Epitaxial Growth Of Thin Films Research Articles

Epitaxial growth, structural and magnetic characterization of thulium thin films

Epitaxial growth, structural and magnetic characterization of thulium thin films

Expanded Stability of Layered SnSe-PbSe Alloys and Evidence of Displacive Phase Transformation from Rocksalt in Heteroepitaxial Thin Films.

Bulk PbSnSe has a two-phase region, or miscibility gap, as the crystal changes from a van der Waals-bonded orthorhombic 2D layered structure in SnSe-rich compositions to the related 3D-bonded rocksalt structure in PbSe-rich compositions. This structural transition drives a large contrast in the electrical, optical, and thermal properties. We realize low temperature direct growth of epitaxial PbSnSe thin films on GaAs via molecular beam epitaxy using an in situ PbSe surface treatment and show a significantly reduced two-phase region by stabilizing the Pnma layered structure out to Pb0.45Sn0.55Se, beyond the bulk limit around Pb0.25Sn0.75Se at low temperatures. Pushing further, we directly access metastable two-phase films of layered and rocksalt grains that are nearly identical in composition around Pb0.50Sn0.50Se and entirely circumvent the miscibility gap. We present microstructural and compositional evidence for an incomplete displacive transformation from a rocksalt to layered structure in these films, which we speculate occurs during the sample cooling to room temperature after synthesis. In situ temperature-cycling experiments on a Pb0.58Sn0.42Se rocksalt film reproduce characteristic attributes of a displacive transition and show a modulation in electronic properties. We find well-defined orientation relationships between the phases formed and reveal unconventional strain relief mechanisms involved in the crystal structure transformation using transmission electron microscopy. Overall, our work adds a scalable thin film integration route to harness the dramatic contrast in material properties in PbSnSe across a potentially ultrafast crystalline-crystalline structural transition.

Epitaxial growth and stoichiometry control of pyrochlore Nd2Ru2O7 thin films

We report on the epitaxial growth of pyrochlore NRO thin films utilizing a reactive off-axis sputtering technique. The growth process employed Ru and Nd metal targets with a repetitive substrate temperature sequence. X-ray diffraction, magnetic susceptibility, and spectroscopic ellipsometry measurements confirm that the structural, magnetic, and electronic properties of near-stoichiometric NRO films match those of the bulk material. Our spin-polarized density functional calculations based on Nd2Ru2O7 structural parameters accurately describe the optical spectra and assign Hubbard bands to the interband transitions observed above the optical band gap of 0.2 eV. By utilizing the technique's capability to adjust the degree of ruthenium deficiency, we investigated Nd2Ru2O7 films across a wide range of stoichiometric variations. Decreasing the Ru/Nd ratio results in lattice expansion, an increase in the optical band gap, and the suppression of Ru 4d intersite optical transitions. Additionally, this adjustment facilitates the elimination of minor inclusions of a ferromagnetic NdOx impurity phase, influencing the magnetic properties of stoichiometric films at low temperatures. The successful growth of Nd2Ru2O7 films opens up promising opportunities for designing and exploring strain- and light-induced states in pyrochlore ruthenates. Published by the American Physical Society 2024

Blow-up at infinity of solutions to a class of pseudo-parabolic equations with logarithmic nonlinearity and singular potential

We study the initial–boundary value problem for a class of pseudo-parabolic equations in a bounded domain Ω with smooth boundary ∂Ω and 0∈Ω⊂BR(0)⊂Rn(n≥1), where BR(0) is a ball centered at 0 with radius R. First, we simplify the scheme of potential well method, which helps us obtain the invariant set in an easier way. Combining logarithmic Sobolev inequality and Hardy inequality, we prove that the solutions to the pseudo-parabolic equations with logarithmic nonlinearity ulog|u| blow up at infinity when R≤1. However, there is no restriction on R if the singular potential is 1. Second, when the singular potential is 1 and the pseudo-parabolic term vanishes, the equations model the epitaxial growth of thin films. We also show that the solutions have better growth rate under weaker conditions, which improves the result in Han et al. (2019).

