Spontaneous polarization in NaNbO3_{3} film on NdGaO3_{3} and DyScO3_{3} substrates

Pure NaNbO$_{3}$ is an antiferroelectric material at room temperature that irreversibly transforms to a ferroelectric polar state when subjected to an external electrical field or lattice strain. Experimentally, it has been observed that NaNbO$_{3}$ films grown on NdGaO$_{3}$ exhibit an electrical polarization along the [001]$_{\mathrm{PC}}$ direction, whereas films on DyScO$_{3}$ substrates exhibit a polarization along the [011]$_{\mathrm{PC}}$ direction. These effects have been attributed to the realization of different lattice symmetries in the films due to the incorporation of lattice strain imposed by the use of oxide substrates with different lattice parameters. However, the underlying atomistic mechanisms of the resulting phase symmetry in the films are hardly clear, given that NaNbO$_{3}$ features a diverse and complex phase diagram. In turn, these also impede a straightforward tailoring and optimization of the resulting macroscopic properties on different substrates. To clarify this issue, we perform all-electron first-principles calculations for several potential NaNbO$_{3}$ polymorphs under stress and strain. The computed properties, including the ferroelectric polarization, reveal that an orthorhombic $Pmc2_{1}$ phase is realized on NdGaO$_{3}$ substrates since this is the only phase with an out-of-plane polarization under a compressive strain. Conversely, the monoclinic $Pm$ phase is consistent for the samples grown on DyScO$_{3}$ substrate, since this phase exhibits a spontaneous in-plane polarization along [011]$_{\mathrm{PC}}$ under tensile strain.Comment: 9 pages, 5 figures, and supplementary material

Approaching the High Intrinsic Electrical Resistivity of NbO2 in Epitaxially Grown Films

NbO2 is a promising candidate for resistive switching devices due to an insulator-metal transition above room temperature, which is related to a phase transition from a distorted rutile structure to an undistorted one. However, the electrical resistivity of the NbO2 thin films produced so far has been too low to achieve high on-off switching ratios. Here, we report on the structural, electrical, and optical characterization of single-crystalline NbO2 (001) thin films grown by pulsed laser deposition on MgF2 (001) substrates. An annealing step reduced the full width at half maximum of the NbO2 (004) x-ray Bragg reflection by one order of magnitude, while the electrical resistivity of the films increased by two orders of magnitude to about 1k Omega cm at room temperature. Temperature-dependent resistivity measurements of an annealed sample revealed that below 650K, two deep-level defects with activation energies of 0.25eV and 0.37eV dominate the conduction, while above 650K, intrinsic conduction prevails. Optical characterization by spectroscopic ellipsometry and by absorption measurements with the electric field vector of the incident light perpendicular to the c-axis of the distorted rutile structure indicates the onset of fundamental absorption at about 0.76eV at room temperature, while at 4K, the onset shifts to 0.85eV. These optical transitions are interpreted to take place across the theoretically predicted indirect bandgap of distorted rutile NbO2

Perspectives on MOVPE-grown (100) β-Ga2O3thin films and its Al-alloy for power electronics application

Beta gallium oxide (β-Ga2O3) is a promising ultra-wide bandgap semiconductor with attractive physical properties for next-generation high-power devices, radio frequency electronics, and solar-blind ultraviolet radiation detectors. Here, we present an overview and perspective on the development of MOVPE-grown (100) β-Ga2O3 thin films and its role in supplementing high-power electronics. We review the development path of the growth process on (100) β-Ga2O3 thin films with a discussion regarding the solved and remaining challenges. The structural defect formation mechanism, substrate treatment strategies, and different growth windows are analyzed to optimize the grown film to fulfill the requirements for device fabrication. Toward industrial applications, MOVPE-grown β-Ga2O3 thin films are evaluated in two aspects: thick layers with smooth surface roughness and the electrical properties in terms of high carrier mobility and low doping concentration. Based on the reviewed results, we propose strategies in substrate preparation treatments and supportive tools such as the machine learning approaches for future growth process optimization and envision the rising interest of the β-Ga2O3-related alloy, β-(AlxGa1-x)2O3

Effect of post-metallization anneal on (100) Ga2O3/Ti–Au ohmic contact performance and interfacial degradation

Here, we investigate the effect of post-metallization anneal temperature on Ti/Au ohmic contact performance for (100)-oriented Ga2O3. A low contact resistance of ∼2.49 × 10−5 Ω·cm2 is achieved at an optimal anneal temperature of ∼420 °C for (100) Ga2O3. This is lower than the widely-used temperature of 470 °C for (010)-oriented Ga2O3. However, drastic degradation of the (100)-oriented contact resistance to ∼1.36 × 10−3 Ω·cm2 is observed when the anneal temperature was increased to 520 °C. Microscopy at the degraded ohmic contact revealed that the reacted Ti–TiOx interfacial layer has greatly expanded to 25–30 nm thickness and GaAu2 inclusions have formed between (310)-Ga2O3 planes and the Ti–TiOx layer. This degraded interface, which corresponds to the deterioration of ohmic contact properties, likely results from excess in-diffusion of Au and out-diffusion of Ga, concurrent with the expansion of the Ti–TiOx layer. These results demonstrate the critical influence of Ga2O3 anisotropy on the optimal post-metallization anneal temperature. Moreover, the observed Ti/Au contact degradation occurs for relatively moderate anneal conditions (520 °C for 1 min in N2), pointing to the urgent necessity of developing alternative metallization schemes for gallium oxide, including the use of Au-free electrode

