolution of the band offsets between differently oriented β-(AlxGa1−x)2O3/Ga2O3 heterointerfaces as a function of Al compositions. This work presents the valence and conduction band offsets at (010) and (2¯01) oriented β-(AlxGa1−x)2O3/Ga2O3 interfaces using x-ray photoelectron spectroscopy. β-(AlxGa1−x)2O3 films with x ≤ 0.35 and x ≤ 0.48 were grown by metalorganic chemical vapor deposition on (010) and (2¯01) oriented β-Ga2O3 substrates, respectively. The determined band offsets reveal the formation of a type-II (staggered) band alignment at (010) oriented β-(AlxGa1−x)2O3/Ga2O3 and a type-I (straddling) heterojunction between (2¯01) β-(AlxGa1−x)2O3 and β-Ga2O3. For both crystalline orientations, the valence and conduction band offsets are found to increase with increasing Al content with a much weaker variation in the valence band offsets as compared to the conduction band offsets. Among different orientations investigated, such as (010), (2¯01), and (100), the largest conduction band offset occurs at a β-(AlxGa1−x)2O3/Ga2O3 interface with (100) orientation, providing opportunities for excellent electron confinement with a high-density two-dimensional electron gas. Results from this study on the tunable and orientation-dependent band offsets with the variation of the Al alloy fraction will provide guidance for the design of heterostructures in future β-(AlxGa1−x)2O3/Ga2O3 based devices.

Process Steps for High Quality Si-Based Epitaxial Growth at Low Temperature via RPCVD.

The key process steps for growing high-quality Si-based epitaxial films via reduced pressure chemical vapor deposition (RPCVD) are investigated herein. The quality of the epitaxial films is largely affected by the following steps in the epitaxy process: ex-situ cleaning, in-situ bake, and loading conditions such as the temperature and gaseous environment. With respect to ex-situ cleaning, dry cleaning is found to be more effective than wet cleaning in 1:200 dilute hydrofluoric acid (DHF), while wet cleaning in 1:30 DHF is the least effective. However, the best results of all are obtained via a combination of wet and dry cleaning. With respect to in-situ hydrogen bake in the presence of H2 gas, the level of impurities is gradually decreased as the temperature increases from 700 °C to a maximum of 850 °C, at which no peaks of O and F are observed. Further, the addition of a hydrogen chloride (HCl) bake step after the H2 bake results in effective in-situ bake even at temperatures as low as 700 °C. In addition, the effects of temperature and environment (vacuum or gas) at the time of loading the wafers into the process chamber are compared. Better quality epitaxial films are obtained when the samples are loaded into the process chamber at low temperature in a gaseous environment. These results indicate that the epitaxial conditions must be carefully tuned and controlled in order to achieve high-quality epitaxial growth.

Epitaxy of LiNbO3: Historical Challenges and Recent Success

High-quality epitaxial growth of thin film lithium niobate (LiNbO3) is highly desirable for optical and acoustic device applications. Despite decades of research, current state-of-the-art epitaxial techniques are limited by either the material quality or growth rates needed for practical devices. In this paper, we provide a short summary of the primary challenges of lithium niobate epitaxy followed by a brief historical review of lithium niobate epitaxy for prevalent epitaxial techniques. Available figures of merit for crystalline quality and optical transmission losses are given for each growth method. The highest crystalline quality lithium niobate thin film was recently grown by halide-based molecular beam epitaxy and is comparable to bulk lithium niobate crystals. However, these high-quality crystals are grown at slow rates that limit many practical applications. Given the many challenges that lithium niobate epitaxy imposes and the wide variety of methods that have unsuccessfully attempted to surmount these barriers, new approaches to lithium niobate epitaxy are required to meet the need for simultaneously high crystalline quality and sufficient thickness for devices not currently practical by existing techniques.

Strain engineering of epitaxial oxide heterostructures beyond substrate limitations

Strain engineering of epitaxial oxide heterostructures beyond substrate limitations

Thin-film growth of MAX phases as functional materials

Abstract Layered nanolaminate ternary carbides, nitrides and carbonitrides with general formula Mn+1AXn or MAX (n = 1, 2, or 3, M is an early transition metal, A is mostly group 13 or 14 element and X is C and/or N) has revolutionized the world of nanomaterials, due to the coexistence of both ceramic and metallic nature, giving rise to exceptional mechanical, thermal, electrical, chemical properties and wide range of applications. Although several solid-state bulk synthesis methods have been developed to produce a variety of MAX phases, however, for certain applications, the growth of MAX phases, especially in its high-quality epitaxial thin-films form is of increasing interest. Here, we summarize the progress made thus far in epitaxial growth and property evaluation of MAX phase thin films grown by various deposition techniques. We also address the important future research directions to be made in terms of thin-film growth. Overall, in the future, high-quality single-phase epitaxial thin-film growth and engineering of chemically diverse MAX phases may open up interesting new avenues for next-generation technology.

