xN Layers Research Articles

Designing TaC Virtual Substrates for Vertical AlxGa1−xN Power Electronics Devices

Power electronics are critical for a sustainable energy future, playing a key role in electrification and integration of renewable energy sources into the grid. Advances in ultrawide band gap materials are needed to handle higher powers in smaller form factors while reducing electrical and thermal losses. High Al content AlxGa1−xN is theoretically capable of meeting these demands, but its impact in power electronics has been severely restricted by a lack of substrates that can satisfy conductivity, lattice matching, and/or thermal expansion requirements. We demonstrate that electrically conductive TaC can be used as a virtual substrate for AlxGa1−xN heteroepitaxy. Scaleably sputtered TaC grown on Al2O3, followed by high-temperature face-to-face annealing, produces a thin film TaC template with an effective hexagonal lattice constant matched to Al0.70Ga0.30N. Annealing of the TaC promotes recrystallization, significantly improving crystallinity and reducing crystalline defects from as-deposited columnar grains to a step-and-terrace surface morphology, enabling the subsequent growth of high-quality Al0.70Ga0.30N by molecular beam epitaxy. X-ray diffraction and scanning transmission electron microscopy confirm that the AlxGa1−xN layer is heteroepitaxially aligned, strain-free, and lattice-matched, transitioning abruptly from TaC to AlxGa1−xN without intermediate phases. These results demonstrate TaC virtual substrates as electrically conductive, lattice-matched, and thermally compatible templates for vertical AlxGa1−xN devices that can meet the growing power needs of a sustainable energy future. Published by the American Physical Society 2024

Pinpointing lattice-matched conditions for wurtzite ScxAl1−xN/GaN heterostructures with x-ray reciprocal space analysis

Using comprehensive x-ray reciprocal space mapping, we establish the precise lattice-matching composition for wurtzite ScxAl1−xN layers on (0001) GaN to be x = 0.14 ± 0.01. 100 nm thick ScxAl1−xN films (x = 0.09–0.19) were grown in small composition increments on c-plane GaN templates by plasma-assisted molecular beam epitaxy. The alloy composition was estimated from the fit of the (0002) x-ray peak positions, assuming the c-lattice parameter of ScAlN films coherently strained on GaN increases linearly with Sc-content determined independently by Rutherford backscattering spectrometry [Dzuba et al., J. Appl. Phys. 132, 175701 (2022)]. Reciprocal space maps obtained from high-resolution x-ray diffraction measurements of the (101¯5) reflection reveal that ScxAl1−xN films with x = 0.14 ± 0.01 are coherently strained with the GaN substrate, while the other compositions show evidence of relaxation. The in-plane lattice-matching with GaN is further confirmed for a 300 nm thick Sc0.14Al0.86N layer. The full-width-at-half-maximum of the (0002) reflection rocking curve for this Sc0.14Al0.86N film is 106 arc sec and corresponds to the lowest value reported in the literature for wurtzite ScAlN films.

Extraordinary Structural Reconstruction of Nanolaminated Ta2FeC MAX Phase for Enhanced Oxygen Evolution Performance.

Renewable energy technologies, such as water splitting, heavily depend on the oxygen evolution reaction (OER). Nanolaminated ternary compounds, referred to as MAX phases, show great promise for creating efficient electrocatalysts for OER. However, their limited intrinsic oxidative resistance hinders the utilization of conductivity in Mn+1Xn layers, leading to reduced activity. In this study, a method is proposed to improve the poor inoxidizability of MAX phases by carefully adjusting the elemental composition between Mn+1Xn layers and single-atom-thick A layers. The resulting Ta2FeC catalyst demonstrates superior performance compared to conventional Fe/C-based catalysts with a remarkable record-low overpotential of 247mV (@10mA cm-2) and sustained activity for over 240h. Notably, during OER processing, the single-atom-thick Fe layer undergoes self-reconstruction and enrichment from the interior of the Ta2FeC MAX phase toward its surface, forming a Ta2FeC@Ta2C@FeOOH heterostructure. Through density functional theory (DFT) calculations, this study has found that the incorporation of Ta2FeC@Ta2C not only enhances the conductivity of FeOOH but also reduces the covalency of Fe─O bonds, thus alleviating the oxidation of Fe3+ and O2-. This implies that the Ta2FeC@Ta2C@FeOOH heterostructure experiences less lattice oxygen loss during the OER process compared to pure FeOOH, leading to significantly improved stability. These results highlight promising avenues for further exploration of MAX phases by strategically engineering M- and A-site engineering through multi-metal substitution, to develop M2AX@M2X@AOOH-based catalysts for oxygen evolution.