Beta-Gallium Oxide Material and Device Technologies

Beta-gallium oxide (β-Ga2O3) is a material with a history of research and development spanning about 70 years; however, it has attracted little attention as a semiconductor for a long time. The situation has changed completely in the last ten years, and the world has seen increasing demand for active research and development of both materials and devices. Many of its distinctive physical properties are attributed to its very large bandgap energy of 4.5 eV. Another important feature is that it is possible to grow large bulk single crystals by melt growth. In this article, we first discuss the physical properties of β-Ga2O3, which are mainly important for electronic device applications, bulk melt growth, and thin-film epitaxial growth technologies. Then, state-of-the-art β-Ga2O3 transistor and diode technologies are discussed.

Highly oriented epitaxial Cu2O (011) thin film grown on MgO (001) substrate by dynamic aurora PLD method

The epitaxial Cu2O films are grown on MgO (001) substrates by the dynamic aurora pulsed laser deposition (PLD) method. The structure and epitaxial growth of the as-prepared thin films at different substrate temperatures (25 °C to 600 °C) were investigated. The thin film prepared at room temperature (RT, 25 °C) exhibits (111) plane of monoclinic CuO phase with poor crystallinity. The thin films deposited at 200 °C to 600 °C show single-phase cubic Cu2O with good crystallinity. The highly oriented epitaxial Cu2O thin film on the MgO substrate is achieved at low temperatures of 200 °C by applying an induced electromagnetic field during thin film growth. The quality and crystallinity of epitaxial Cu2O thin films remarkably improved with increasing temperature from 200 °C to 600 °C and all these thin films exhibited an out-of-plane epitaxial relationship of Cu2O (011) ‖ MgO (001). The CuO thin film grown on MgO substrate at RT shows a single domain structure, as observed by RHEED. In constrast, Cu2O films grown at 200 °C to 600 °C exhibit two different kinds of domain structure with corresponding in-plane epitaxial relationship of Cu2O [100] ‖ MgO [110] and Cu2O [100] ‖ MgO [11¯0]. This report reveals, for the first time, the feasibility of epitaxial growth of highly oriented Cu2O (011) thin film achieved at the low temperature of 200 °C by the dynamic aurora PLD method. The quality of epitaxial Cu2O (011) is significantly enhanced with increasing substrate temperature from 200 °C to 600 °C.

Epitaxial growth of AgCrSe2 thin films by molecular beam epitaxy

AgCrS e 2 exhibits remarkably high ionic conduction, an inversion symmetry-breaking structural transition, and is host to complex non-colinear magnetic orders. Despite its attractive physical and chemical properties and its potential for technological applications, studies of this compound to date are focused almost exclusively on bulk samples. Here, we report the growth of AgCrSe2 thin films via molecular beam epitaxy. Single-orientated epitaxial growth was confirmed by x-ray diffraction, while resonant photoemission spectroscopy measurements indicate a consistent electronic structure as compared to bulk single crystals. We further demonstrate significant flexibility of the grain morphology and cation stoichiometry of this compound via control of the growth parameters, paving the way for the targeted engineering of the electronic and chemical properties of AgCrSe2 in thin-film form.

Evaluation of Sputtering Processes in Strontium Iridate Thin Films

The growth of epitaxial thin films from the Ruddlesden–Popper series of strontium iridates by magnetron sputtering is analyzed. It was found that, even using a non-stoichiometric target, the films formed under various conditions were consistently of the perovskite-like n = ∞ SrIrO3 phase, with no evidence of other RP series phases. A detailed inspection of the temperature–oxygen phase diagram underscored that kinetics mechanisms prevail over thermodynamics considerations. The analysis of the angular distribution of sputtered iridium and strontium species indicated clearly different spatial distribution patterns. Additionally, significant backsputtering was detected at elevated temperatures. Thus, it is assumed that the interplay between these two kinetic phenomena is at the origin of the preferential nucleation of the SrIrO3 phase. In addition, strategies for controlling cation stoichiometry off-axis have also been explored. Finally, the long-term stability of the films has been demonstrated.

