Electron beam techniques have been used to analyze the impact of substrate choice and growth parameters on the compositional and optical properties of tin gallium oxide [(SnxGa1−x)2O3] thin films grown by plasma‐assisted molecular beam epitaxy. Sn incorporation and film quality are found to be highly dependent on growth temperature and substrate material (silicon, sapphire, and bulk Ga2O3) with alloy concentrations varying up to an x value of 0.11. Room temperature cathodoluminescence spectra show the Sn alloying suppressing UV (3.3–3.0 eV), enhancing blue (2.8–2.4 eV), and generating green (2.4–2.0 eV) emission, indicative of the introduction of a high density of gallium vacancies (VGa) and subsequent VGa–Sn complexes. This behavior was further analyzed by mapping composition and luminescence across a cross section. Compared to Ga2O3, the spectral bands show a clear redshift due to bandgap reduction, confirmed by optical transmission measurements. The results show promise that the bandgap of gallium oxide can successfully be reduced through Sn alloying and used for bandgap engineering within UV optoelectronic devices.
Tin-gallium oxide (TGO) epilayers have been characterized through the electron microscopy techniques of wavelength-dispersive X-ray spectroscopy (WDX) and cathodoluminescence. Tin incorporation was found to be highly dependent on growth conditions with (0001)-sapphire and (010)-Ga2O3 substrates enhancing tin incorporation. Cathodoluminescence measurements show that TGO luminescence consists of an enhanced blue emission and quenched UV when compared to Ga2O3.and the onset of new green emission originating from the TGO, further correlated through cross-sectional WDX and cathodoluminescence mapping. As well as luminescence intensity changes TGO films display redshifted luminescence bands associated with a bandgap reduction due to the alloying, confirmed through optical transmission measurements.
We report ultra-high responsivity of epitaxial (SnxGa1−x)2O3 (TGO) Schottky UV-C photodetectors and experimentally identified the source of gain as deep-level defects, supported by first principles calculations. Epitaxial TGO films were grown by plasma-assisted molecular beam epitaxy on (−201) oriented n-type β-Ga2O3 substrates. Fabricated vertical Schottky devices exhibited peak responsivities as high as 3.5 ×104 A/W at −5 V applied bias under 250 nm illumination with sharp cutoff shorter than 280 nm and fast rise/fall time in milliseconds order. Hyperspectral imaging cathodoluminescence (CL) spectra were examined to find the mid-bandgap defects, the source of this high gain. Irrespective of different tin mole fractions, the TGO epilayer exhibited extra CL peaks at the green band (∼2.20 eV) not seen in β-Ga2O3 along with enhancement of the blue emission-band (∼2.64 eV) and suppression of the UV emission-band. Based on hybrid functional calculations of the optical emission expected for defects involving Sn in β-Ga2O3, VGa–Sn complexes are proposed as potential defect origins of the observed green and blue emission-bands. Such complexes behave as acceptors that can efficiently trap photogenerated holes and are predicted to be predominantly responsible for the ultra-high photoconductive gain in the Sn-alloyed Ga2O3 devices by means of thermionic emission and electron tunneling. Regenerating the VGa–Sn defect complexes by optimizing the growth techniques, we have demonstrated a planar Schottky UV-C photodetector of the highest peak responsivity.
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.
Abstract Wavelength-dispersive X-ray (WDX) spectroscopy was used to measure silicon atom concentrations in the range 35–100 ppm [corresponding to (3–9) × 1018 cm−3] in doped AlxGa1–xN films using an electron probe microanalyser also equipped with a cathodoluminescence (CL) spectrometer. Doping with Si is the usual way to produce the n-type conducting layers that are critical in GaN- and AlxGa1–xN-based devices such as LEDs and laser diodes. Previously, we have shown excellent agreement for Mg dopant concentrations in p-GaN measured by WDX with values from the more widely used technique of secondary ion mass spectrometry (SIMS). However, a discrepancy between these methods has been reported when quantifying the n-type dopant, silicon. We identify the cause of discrepancy as inherent sample contamination and propose a way to correct this using a calibration relation. This new approach, using a method combining data derived from SIMS measurements on both GaN and AlxGa1–xN samples, provides the means to measure the Si content in these samples with account taken of variations in the ZAF corrections. This method presents a cost-effective and time-saving way to measure the Si doping and can also benefit from simultaneously measuring other signals, such as CL and electron channeling contrast imaging.
A high figure‐of‐merit UV‐C solar‐blind photodetector (PD) fabricated from thin‐film beta‐gallium oxide (β‐Ga2O3) grown on n‐Si substrates by plasma‐assisted molecular beam epitaxy is demonstrated. Film growth sequences for nucleation of Ga2O3 on (100)‐ and (111)‐oriented Si substrates are developed, and the influence of crucial growth parameters is systematically investigated, namely, substrate temperature, oxygen flow rate, and plasma power on the functional properties of the PDs. The PDs show an ultra‐high responsivity of 837 A W−1 and a fast ON/OFF time below 4 ms at −5 V. In addition, they display strong rectifying properties and a sharp cutoff below 280 nm with the average responsivities between 10 and 80 A W−1, a detectivity on the order of 1010 Jones, and rise/fall times between 4 and 500 ms. High photoconductive gain is likely to be due to the mid‐bandgap donor/acceptor defect levels, including oxygen vacancies in the form of self‐trapped holes. It is demonstrated that these defect levels can be modified by controlling the growth conditions, thereby allowing for tailoring of the PD characteristics for specific applications. The methodology represents a cost‐effective solution over homoepitaxial approaches, with characteristics that meet or exceed those reported previously, offering new possibilities for on‐wafer integration with Si opto‐electronics.
Heterogeneous integration of β-(SnxGa1−x)2O3 (TGO) UV-C photodetectors on silicon substrates by molecular beam epitaxy is demonstrated. Multimodal electron microscopy and spectroscopy techniques reveal a direct correlation between structural, compositional, and optical properties of TGO and the functional properties of the photodetectors. Wavelength dispersive x-ray spectroscopy results accurately determine Sn concentrations (x) in the region of 0.020, and room temperature cathodoluminescence (CL) hyperspectral imaging shows changes in the CL emission intensity in TGO compared with a Ga2O3 sample with no Sn. Alloying Ga2O3 with Sn is shown to quench the red emission and enhance the blue emission. The increase in blue emission corresponds to the rise in VGa-related deep acceptors responsible for the high gain observed in the TGO detectors. A Ga2O3 nucleation layer is shown to improve the TGO surface quality and give better device properties compared to TGO grown directly onto the Si substrate, including a higher specific detectivity on the order of 1012 Jones.
In this work, the growth and conductivity of semipolar AlxGa1−xN:Si with (11-22) orientation are investigated. AlxGa1−xN:Si (x = 0.60 ± 0.03 and x = 0.80 ± 0.02) layers were grown with different SiH4 partial pressures, and the electrical properties were determined using Hall measurements at room temperature. The aluminum mole fraction was measured by wavelength dispersive x-ray spectroscopy and x-ray diffraction, and the Si-concentration was measured by wavelength dispersive x-ray spectroscopy and secondary ion mass spectroscopy. Layer resistivities as low as 0.024 Ω cm for x = 0.6 and 0.042 Ω cm for x = 0.8 were achieved. For both aluminum mole fractions, the resistivity exhibits a minimum with the increasing Si concentration, which can be explained by compensation due to the formation of cation vacancy complexes at high doping levels. The onset of self-compensation occurs at larger estimated Si concentrations for larger Al contents.