The effect of FeGa (0/–) level presence on material properties in dilute AlxGa1−xN layers

AlxGa1−xN epilayers are used as the basis of ultraviolet LEDs and detectors. The trap states produced by defects and impurities can play a key role in the device performance. In this work, conventional deep-level transient spectroscopy, photoluminescence (PL), and secondary ion mass spectrometry have been used to characterize a deep-level trap termed as E3 in dilute AlxGa1−xN (x < 0.063) epilayers grown by metal-organic vapor phase epitaxy (MOVPE) on highly conductive ammono-GaN substrates. The AlxGa1−xN epilayers were doped with silicon to about 3 × 1016 cm−3. The electrical and the optical measurements were conducted on Ni/Au Schottky barrier diodes and virgin samples, respectively. First, we observed a general trend that the E3 (FeGa) electron trap concentration significantly changes along the wafers in AlxGa1−xN layers that is fully consistent with previously reported results for GaN materials grown by the MOVPE technique. Second, we report that the activation energies for electron emission for the E1 and E3 traps in dilute AlxGa1−xN exhibit linear variations with Al content. Moreover, low-temperature PL results show a proportional relation between the intensity of the line with its maximum at 1.299 eV and concentration of residual Fe impurity. Finally, we discuss how the presence of defects resulting from Fe contamination may result in degradation of AlxGa1−xN-based devices.

Theoretical Studies of 2D Electron Gas Distributions and Scattering Characteristics in Double‐Channel n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN High‐Electron‐Mobility Transistors

A detailed analysis of self‐consistent potentials, electric fields, electron distributions, and transport properties of dual‐channel (DC) n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN high‐electron‐mobility transistors (HEMTs) is performed in this article. The 2D electron gas (2DEG) densities and mobility states limited by different scattering mechanisms in channel 1 and channel 2 are obtained, with varying values of doping concentrations, ambient temperatures, Al components, and thicknesses of the back barrier layer. The reduced and increased 2DEG densities are respectively observed in channel 1 and channel 2 with growing Al fractions and thicknesses of the AlxGa1−xN layer. Alloy disorder scattering exhibits a superior effect on carriers in channel 2 due to the lower barrier height and higher permeable electrons, which together with the interface roughness scattering severely depends on the thicknesses and Al fractions of the back barrier layer. Polar optical phonon scattering becomes important at higher temperatures. The trend of individual mobility in channel 1 is exactly opposite to that in channel 2. The parameter variation of the back barrier layer can effectively change the scattering characteristics of the main channel. Low‐temperature mobilities of n‐Al0.3Ga0.7N/GaN/i‐AlxGa1−xN/GaN HEMTs under varied doping concentrations are also obtained. Finally, the results are verified by comparison with the technology computer‐aided design simulations for DC HEMTs.

Effects of structural defects on optical properties of InxGa1−xN layers and quantum wells

This review concentrates on the microstructure of InxGa1−xN layers and quantum wells (QWs) in relation to their optical properties. The microstructure of InxGa1−xN, with a constant In(x) concentration, shifts with layer thickness. Only layers below 100 nm for x = 0.1 are nearly defect-free. A photoluminescence peak is observed at 405 nm, in line with ∼10% In, suggesting band-edge luminescence. Layers with greater thickness and In content present a corrugated surface with numerous structural defects, including V-defects, causing redshifts and multi-peaks in photoluminescence up to 490 nm. These defects, resembling those in GaN, lead to a corrugated sample surface. Atomic force microscopy shows a 3.7-fold larger corrugation in samples with 20 QWs compared to those with 5 QWs measured on 2 × 2 μm2 areas. Like in GaN, dual growth on different crystallographic planes results in varied QW thicknesses, influencing optical traits of devices made from InxGa1−xN layers. The purpose of this review and the chosen subject is to highlight the significant contribution of Wladek Walukiewicz and his group to the current research on the properties of InxGa1−xN, which are crucial alloys in the field of optoelectronics.