In-situ study on piezoelectric responses of sol-gel derived epitaxial Pb[Zr,Ti]O3 thin films on Si substrate

Pb[Zr,Ti]O3 (PZT) thin films with the Zr/Ti ratio of 45/55, 52/48, and 60/40 (PZT(45/55), PZT(52/48), and PZT(60/40), respectively) are deposited on (001)SrRuO3/(001)Pt/ZrO2/Si by sol-gel method. We confirm that the epitaxial (001)Pt electrode facilitate the epitaxial growth of the PZT thin films along the c-axis direction. Basic characteristics such as structural, dielectric, and ferroelectric properties are examined. Furthermore, direct and converse piezoelectric properties are evaluated using effective transverse piezoelectric coefficients, |e31,f|. In particular, the epitaxial PZT thin films manifest a dependence of the converse |e31,f| on applied voltages with the values as follows; 9.7–11.5 C/m2, 11.2–12.5 C/m2, and 11.7–12.3 C/m2 for the epitaxial PZT(45/55), PZT(52/48), and PZT(60/40), respectively. Moreover, by analyzing bias-resolved in-situ reciprocal space map (RSM) obtained from synchrotron radiation X-ray diffraction (SR-XRD) which allows for the understanding on the transition of crystal structures, we explore the voltage-induced contributions for the converse |e31,f|.

Orientation-dependent atomic-scale mechanism and defect evolution in β-Ga2O3 thin film epitaxial growth

β-Ga2O3 has been subjected to intense research interest as an ultrawide bandgap semiconductor. The epitaxial growth technique of β-Ga2O3 thin films plays a fundamental and vital role in Ga2O3-based device fabrication. In this work, the epitaxial growth mechanisms of β-Ga2O3 on four low-Miller-index facets, (100), (010), (001), and (2¯01), are systematically explored using large-scale machine-learning molecular dynamics simulations at the atomic scale. The simulations reveal that the migration of the face-centered cubic stacking O sublattice plays a dominant role in the different growth mechanisms between the (100)/(010)/(001) and (2¯01) orientations. The resultant complex combinations of the stacking faults and twin boundaries are carefully identified and show good agreement with experimental observations and ab initio calculations. Our results provide useful insights into the gas-phase epitaxial growth of β-Ga2O3 thin films and suggest possible ways to tailor its properties for specific applications.

MOCVD Epitaxial Growth and Characterization of Polar, Semipolar and Nonpolar InN Thin Films

MOCVD Epitaxial Growth and Characterization of Polar, Semipolar and Nonpolar InN Thin Films

Towards the epitaxial growth of Au thin films on MgO substrates for plasmonic applications

Surface Plasmon Polaritons (SPPs) in Au thin films are nowadays intensively exploited for sensing applications that leverage the strong optical field confinement at the metal/dielectric interface and the easy functionalization of the Au surface. Moreover, Au thin films represent one of the common starting points for the top-down nanofabrication of plasmonic nanostructures supporting localized resonances. In this framework, strategies for the growth of high-quality Au films on transparent substrates are crucial and not yet fully established. In this study, we exploit MgO(001) substrates for the growth of thin (about 45 nm) Au films, also including an additional buffer layer of Fe. We successfully demonstrate Au samples with reduced roughness and presenting Low-Energy Electron Diffraction (LEED) features, indicating a high degree of crystalline ordering. This is supported by the experimental evidence of an increased (by almost a factor of 3) propagation length compared to a reference Au sample grown on standard glass slides, which is however still significantly lower than the one expected from first principles.

