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Kinetics of charge carrier recombination in beta-Ga2O3 crystals

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 Added by Cuong Ton-That
 Publication date 2020
  fields Physics
and research's language is English




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Cathodoluminescence spectra were measured to determine the characteristics of luminescence bands and carrier dynamics in beta-Ga2O3 bulk single crystals. The CL emission was found to be dominated by a broad UV emission peaked at 3.40 eV, which exhibits strong quenching with increasing temperature; however, its spectral shape and energy position remain virtually unchanged. We observed a super-linear increase of CL intensity with excitation density; this kinetics of carrier recombination can be explained in terms of carrier trapping and charge transfer at Fe impurity centres. The temperature-dependent properties of this UV band are consistent with weakly bound electrons in self-trapped excitons with an activation energy of 48 +/- 10 meV. In addition to the self-trapped exciton emission, a blue luminescence (BL) band is shown to be related to a donor-like defect, which increases significantly in concentration after hydrogen plasma annealing. The point defect responsible for the BL, likely an oxygen vacancy, is strongly coupled to the lattice exhibiting a Huang-Rhys factor of ~ 7.3.



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We derive a dielectric function tensor model approach to render the optical response of monoclinic and triclinic symmetry materials with multiple uncoupled infrared and farinfrared active modes. We apply our model approach to monoclinic $beta$-Ga$_2$O$_3$ single crystal samples. Surfaces cut under different angles from a bulk crystal, (010) and ($bar{2}$01), are investigated by generalized spectroscopic ellipsometry within infrared and farinfrared spectral regions. We determine the frequency dependence of 4 independent $beta$-Ga$_2$O$_3$ Cartesian dielectric function tensor elements by matching large sets of experimental data using a point by point data inversion approach. From matching our monoclinic model to the obtained 4 dielectric function tensor components, we determine all infared and farinfrared active transverse optic phonon modes with $A_u$ and $B_u$ symmetry, and their eigenvectors within the monoclinic lattice. We find excellent agreement between our model results and results of density functional theory calculations. We derive and discuss the frequencies of longitudinal optical phonons in $beta$-Ga$_2$O$_3$. We derive and report density and anisotropic mobility parameters of the free charge carriers within the tin doped crystals. We discuss the occurrence of longitudinal phonon plasmon coupled modes in $beta$-Ga$_2$O$_3$ and provide their frequencies and eigenvectors. We also discuss and present monoclinic dielectric constants for static electric fields and frequencies above the reststrahlen range, and we provide a generalization of the Lyddane-Sachs-Teller relation for monoclinic lattices with infrared and farinfrared active modes. We find that the generalized Lyddane-Sachs-Teller relation is fulfilled excellently for $beta$-Ga$_2$O$_3$.
The effects of hydrogen incorporation into beta-Ga2O3 thin films have been investigated by chemical, electrical and optical characterization techniques. Hydrogen incorporation was achieved by remote plasma doping without any structural alterations of the film; however, X-ray photoemission reveals major changes in the oxygen chemical environment. Depth-resolved cathodoluminescence (CL) reveals that the near-surface region of the H-doped Ga2O3 film exhibits a distinct red luminescence (RL) band at 1.9 eV. The emergence of the H-related RL band is accompanied by an enhancement in the electrical conductivity of the film by an order of magnitude. Temperature-resolved CL points to the formation of abundant H-related donors with a binding energy of 28 +/- 4 meV. The RL emission is attributed to shallow donor-deep acceptor pair recombination, where the acceptor is a VGa-H complex and the shallow donor is interstitial H. The binding energy of the VGa-H complex, based on our experimental considerations, is consistent with the computational results by Varley et al [J. Phys.: Condens. Matter, 23, 334212, 2011].
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