Alloy splitting of the FeGa acceptor level in dilute AlxGa1−xN

The results of conventional deep-level transient spectroscopy (DLTS) and high-resolution Laplace DLTS measurements of the FeGa(0/−) acceptor level in dilute AlxGa1−xN layers (x ≤ 0.05) grown by MOVPE technique (metal–organic vapor phase epitaxy) on native ammono-GaN substrates are analyzed and discussed. It is shown that the electron emission signal related to the FeGa acceptor level in AlxGa1−xN splits into individual components due to aluminum fluctuations in the second-nearest neighbor (2NN) shell around the FeGa impurity atoms. The calculations of the probability of finding a given number of aluminum atoms in the 2NN shell of the FeGa defect agree well with the experimental concentrations determined from Laplace DLTS peak intensities. This finding shows that in dilute AlxGa1−xN layers grown by MOVPE, aluminum and iron atoms are randomly distributed in the material. Finally, we demonstrate that the energy level of the FeGa acceptor with no Al atoms in the 2NN shell in the AlxGa1−xN samples shifts linearly with the aluminum content and the shifts are 28 and 55 meV relative to that in GaN for the samples with x = 0.025 and 0.05, respectively.

A nonvolatile memory element for integration with superconducting electronics

We demonstrate a nonvolatile cryogenic magnetic memory element needed to support emerging superconducting- and quantum-computing technologies. The central element is a switchable tri-layer thin film magnetic dot comprising two semiconducting ferromagnetic GdxSm1−xN layers separated by an exchange-blocking Al layer. The materials are explored for their tunable magnetic responses, the potential to engineer compensating magnetic moments in the anti-parallel tri-layers. The stability of the parallel and anti-parallel states and the reproducibility over repeated cycles are also demonstrated. We show that the tri-layer stacks can be formed into dots as small as 4 μm diameter, without affecting their magnetic behavior.

A Threshold‐Voltage and Drain–Source Current Model for Double‐Channel AlxGa1−xN/GaN/AlyGa1−yN/GaN High‐Electron‐Mobility Transistors

A physics‐based threshold voltage and drain–source current model based on double‐channel AlxGa1−xN/GaN/AlyGa1−yN/GaN high‐electron‐mobility transistors (HEMTs) is proposed in this article. Electrons limited in the potential well are derived from ionized donor‐like surface states of the AlxGa1−xN layer. Accumulated 2D electron gases (2DEGs) and positive charges left are equivalent to planar plate capacitors and further form electric fields, weakening the polarization fields in barrier layers. The physical properties of the dual‐channel HEMT are considered holistically rather than two separate and independent single heterojunctions. The effect of the charges and 2DEGs distributed in lower layers on the upper channel is contained in our model as well. Subsequently, a drain–source current model is proposed through coupling the critical electric field with the threshold voltage (VTH). The influence of channel length modulation, short channel effect, self‐heating effect, and kink effect is involved in this model. The accuracy of the proposed models is verified by comparison with technology computer‐aided design simulations and the experimental results. Proposed models can greatly describe the output characteristics, the transmission characteristics, and the relationship between VTH and device parameters of double‐channel AlGaN/GaN HEMTs.

Alloy distribution and compositional metrology of epitaxial ScAlN by atom probe tomography

The properties of ScAlN layers grown by molecular beam epitaxy have been carefully studied using atom probe tomography (APT) and complementary techniques. The measured III-site fraction within the ScxAl1−xN layer is x = 0.16 ± 0.02, in good agreement with the values determined by x-ray photoelectron spectroscopy (XPS, x = 0.14) and secondary ion mass spectrometry (SIMS, x = 0.14). The frequency distribution analysis indicates that the compound behaves as a random alloy. A significant amount of oxygen, around 0.2% in site fraction, is found within the ScAlN layer as a randomly distributed impurity. The alloy composition measurement in terms of Sc fraction is rather independent of the surface electric field, which excludes compositional inaccuracies for the experimental parameters used in the APT analysis.