Sputter-grown two-dimensional α-MoO3 thin films: Microstructure dependence on growth conditions

Van der Waals epitaxy is an emerging technology for transferring freestanding films grown at high temperatures onto arbitrary substrates using two-dimensional epitaxial layers. This study investigates the microstructure and growth of α-MoO3 thin films prepared via sputtering. Under a narrow deposition temperature range, epitaxial α-MoO3 thin films were successfully grown on SrTiO3 substrates. The films were characterized by a flat surface morphology, corresponding to (0k0) planes, without undergoing reaction with the substrates. To examine the growth behavior and surface morphological variation of the α-MoO3 thin films under various process parameters, we modified the Ar:O2 ratio, working pressure, sputtering power, and crystal structure of the substrates. Transmittance electron microscopy confirmed the epitaxial growth of the α-MoO3 thin films on (001)-oriented SrTiO3 substrates with a two-dimensional layer structure. Finally, we demonstrate the morphological evolution of the α-MoO3 thin films etched in heated water as a function of soaking time. The etching results suggest that the α-MoO3 thin films are promising sacrificial layers for the transfer of large-scale epitaxial thin films onto flexible substrates. External control of the strain states of transferred freestanding thin films by bending or stretching provides new perspectives for the design of flexible or wearable electronic devices.

Thin Films of α-Quartz GeO2 on TiO2-Buffered Quartz Substrates.

α-Quartz (SiO2) is one of the most widely used piezoelectric materials. However, the challenges associated with the control of the crystallization and the growth process limit its production to the hydrothermal growth of bulk crystals. GeO2 can also crystallize into the α-quartz phase, with a higher piezoelectric response and better thermal stability than SiO2. In a previous study, we have found that GeO2 crystallization on nonquartz substrates shows a tendency to form spherulites with a randomized orientation; while epitaxial growth of crystalline GeO2 thin films can take place on quartz (SiO2) substrates. However, in the latter case, the α-β phase transition that takes place in both substrates and thin films during heating deteriorates the long-range order and, thus, the piezoelectric properties. Here, we report the ousting of spherulitic growth by using a buffer layer. Using TiO2 as a buffer layer, the epitaxial strain of the substrates can be transferred to the growing films, leading to the oriented crystallization of GeO2 in the α-quartz phase. Moreover, since the TiO2 separates the substrates and the thin films, the thermal stability of the GeO2 is kept across the substrate's phase transitions. Our findings reveal the complexity of the crystallization process of quartz thin films and present a way to eliminate the tendency for spherulitic growth of quartz thin films by epitaxial strain.

Investigating Anisotropic Magnetoresistance in Epitaxially Strained CoFe Thin Films on a Flexible Mica.

This study investigates the crystal structure, epitaxial relation, and magnetic properties in CoFe thin films deposited on a flexible mica substrate. The epitaxial growth of CoFe thin films was successfully achieved by DC magnetron sputtering, forming three CoFe(002) domains exhibiting four-fold symmetry on the mica substrate. A notable achievement of this work was the attainment of the highest anisotropic magnetoresistance (AMR) value reported to date on a flexible substrate. Additionally, it was observed that the magnetic characteristics of the CoFe films on the flexible mica substrate display reversibility upon strain release. More importantly, the AMR effect of epitaxial CoFe films on flexible mica shows lesser dependence on the crystalline orientation and remains the same under different bending states. These findings demonstrate the potential of utilizing CoFe films on flexible substrates to develop wearable magnetoresistance sensors with diverse applications.

Stabilizing Crystal Framework of an Overlithiated Li1+xMn2O4 Cathode by Heterointerfacial Epitaxial Strain for High-Performance Microbatteries.

To meet the increasing demands of high-energy and high-power-density lithium-ion microbatteries, overlithiated Li1+xMn2O4 (0 ≤ x ≤ 1) is an attractive cathode candidate due to the high theoretical capacity of 296 mAh g-1 and the interconnected lithium-ion diffusion pathways. However, overlithiation triggers the irreversible cubic-tetragonal phase transition due to Jahn-Teller distortion, causing rapid capacity degradation. In contrast to conventional lithium-ion batteries, microbatteries offer the opportunity to develop specific thin-film-based modification strategies. Here, heterointerfacial lattice strain is proposed to stabilize the spinel crystal framework of an overlithiated Li1+xMn2O4 (LMO) cathode by epitaxial thin film growth on an underlying SrRuO3 (SRO) electronic conductor layer. It is demonstrated that the lattice misfit at the LMO/SRO heterointerface results in an in-plane epitaxial constraint in the full LMO film. This suppresses the lattice expansion during overlithiation that typically occurs in the in-plane direction. It is proposed by density functional theory modeling that the epitaxial constraint can accommodate the internal lattice stress originating from the cubic-tetragonal transition during overlithiation. As a result, a doubling of the capacity is achieved by reversibly intercalating a second lithium ion in a LiMn2O4 epitaxial cathode with a complete reversible phase transition. An impressive cycling stability can be obtained with reversible capacity retentions of above 90.3 and 77.4% for the 4 and 3 V range, respectively. This provides an effective strategy toward a stable overlithiated Li1+xMn2O4 epitaxial cathode for high-performance microbatteries.

