Quaternary BeMgZnO by plasma-enhanced molecular beam epitaxy for BeMgZnO/ZnO heterostructure devices

We investigated the crystal structure, growth kinetics and electrical properties of BeMgZnO/ZnO heterostructures grown by Molecular Beam Epitaxy (MBE). Transmission Electron Microscopy (TEM) studies revealed that incorporation of Mg into the BeZnO solid solution eliminates the high angle grain boundaries that are the major structural defects in ternary BeZnO. The significant improvement of x-ray diffraction intensity from quaternary BeMgZnO alloy compared to ternary BeZnO was attributed to the reduction of lattice strain, which is present in the latter due to the large difference of covalent radii between Be and Zn (1.22 Å for Zn, 0.96 Å for Be). Incorporation of Mg, which has a larger covalent radius of 1.41Å, reduced the strain in BeMgZnO thin films and also enhanced Be incorporation on lattice sites in the wurtzite lattice. The Zn/(Be + Mg) ratio necessary to obtain single-crystal O-polar BeMgZnO on (0001) GaN/sapphire templates was found to increase with increasing substrate temperature:3.9, 6.2, and 8.3 at substrate temperatures of 450°C, 475°C, and 500°C, respectively. Based on analysis of photoluminescence spectra from Be0.03MgyZn0.97-yO and evolution of reflection high-energy electron diffraction patterns observed in situ during the MBE growth, it has been deduced that more negative formation enthalpy of MgO compared to ZnO and the increased surface mobility of Mg adatoms at elevated substrate temperatures give rise to the nucleation of a MgO-rich wurtzite phase at relatively low Zn/(Be + Mg) ratios. We have demonstrated both theoretically and experimentally that the incorporation of Be into the barrier in Zn-polar BeMgZnO/ZnO and O-polar ZnO/BeMgZnO polarization doped heterostructures allows the alignment of piezoelectric polarization vector with that of spontaneous polarization due to the change of strain sign, thus increasing the amount of net polarization. This made it possible to achieve Zn-polar BeMgZnO/ZnO heterostructures grown on GaN/sapphire templates with two-dimensional electron gas densities substantially exceeding those in Zn-polar MgZnO/ZnO and O-polar ZnO/MgZnO heterostructures with similar Mg content.

[1]  S. Chichibu,et al.  Structural, elastic, and polarization parameters and band structures of wurtzite ZnO and MgO , 2012 .

[2]  E. Segnit,et al.  The System MgO‐ZnO‐SiO2 , 1965 .

[3]  Akira Ohtomo,et al.  MgxZn1−xO as a II–VI widegap semiconductor alloy , 1998 .

[4]  H. Morkoç,et al.  Zinc Oxide: Fundamentals, Materials and Device Technology , 2009 .

[5]  Challenges and opportunities of ZnO-related single crystalline heterostructures , 2013, 1311.5088.

[6]  W. Fan,et al.  Electronic structures of wurtzite ZnO, BeO, MgO and p-type doping in Zn1−xYxO (Y = Mg, Be) , 2008 .

[7]  Xingzhong Cao,et al.  Effects of the oxygen pressure on the structural and optical properties of ZnBeMgO films prepared by pulsed laser deposition , 2010 .

[8]  Takafumi Yao,et al.  Control of crystal polarity in a wurtzite crystal: ZnO films grown by plasma-assisted molecular-beam epitaxy on GaN , 2002 .

[9]  Mitsuaki Yano,et al.  Molecular beam epitaxial growth of wide bandgap ZnMgO alloy films on (111)-oriented si substrate toward UV-detector applications , 2005 .

[10]  B. Pan,et al.  Wide range bandgap modulation based on ZnO-based alloys and fabrication of solar blind UV detectors with high rejection ratio. , 2014, ACS applied materials & interfaces.

[11]  Y Zhang,et al.  ZnO based oxide system with continuous bandgap modulation from 3.7 to 4.9 eV , 2008 .

[12]  Zhigang Yin,et al.  Applications of ZnO in organic and hybrid solar cells , 2011 .

[13]  Y. Uetsuji,et al.  Polarization-induced two-dimensional electron gas at Zn1−xMgxO/ZnO heterointerface , 2007 .

[14]  Benjamin J. Norris,et al.  ZnO-based transparent thin-film transistors , 2003 .

[15]  W. C. Walker,et al.  Electronic spectrum of crystalline beryllium oxide , 1969 .

[16]  H. Morkoç,et al.  A COMPREHENSIVE REVIEW OF ZNO MATERIALS AND DEVICES , 2005 .

[17]  Z. Mei,et al.  Controlled Growth of High‐Quality ZnO‐Based Films and Fabrication of Visible‐Blind and Solar‐Blind Ultra‐Violet Detectors , 2009 .

[18]  Lester F. Eastman,et al.  Two-dimensional electron gases induced by spontaneous and piezoelectric polarization charges in N- and Ga-face AlGaN/GaN heterostructures , 1999 .

[19]  Beatriz Cordero,et al.  Covalent radii revisited. , 2008, Dalton transactions.

[20]  Jenshan Lin,et al.  Hydrogen-selective sensing at room temperature with ZnO nanorods , 2005 .

[21]  Min Han,et al.  Wide-band gap oxide alloy: BeZnO , 2006 .

[22]  T. Hanada Basic Properties of ZnO, GaN, and Related Materials , 2009 .

[23]  H. Morkoç,et al.  Enhancement of Be and Mg incorporation in wurtzite quaternary BeMgZnO alloys with up to 5.1 eV optical bandgap , 2014 .

[24]  John F. Muth,et al.  Optical and Structural Properties of Epitaxial MgxZn1-xO Alloys , 1999 .

[25]  B. Pan,et al.  Formation behavior of BexZn1−xO alloys grown by plasma-assisted molecular beam epitaxy , 2013 .

[26]  Robert M. Hazen,et al.  High‐pressure and high‐temperature crystal chemistry of beryllium oxide , 1986 .

[27]  Lattice parameters and electronic structure of BeMgZnO quaternary solid solutions: Experiment and theory , 2016 .

[28]  Atsuo Yamada,et al.  Polarization-induced two-dimensional electron gases in ZnMgO/ZnO heterostructures , 2008 .

[29]  Priya Gopal,et al.  Polarization, piezoelectric constants, and elastic constants of ZnO, MgO, and CdO , 2005, cond-mat/0507217.

[30]  Effect of oxygen-to-metal flux ratio on incorporation of metal species into quaternary BeMgZnO grown by plasma-assisted molecular beam epitaxy , 2017 .

[31]  Zikang Tang,et al.  Temperature-dependent structural relaxation of BeZnO alloys , 2013 .

[32]  Solar-blind wurtzite MgZnO alloy films stabilized by Be doping , 2013 .

[33]  Tanner A. Nakagawara,et al.  Growth kinetics of O-polar BexMgyZn1-x-yO alloy: Role of Zn to Be and Mg flux ratio as a guide to growth at high temperature , 2017 .

[34]  H. Morkoç,et al.  Polarity control and residual strain in ZnO epilayers grown by molecular beam epitaxy on (0001) GaN/sapphire , 2016 .

[35]  Hadis Morkoç,et al.  Exciton localization and large Stokes shift in quaternary BeMgZnO grown by molecular beam epitaxy , 2016, SPIE OPTO.