Structural and optical properties of composition-graded InGaN nanowires

At the moment, InGaN ternary compounds are of a great interest for the development of devices for sunlight driven water splitting. However, the synthesis of such materials is hindered by the fact that InxGa1–xN layers are susceptible to phase decomposition at x from 20 to 80%. Nanowires can be a promising solution to this problem. The purpose of our study was to analyze the structural and optical properties of InxGa1–xN nanowires with a gradient x content being inside the miscibility gap. InxGa1–xN nanowires were grown on silicon substrates using plasma-assisted molecular beam epitaxy. The structural properties of nanowires were studied using scanning and transmission electron microscopy. The chemical composition and optical properties of nanowires were analyzed using energy-dispersive microanalysis and photoluminescence spectroscopy. It was shown for the first time that the composition-graded InxGa1–xN nanowires with x from 40 to 60% can be grown using plasma-assisted molecular beam epitaxy. The grown samples exhibit photoluminescence at room temperature with a maximum at about 890 nm, which corresponds to an In content of about 62% according to the modified Vegard’s rule and the transmission electron microscopy data. The obtained results can be of practical interest for the development of devices for water splitting induced by sunlight or sources of near IR radiation

Microstructural characterization of AlxGa1−xN/GaN high electron mobility transistor layers on 200 mm Si(111) substrates

Realization of high crystal quality GaN layers on silicon substrates requires a great control over epitaxy as well as detailed characterization of the buried defects and propagating dislocations within the epilayers. In this Letter, we present the microstructural characterization of AlxGa1−xN/GaN high electron mobility transistor (HEMT) structures epitaxially grown on 200 mm Si (111) substrates with superlattice (SL) buffers. The HEMT stack is also composed of an intermediate thick AlxGa1−xN layer sandwiched between the short-period and long-period AlxGa1−xN/AlN SLs. Structural and morphological characteristics of the GaN-based epilayers are studied to assess the quality of the HEMT stack grown on such 200 mm diameter substrates. The detailed microstructural uniformity of the epilayers is addressed by the transmission electron microscopy (TEM) technique. In depth scanning TEM with electron energy loss spectroscopy (EELS) investigations have been carried out to probe the microstructural quality of the HEMT stack comprising of such short- and long-period AlxGa1−xN/AlN SLs. The EELS-plasmon maps are utilized to address the sharp interface characteristics of the SL layers as well as the top active p-GaN/AlxGa1−xN/GaN layers. This work highlights the capability of high-resolution TEM as a complementing characterization method to produce reliable AlxGa1−xN/GaN HEMTs on such a large diameter silicon substrate.

Nucleation control of high crystal quality heteroepitaxial Sc0.4Al0.6N grown by molecular beam epitaxy

High ScN fraction ScxAl1−xN has promise in important application areas including wide bandwidth RF resonators and filters, and ferroelectric devices such as non-volatile memory, but demands high crystal quality. In this work, the role of the nucleation layer (NL), ScxAl1−xN growth temperature, and strain management to preserve the wurtzite crystal structure are investigated to maximize both acoustoelectric and ferroelectric material properties for high ScN fraction ScxAl1−xN grown on SiC substrates. A 5 nm AlN nucleation layer reduces the x-ray diffraction 0002 reflection full width at half maximum (FWHM) for a Sc0.32Al0.68N film by almost a factor of 2, and reducing the growth temperature to 430 °C enables a Sc0.40Al0.60N film with a FWHM of 4100 arcsec (1.1°) while being only 150 nm thick. Grading the initial ScxAl1−xN layer from x = 0.32 to 0.40 suppresses the formation of rock-salt grain nucleation at the Sc0.40Al0.60N lower interface and reduces the anomalously oriented grain density by an order of magnitude. Increasing the total ScxAl1−xN growth thickness to 500 nm produces an average x = 0.39 ScxAl1−xN layer with a FWHM of 3190 arcsec (0.89°) and an anomalously oriented grain areal fill factor of 1.0%. These methods enable the lowest heteroepitaxial ScxAl1−xN FWHM reported for x ∼ 0.4, with layer thicknesses and defect densities appropriate for high frequency (>10 GHz) filter applications.