Pulsed-Mode Metalorganic Vapor-Phase Epitaxy of GaN on Graphene-Coated c-Sapphire for Freestanding GaN Thin Films.

We report the growth of high-quality GaN epitaxial thin films on graphene-coated c-sapphire substrates using pulsed-mode metalorganic vapor-phase epitaxy, together with the fabrication of freestanding GaN films by simple mechanical exfoliation for transferable light-emitting diodes (LEDs). High-quality GaN films grown on the graphene-coated sapphire substrates were easily lifted off by using thermal release tape and transferred onto foreign substrates. Furthermore, we revealed that the pulsed operation of ammonia flow during GaN growth was a critical factor for the fabrication of high-quality freestanding GaN films. These films, exhibiting excellent single crystallinity, were utilized to fabricate transferable GaN LEDs by heteroepitaxially growing InxGa1-xN/GaN multiple quantum wells and a p-GaN layer on the GaN films, showing their potential application in advanced optoelectronic devices.

Epitaxial growth of Si thin films with hexagonal close-packed structures on metal substrates.

We have studied the epitaxial growth of Si thin films on the Cd(0001) surface using low-temperature scanning tunneling microscopy. When deposited at low temperatures (100K), Si atoms form dendritic islands with triangular shapes, indicating the existence of anisotropic edge diffusion in the process of Si film growth. After annealing to elevated temperatures, the triangular dendritic Si islands become hexagonal compact islands. Moreover, the 2D Si islands located on two different substrate terraces exhibit different heights due to the influence of quantum-well states in Cd(0001) films. Based on high-resolution scanning tunneling microscopy images, it is observed that the first, second, and third Si layers show the pseudomorphic 1 × 1 structure. In particular, the first and second layer islands reveal the opposite triangles, indicating the hexagonal close-packed stacking of Si atoms. These results provide important information for the growth of pristine Si films on metal substrates and the understanding of Si-metal interaction.

Epitaxial growth of thin films of X-type Sr2Co2Fe28O46 hexaferrite by chemical solution deposition

Epitaxial growth of thin films of X-type Sr2Co2Fe28O46 hexaferrite by chemical solution deposition

Spin Hall Switching Enabled by Uniaxial In-Plane Magnetocrystalline Anisotropy

We present a new method for stabilization of magnetic devices: in-plane uniaxial magnetocrystalline anisotropy, achieved through epitaxial growth of a magnetic thin film on a single-crystal substrate. This paradigm enables the creation of in-plane spin orbit torque magnetic random access memory (SOT-MRAM) devices that function without external fields and exhibit the same scalability as perpendicular SOT-MRAM. Through theoretical derivations and numerical simulations based on the Landau-Lifshitz-Gilbert (LLG) equation with spin transfer torque, we show that switching of such devices can be optimized by varying the angle between the injected spin current and the crystalline easy axis, and contrast this angular dependence with the Stoner-Wohlfarth model. Furthermore, we demonstrate rich and complex magnetization dynamics in this system, including strong and tunable dependence on bulk and interfacial magnetoresistance and boundaries between stochastic and deterministic switching. Finally, we present a concept that couples our in-plane anisotropy layer with an out-of-plane ferromagnet to achieve out-of-plane field-free SOT-MRAM switching. We quantify regions of operation for this new device and link them to simulation results for the in-plane layer alone.