Refractory metal-based ohmic contacts on β-Ga2O3 using TiW

The present work investigates the use of the refractory metal alloy TiW as a possible candidate for the realization of ohmic contacts to the ultrawide bandgap semiconductor β-Ga2O3. Ohmic contact properties were analyzed by transfer length measurements of TiW contacts annealed at temperatures between 400 and 900 °C. Optimum contact properties with a contact resistance down to 1.5 × 10-5 ω cm2 were achieved after annealing at 700 °C in nitrogen on highly doped β-Ga2O3. However, a significant contact resistance increase was observed at annealing temperatures above 700 °C. Cross-sectional analyses of the contacts using scanning transmission electron microscopy revealed the formation of a TiOx interfacial layer of 3-5 nm between TiW and β-Ga2O3. This interlayer features an amorphous structure and most probably possesses a high amount of vacancies and/or Ga impurities supporting charge carrier injection. Upon annealing at temperatures of 900 °C, the interlayer increases in thickness up to 15 nm, featuring crystalline-like properties, suggesting the formation of rutile TiO2. Although severe morphological changes at higher annealing temperatures were also verified by atomic force microscopy, the root cause for the contact resistance increase is attributed to the structural changes in thickness and crystallinity of the interfacial layer

High-mobility 4 μm MOVPE-grown (100) β-Ga2O3 film by parasitic particles suppression

In this work, we comprehensively investigate the development of unwanted parasitic particles in the MOVPE chamber while growing μm level films. The density of the parasitic particles is found to be pronounced at film thicknesses starting from >1.5 to 2 μm. These particles seem to induce structural defects such as twin lamellae, thereby harming the electrical properties of the grown film. The origin of the parasitic particle is attributed to the parasitic reactions within the chamber triggered by the promoted gas-phase reactions during the growth process, which can be largely reduced by increasing the total gas flow and decreasing the showerhead distance to the susceptor. A film thickness of up to 4 μm has been achieved after minimizing the density of parasitic particles. Thereby, RT Hall measurements reveal carrier mobilities of 160 cm2V−1s−1 at carrier concentrations of 5.7 × 1016cm−

Suppression of particle formation by gas-phase pre-reactions in (100) MOVPE-grown β -Ga2O3films for vertical device application

This work investigated the metalorganic vapor-phase epitaxy (MOVPE) of (100) β-Ga2O3 films with the aim of meeting the requirements to act as drift layers for high-power electronic devices. A height-adjustable showerhead achieving a close distance to the susceptor (1.5 cm) was demonstrated to be a critical factor in increasing the stability of the Ga wetting layer (or Ga adlayer) on the surface and reducing parasitic particles. A film thickness of up to 3 μm has been achieved while keeping the root mean square below 0.7 nm. Record carrier mobilities of 155 cm2 V-1 s-1 (2.2 μm) and 163 cm2 V-1 s-1 (3 μm) at room temperature were measured for (100) β-Ga2O3 films with carrier concentrations of 5.7 × 1016 and 7.1 × 1016 cm-3, respectively. Analysis of temperature-dependent Hall mobility and carrier concentration data revealed a low background compensating acceptor concentration of 4 × 1015 cm-3

Bulk single crystals and physical properties of β-(AlxGa1-x)2O3(x = 0-0.35) grown by the Czochralski method

We have systematically studied the growth, by the Czochralski method, and basic physical properties of a 2 cm and 2 in. diameter bulk β-(AlxGa1-x)2O3 single crystal with [Al] = 0-35 mol. % in the melt in 5 mol. % steps. The segregation coefficient of Al in the Ga2O3 melt of 1.1-1.2 results in a higher Al content in the crystals than in the melt. The crystals were also co-doped with Si or Mg. [Al] = 30 mol. % in the melt (33-36 mol. % in the crystals) seems to be a limit for obtaining bulk single crystals of high structural quality suitable for homoepitaxy. The crystals were either semiconducting (no intentional co-dopants with [Al] = 0-30 mol. % and Si-doped with [Al] = 15-20 mol. %), degenerately semiconducting (Si-doped with [Al] ≤ 15 mol. %), or semi-insulating ([Al] ≥ 25 mol. % and/or Mg-doped). The full width at half maximum of the rocking curve was 30-50 arcsec. The crystals showed a linear but anisotropic decrease in all lattice constants and a linear increase in the optical bandgap (5.6 eV for [Al] = 30 mol. %). The room temperature electron mobility at similar free electron concentrations gradually decreases with [Al], presumably due to enhanced scattering at phonons as the result of a larger lattice distortion. In Si co-doped crystals, the scattering is enhanced by ionized impurities. Measured electron mobilities and bandgaps enabled to estimate the Baliga figure of merit for electronic devices

Kinetic Monte Carlo model for homoepitaxial growth of Ga_{2}O_{3}

We developed a kinetic Monte Carlo (KMC) model for the homoepitaxy of β-Ga_{2}O_{3}. It comprises adsorption, diffusion, and desorption and reflects the structure of β-Ga_{2}O_{3} with its two kinds of atoms: Ga and O. The knowledge gained from metal organic vapour phase experiments (MOVPE) experiments combined with AFM and TEM characterisation was used for the setup of rules and activation energies for the various surface processes. We performed a set of runs for the growth on flat and vicinal (100) surfaces. The nucleation on the flat surface requires a minimum ratio of the impingement rate of O_{2} and Ga. The behavior at different substrate temperatures was similar in experiment and in simulation. At high temperatures, we observe the formation of large islands whereas at low temperatures small islands are formed. The growth rate is increasing with decreasing temperature. On a vicinal surface (6^{∘}) different growth modes have been observed when using different desorption energies. Low desorption energy (high desorption rate) leads to step bunching, intermediate to step growth, and high energy (low desorption rate) to nucleation on terraces with a final configuration similar to step bunching