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Modulation-Doped SrTiO3/SrTi1-xZrxO3 Heterostructures


Two-dimensional electron gases (2DEGs) in SrTiO3 have attracted considerable attention for exhibiting a variety of interesting physical phenomena, such as superconductivity and magnetism. So far, most of the literature has focused on interfaces between nonpolar SrTiO3 and polar perovskite oxides (e.g. LaAlO3 or rare-earth titanates), where high carrier density 2DEGs (~3 × 1014 cm-2) are generated by polar discontinuity. Modulation doping is an alternative approach to generating a 2DEG that has been explored extensively in III-V semiconductors but has not heretofore been explored in complex oxides. This approach involves interfacing an undoped semiconductor with a doped semiconductor whose conduction band edge lies at a higher energy, which results in electrons diffusing into the undoped semiconductor transport channel, where scattering from ionized dopants is minimized. Realizing a high-mobility modulation-doped structure with a SrTiO3 transport channel therefore requires both the optimization of the transport channel by minimizing native defects as well as the development of a perovskite oxide which has a suitable band offset with SrTiO3 and can be electron-doped.

The growth of high electron mobility SrTiO3 as a suitable transport channel material was previously demonstrated using the hybrid molecular beam epitaxy (MBE) approach, where Sr is delivered via a solid source and Ti is delivered using a metal-organic precursor, titanium (IV) tetra-isopropoxide (TTIP). Expanding on this, in-situ reflection high-energy electron diffraction (RHEED) is used to track the surface and resulting film cation stoichiometry of homoepitaxial SrTiO3 (001) thin films grown by hybrid MBE. It is shown that films with lattice parameters identical to bulk single-crystal substrates within the detection limit of high-resolution X-ray diffraction (XRD) measurements exhibit an evolution in surface reconstruction with increasing TTIP beam-equivalent pressure. The change in the observed surface reconstruction from (1×1) to (2×1) to c(4×4) is correlated with a change from mixed SrO/TiO2 to pure TiO2 surface termination. It is argued that optimal cation stoichiometry is achieved for growth conditions within the XRD-defined growth window that result in a c(4×4) surface lattice.

The development of a doped perovskite oxide semiconductor with a suitable conduction band offset is then discussed as the next necessary step towards realizing modulation-doped heterostructures. The SrTixZr1-xO3 solid solution is investigated for this purpose, with a focus on optimizing cation stoichiometry to allow for controlled doping. In particular, the hybrid MBE growth of SrTixZr1-xO3 thin films is explored using a metal-organic precursor for Zr, zirconium tert-butoxide (ZTB). The successful generation of 2DEGs by modulation doping of SrTiO3 is then demonstrated in SrTiO3/La:SrTi0.95Zr0.05O3 heterostructures, and the electronic structure is studied by Shubnikov-de Haas analysis using multiple-subband models.

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