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Register a new userUltrafast Dynamics of Gallium Vacancy Charge States in $beta$-Ga$_2$O$_3$
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Point defects in crystalline materials often occur in multiple charge states. Although many experimental methods to study and explore point defects are available, techniques to explore the non-equilibrium dynamics of the charge states of these defects at ultrafast (sub-nanosecond) time scales have not been discussed before. We present results from ultrafast optical-pump supercontinuum-probe spectroscopy measurements on $beta$-Ga$_2$O$_3$. The study of point defects in $beta$-Ga$_2$O$_3$ is essential for its establishment as a material platform for high-power electronics and deep-UV optoelectronics. Use of a supercontinuum probe allows us to obtain the time-resolved absorption spectra of material defects under non-equilibrium conditions with picosecond time resolution. The probe absorption spectra shows defect absorption peaks at two energies, $sim$2.2 eV and $sim$1.63 eV, within the 1.3-2.5 eV probe energy bandwidth. The strength of the absorption associated with each peak is time-dependent and the spectral weight shifts from the lower energy peak to the higher energy peak with pump-probe delay. Further, maximum defect absorption is seen for probe polarized along the crystal c-axis. The time-dependent probe absorption spectra and the observed dynamics for all probe wavelengths at all pump-probe delays can be fit with a set of rate equations for a single multi-level defect. Based on first-principles calculations within hybrid density functional theory we attribute the observed absorption features to optical transitions from the valence band to different charge states of Gallium vacancies. Our results demonstrate that broadband ultrafast supercontinuum spectroscopy can be a useful tool to explore charge states of defects and defect dynamics in semiconductors.
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We report results from ultrafast two-color optical pump-probe spectroscopy on bulk $beta$-Ga$_2$O$_3$. A two-photon absorption scheme is used to photoexcite carriers with the pump pulse and free-carrier absorption of the probe pulse is used to record the subsequent dynamics of the photoexcited carriers. Our results are consistent with carrier recombination via defect-assisted processes. We also observe transient polarization-selective optical absorption of the probe pulse by defect states under nonequilibrium conditions. A rate equation model for electron and hole capture by defects is proposed and used to explain the data. Whereas the rate constants for electron capture by defects are found to be temperature-independent, they are measured to be strongly temperature-dependent for hole capture and point to a lattice deformation/relaxation process accompanying hole capture. Our results shed light on the mechanisms and rates associated with carrier capture by defects in $beta$-Ga$_2$O$_3$.
$beta$-Ga$_2$O$_3$ is a promising ultra-wide bandgap semiconductor whose properties can be further enhanced by alloying with Al. Here, using atomic-resolution scanning transmission electron microscopy (STEM), we find the thermodynamically-unstable $gamma$-phase is a ubiquitous defect in both $beta$-(Al$_x$Ga$_{1text{-}x}$)$_2$O$_3$ films and doped $beta$-Ga$_2$O$_3$ films grown by molecular beam epitaxy. For undoped $beta$-(Al$_x$Ga$_{1text{-}x}$)$_2$O$_3$ films we observe $gamma$-phase inclusions between nucleating islands of the $beta$-phase at lower growth temperatures (~400-600 $^{circ}$C). In doped $beta$-Ga$_2$O$_3$, a thin layer of the $gamma$-phase is observed on the surfaces of films grown with a wide range of n-type dopants and dopant concentrations. The thickness of the $gamma$-phase layer was most strongly correlated with the growth temperature, peaking at about 600 $^{circ}$C. Ga interstitials are observed in $beta$-phase, especially near the interface with the $gamma$-phase. By imaging the same region of the surface of a Sn-doped $beta$-(Al$_x$Ga$_{1text{-}x}$)$_2$O$_3$ after ex-situ heating up to 400 $^{circ}$C, a $gamma$-phase region is observed to grow above the initial surface, accompanied by a decrease in Ga interstitials in the $beta$-phase. This suggests that the diffusion of Ga interstitials towards the surface is likely the mechanism for growth of the surface $gamma$-phase, and more generally that the more-open $gamma$-phase may offer diffusion pathways to be a kinetically-favored and early-forming phase in the growth of Ga$_2$O$_3$.
Based on first-principles calculations, we show that the maximum reachable concentration $x$ in the (Ga$_{1-x}$In$_x$)$_2$O$_3$ alloy in the low-$x$ regime (i.e. In solubility in $beta$-Ga$_2$O$_3$) is around 10%. We then calculate the band alignment at the (100) interface between $beta$-Ga$_2$O$_3$ and (Ga$_{1-x}$In$_x$)$_2$O$_3$ at 12%, the nearest computationally treatable concentration. The alignment is strongly strain-dependent: it is of type-B staggered when the alloy is epitaxial on Ga$_2$O$_3$, and type-A straddling in a free-standing superlattice. Our results suggest a limited range of applicability of low-In-content GaInO alloys.
Steep-slope $beta$-Ga$_2$O$_3$ nano-membrane negative capacitance field-effect transistors (NC-FETs) are demonstrated with ferroelectric hafnium zirconium oxide in gate dielectric stack. Subthreshold slope less than 60 mV/dec at room temperature is obtained for both forward and reverse gate voltage sweeps with a minimum value of 34.3 mV/dec at reverse gate voltage sweep and 53.1 mV/dec at forward gate voltage sweep at $V_{DS}$=0.5 V. Enhancement-mode operation with threshold voltage ~0.4 V is achieved by tuning the thickness of $beta$-Ga$_2$O$_3$ membrane. Low hysteresis of less than 0.1 V is obtained. The steep-slope, low hysteresis and enhancement-mode $beta$-Ga$_2$O$_3$ NC-FETs are promising as nFET candidate for future wide bandgap CMOS logic applications.
Recent breakthroughs in bulk crystal growth of the thermodynamically stable beta phase of gallium oxide ($beta$-Ga$_2$O$_3$) have led to the commercialization of large-area beta-Ga$_2$O$_3$ substrates with subsequent epitaxy on (010) substrates producing high-quality films. Still, metal-organic chemical vapor deposition (MOCVD), molecular beam epitaxy (MBE), and processing of the (010) $beta$-Ga$_2$O$_3$ surface are known to form sub-nanometer scale facets along the [001] direction as well as larger ridges with features perpendicular to the [001] direction. A density function theory calculation of the (010) surface shows an ordering of the surface as a sub-nanometer-scale feature along the [001] direction. Additionally, the general crystal structure of $beta$-Ga$_2$O$_3$ is presented and recommendations are presented for standardizing (010) substrates to account for and control the larger-scale ridge formation.
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