(Invited) Epitaxial Growth of Ge/III-V Films and Hetero-Layer Lift-off for Ultra-Thin GeOI Fabrication

Monolithic 3D (M3D) integration has been thought of as an attractive idea to realize multi-functional heterogeneous integration devices. M3D integration enables us to combine logic devices with different functional devices such as memory, sensor, or optics to create extremely compact and efficient system-on-chips. Ge and III-V compound semiconductors are expected to be implemented as high mobility channel materials and optical components which cannot be realized with Si. The layer transfer technique with low processing temperature has great potential for stacking non-lattice-matched crystalline materials for M3D ICs. Here, we discuss the layer transfer technology utilizing high quality epitaxial growth, low-temperature direct bonding and advanced epitaxial lift-off (ELO) process, which reveals the applicability of transferred layers for heterogeneous integration.The low temperature ELO process is essential for realizing reliable layer transfer with different materials because the process is almost free from the issues of thermal expansion mismatch. Process flow of GaAs or Ge layer transfer with ELO process is described in Fig. 1. First of all, a lattice-matched single crystal GaAs or Ge layer is epitaxially grown on GaAs substrate with an AlAs release layer by MOCVD. Subsequently, Al2O3 layer is deposited on the epitaxial layer by atomic layer deposition (ALD). ALD Al2O3 layer serves as the buried oxide (BOX) and the passivation layer for Ge or GaAs surface. Then, Ge or GaAs layer is patterned using photolithography. The patterned GaAs or Ge/AlAs/GaAs donor wafer is then bonded on host substrate by direct bonding technique with wet activation process. Finally, the epitaxial GaAs or Ge layer is transferred on host substrates by splitting GaAs donor wafer from AlAs layer with HCl side etching thanks to extremely high etching selectivity. Note that the fabrication of patterned transfer layer is effective in shortening the required time of ELO process. In this ELO process, the thickness of a transferred layer can be control by epitaxial layer thickness. After the layer transfer process, the released donor GaAs wafer can be reclaimed and reused for the subsequent re-epitaxial growth to reduce the process cost.Figs. 2 (a) and (b) show cross-sectional SEM and TEM images of fabricated GeOI substrate with different BOX structures. Ge pattern edge shows no peeling from SiO2(100nm)/Si substrate, indicating strong bonding strength at the pattern edge. In Fig. 2 (b), the bonding interface is clearly observed at Al2O3(5nm)/SiO2(50nm) interface formed by the wet activation process. The bonding interface exhibits very smooth and no defect. There is no observable defect in transferred Ge layer, suggesting dislocation density is below TEM detection limit. Compared to Smart-CutTM technique, ELO process has significant advantages in terms of crystal quality, thickness control and the surface flatness thanks to totally low temperature processing.To reduce wafer-scale thickness variation, etching stopper (ES) technique with high etching selectivity is quite useful. As a donor wafer, we prepare Ge active layer (20nm)/SiGe ES layer (5nm)/Ge buffer layer/AlAs/GaAs structures. Here, the SiGe layer serves as ES against the etching of Ge buffer layer to control the final GeOI thickness and attain the wafer-scale thickness uniformity. In addition, Si passivation on Ge surface was performed during initial epitaxial growth of donor wafer since Si passivation was proved to be effective in reducing interfacial trap density (D it) between Ge and oxide. After ELO process, Ge buffer layer /SiGe ES layer/Ge active layer / Al2O3 /SiO2/Si heterostructure was obtained. Then, the top Ge buffer layer was removed in HCl/H2O2 solution. We found the etching selectivity was more than 30 between Ge and SiGe layer, which is high enough to yield very smooth SiGe surface. Finally, SiGe layer was removed by TMAH preferentially.Further conformal thinning of Ge active layer was performed by the cyclic dry oxidation/wet digital etching (DE) at room temperature. In addition to thickness control with the etching rate of about 0.8 nm/cycle, it is found that dozens digital etching (DDE) process is effective for reducing Ge surface roughness. Finally, UTB GeOI substrates with high crystal quality down to 3 nm have been successfully fabricated through SiGe ES and DDE processes. Ultra-smooth GeOI surface with reduced thickness fluctuation was confirmed after DDE by TEM cross-sectional images, resulting in significant improvement of device performances. Figure 1

Surface states modulated exchange interaction in Bi2Se3/thulium iron garnet heterostructures* *Project supported by the National Key Basic Research Project of China (Grant No. 2016YFA0300600), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB33020300), and the National Natural Science Foundation of China (Grant Nos. 11604375 and 11874416).

We investigate the modulation of magnetic anisotropy of thulium iron garnet (TmIG) films by interfaced Bi2Se3 thin films. High quality epitaxial growth of Bi2Se3 films has been achieved by molecular beam epitaxy on TmIG films. By the method of ferromagnetic resonance, we find that the perpendicular magnetic anisotropy (PMA) of TmIG can be greatly strengthened by the adjacent Bi2Se3 layer. Moreover, the competition between topological surface states and thickness dependent bulk states of Bi2Se3 gives rise to the modulation of PMA of the Bi2Se3/TmIG heterostructures. The interfacial interaction can be attributed to the enhanced exchange coupling between Fe3+ ions of TmIG mediated by topological surface electrons of Bi2Se3.