Thermal conductivity of ScxAl1−xN and YxAl1−xN alloys

Owing to their very large piezoelectric coefficients and spontaneous polarizations, (Sc,Y)xAl1−xN alloys have emerged as a new class of III-nitride semiconductor materials with great potential for high-frequency electronic and acoustic devices. The thermal conductivity of constituent materials is a key parameter for design, optimization, and thermal management of such devices. In this study, transient thermoreflectance technique is applied to measure the thermal conductivity of ScxAl1−xN and YxAl1−xN (0 ≤x ≤0.22) layers grown by magnetron sputter epitaxy in the temperature range of 100–400 K. The room-temperature thermal conductivity of both alloys is found to decrease significantly with increasing Sc(Y) composition compared to that of AlN. We also found that the thermal conductivity of YxAl1−xN is lower than that of ScxAl1−xN for all studied compositions. In both alloys, the thermal conductivity increases with the temperature up to 250 K and then saturates. The experimental data are analyzed using a model based on the solution of the phonon Boltzmann transport equation within the relaxation time approximation. The contributions of different phonon-scattering mechanisms to the lattice thermal conductivity of (Sc,Y)xAl1−xN alloys are identified and discussed.

Lattice parameters of ScxAl1−xN layers grown on GaN(0001) by plasma-assisted molecular beam epitaxy

An accurate knowledge of lattice parameters of ScxAl1−xN is essential for understanding the elastic and piezoelectric properties of this compound as well as for the ability to engineer its strain state in heterostructures. Using high-resolution x-ray diffractometry, we determine the lattice parameters of 100-nm-thick undoped ScxAl1−xN layers grown on GaN(0001) templates by plasma-assisted molecular beam epitaxy. The Sc content x of the layers is measured independently by both x-ray photoelectron spectroscopy and energy-dispersive x-ray spectroscopy, and it ranges from 0 to 0.25. The in-plane lattice parameter of the layers linearly increases with increasing x, while their out-of-plane lattice parameter remains constant. Layers with x≈0.09 are found to be lattice matched to GaN, resulting in a smooth surface and a structural perfection equivalent to that of the GaN underlayer. In addition, a two-dimensional electron gas is induced at the ScxAl1−xN/GaN heterointerface, with the highest sheet electron density and mobility observed for lattice-matched conditions.

High performance foreign-dopant-free ZnO/AlxGa1−xN ultraviolet phototransistors using atomic-layer-deposited ZnO emitter layer

High-performance foreign-dopant-free ZnO/AlxGa1−xN heterojunction ultraviolet (UV) phototransistors were fabricated and characterized. The ZnO layer with high electron concentration was grown as emitter by atomic layer deposition, while the AlxGa1−xN/GaN heterostructure was epitaxied as base and collector by metal organic chemical vapor deposition. A linearly upgraded/downgraded AlxGa1−xN layer was used as polarization-induced n/p type layer without dopant. The prominent feature of the resulting n+-p-n ZnO/AlxGa1−xN phototransistors is a three-stage rising spectral response matching the biological action spectrum of solar UV radiation. Moreover, the phototransistors demonstrate a low dark current of less than 1 pA at 2 V, a maximum responsivity of ∼8.7 A/W at 5 V and 300 nm, a normalized detectivity of ∼1 × 1013 Jones, and a high response speed with a rise/fall time of 3.5 μs/450 μs. This work shows a feasible and simple-process approach for developing high-performance multiband spectral response photodetectors based on different wide band gap material systems.

Comparison of the Material Quality of AlxIn1-xN (x-0-0.50) Films Deposited on Si(100) and Si(111) at Low Temperature by Reactive RF Sputtering.

AlxIn1−xN ternary semiconductors have attracted much interest for application in photovoltaic devices. Here, we compare the material quality of AlxIn1−xN layers deposited on Si with different crystallographic orientations, (100) and (111), via radio-frequency (RF) sputtering. To modulate their Al content, the Al RF power was varied from 0 to 225 W, whereas the In RF power and deposition temperature were fixed at 30 W and 300 °C, respectively. X-ray diffraction measurements reveal a c-axis-oriented wurtzite structure with no phase separation regardless of the Al content (x = 0–0.50), which increases with the Al power supply. The surface morphology of the AlxIn1−xN layers improves with increasing Al content (the root-mean-square roughness decreases from ≈12 to 2.5 nm), and it is similar for samples grown on both Si substrates. The amorphous layer (~2.5 nm thick) found at the interface with the substrates explains the weak influence of their orientation on the properties of the AlxIn1−xN films. Simultaneously grown AlxIn1−xN-on-sapphire samples point to a residual n-type carrier concentration in the 1020–1021 cm−3 range. The optical band gap energy of these layers evolves from 1.75 to 2.56 eV with the increase in the Al. PL measurements of AlxIn1−xN show a blue shift in the peak emission when adding the Al, as expected. We also observe an increase in the FWHM of the main peak and a decrease in the integrated emission with the Al content in room-temperature PL measurements. In general, the material quality of the AlxIn1-xN films on Si is similar for both crystallographic orientations.

Assessing the Impact of Secondary Fluorescence on X-Ray Microanalysis Results from Semiconductor Thin Films.

The impact of secondary fluorescence on the material compositions measured by X-ray analysis for layered semiconductor thin films is assessed using simulations performed by the DTSA-II and CalcZAF software tools. Three technologically important examples are investigated: AlxGa1−xN layers on either GaN or AlN substrates, InxAl1−xN on GaN, and Si-doped (SnxGa1−x)2O3 on Si. Trends in the differences caused by secondary fluorescence are explained in terms of the propensity of different elements to reabsorb either characteristic or bremsstrahlung X-rays and then to re-emit the characteristic X-rays used to determine composition of the layer under investigation. Under typical beam conditions (7–12 keV), the quantification of dopants/trace elements is found to be susceptible to secondary fluorescence and care must be taken to prevent erroneous results. The overall impact on major constituents is shown to be very small with a change of approximately 0.07 molar cation percent for Al0.3Ga0.7N/AlN layers and a maximum change of 0.08 at% in the Si content of (SnxGa1−x)2O3/Si layers. This provides confidence that previously reported wavelength-dispersive X-ray compositions are not compromised by secondary fluorescence.

Polarization doping—Ab initio verification of the concept: Charge conservation and nonlocality

In this work, we study the emergence of polarization doping in AlxGa1−xN layers with graded composition from a theoretical viewpoint. It is shown that bulk electric charge density emerges in the graded concentration region. The magnitude of the effect, i.e., the relation between the polarization bulk charge density and the concentration gradient is obtained. The appearance of mobile charge in the wurtzite structure grown along the polar direction was investigated using the combination of ab initio and drift-diffusion models. It was shown that the ab initio results can be recovered precisely by proper parameterization of drift-diffusion representation of the complex nitride system. It was shown that the mobile charge appears due to the increase of the distance between opposite polarization-induced charges. It was demonstrated that, for sufficiently large space distance between polarization charges, the opposite mobile charges are induced. We demonstrate that the charge conservation law applies for fixed and mobile charge separately, leading to nonlocal compensation phenomena involving (i) the bulk fixed and polarization sheet charge at the heterointerfaces and (ii) the mobile band and the defect charge. Therefore, two charge conservation laws are obeyed that induces nonlocality in the system. The magnitude of the effect allows obtaining technically viable mobile charge density for optoelectronic devices without impurity doping (donors or acceptors). Therefore, it provides an additional tool for the device designer, with the potential to attain high conductivities: high carrier concentrations can be obtained even in materials with high dopant ionization energies, and the mobility is not limited by scattering at ionized impurities.

Fully Relaxed, Crack-Free AlGaN with upto 50% Al Composition Grown on Porous GaN Pseudo-Substrate

Fully relaxed, crack free, smooth AlxGa1−xN layers with up to 50% Al composition were demonstrated on pseudo-substrates composed of dense arrays of 10 × 10 µm2 compliant porous GaN-on-porous-GaN tiles. The AlGaN layers were grown in steps for a total of 1.3 µm. The growth conditions necessary to demonstrate high quality films at higher Al compositions also suppressed any sidewall growth.