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Register a new userA chemical imaging and Nano-ARPES study of well-ordered thermally reduced SrTiO3(100)
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Added by
Emmanouil Frantzeskakis
Publication date
2011
fields
Physics
and research's language is
English
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The structural and electronic properties of thermally reduced SrTiO3(100) single crystals have been investigated using a probe with real- and reciprocal-space sensitivity: a synchrotron radiation microsopic setup which offers the possibility of Scanning Photoemission Microscopy and Angle Resolved Photoelectron Spectroscopy (ARPES) down to the nanometric scale. We have spectroscopically imaged the chemical composition of samples which present reproducible and suitable low-energy electron diffraction patterns after following well-established thermal reduction protocols. At the micrometric scale, Ca-rich areas have been directly imaged using high-energy resolution core level photoemission. Moreover, we have monitored the effect of Ca segregation on different features of the SrTiO3(100) electronic band structure, measuring ARPES inside, outside and at the interface of surface inhomogeneities with the identified Ca-rich areas. In particular, the interaction of Ca with the well-known intragap localized state, previously attributed to oxygen vacancies, has been investigated. Moreover, the combination of direct imaging and spectroscopic techniques with high spatial resolution has clarified the long-standing dilemma related to the bulk or surface character of Ca segregation in SrTiO3. Our results present solid evidence that the penetration depth of Ca segregation is very small. In contrast to what has been previously proposed, the origin of long-range surface reconstructions can unlikely be associated to Ca due to strong local variations of its surface concentration.
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Doped SrTiO3 becomes a metal at extremely low doping concentrations n and is even superconducting with the superconducting transition temperature adopting a dome-like shape with the carrier concentration. It is shown here within the polarizability model that up to a well-defined carrier concentration transverse optic mode softening takes place together with polar nano-domain formation which evidences inhomogeneity and a two-component type behavior with metallicity coexisting with polarity. Beyond this region a conventional metal is formed where superconductivity as well as mode softening is absent. For this regime the effective electron-phonon coupling follows the superconducting transition temperature. Effusion measurements as well as macroscopic and nanoscopic conductivity measurements indicate that the distribution of oxygen vacancies is local and inhomogeneous from which it is concluded that metallicity stems from filaments which are embedded in a polar matrix as long as the carrier concentration is less than the critical one.
We discuss the structural and electronic properties of tetragonal CuO grown on SrTiO3(100) by means of hybrid density functional theory. Our analysis explains the anomalously large Cu-O vertical distance observed in the experiments (~2.7 A) in terms of a peculiar frustration between two competing local Cu-O environments characterized by different in-plane and out-of-plane bond lengths and Cu electronic populations. The proper inclusion of substrate effects is crucial to understand the tetragonal expansion and to reproduce correctly the measured valence band spectrum for a CuO thickness of 3-3.5 unit cells, in agreement with the experimentally estimated thickness.
The two-dimensional electron gas (2DEG) at oxides interfaces and surfaces has attracted large attention in physics and research due to its unique electronic properties and possible application in optoelectronics and nanoelectronics. The origin of 2DEGes at oxide interfaces has been attributed to the well known polar catastrophe mechanism. On the other hand, recently a 2DEG was also found on a clean SrTiO3(001) surface where it is formed due to oxygen vacancies. However, these 2DEG systems have been until now found mostly on atomically perfect crystalline samples usually grown by pulsed laser deposition or molecular beam epitaxy i.e. samples which are difficult to be prepared and require specific experimental conditions. Here, we report on the fabrication of SrTiO3 thin films deposited by magnetron sputtering which is suitable for mass-production of samples adapted for nanoelectronic applications. The characterization of their structural and electronic properties was done and compared to those of SrTiO3 single crystals. XRD patterns and SEM micrography show that the deposited films are amorphous and their structure changes to polycrystalline by heating them at 900 {deg}C. Photoemission spectroscopy (XPS and UPS) was used to study the electronic properties of the films and the crystal. In both, we observe the 2DEG system at Fermi level and the formation of Ti3+ states after heating the surface at 900 {deg}C.
The release process for the fabrication of freestanding oxide microstructures relies on appropriate, controllable and repeatable wet etching procedures. SrTiO3 is among the most employed substrates for oxide thin films growth and can be decomposed in HF:water solution. Such process is strongly anisotropic and is affected by local defects and substrate cut-plane. We analyze the etching behavior of SrTiO3 substrates having (100), (110), and (111) cut-planes during immersion in a 5% HF:water solution. The etching process over the three substrates is compared in terms of pitting, anisotropy, macroscopic etch rate and underetching effects around HF-resistant (La,Sr)MnO3 thin film micropatterns. The release of targeted structures, such as the reported (La,Sr)MnO3 freestanding microbridges, depends on the substrate crystallographic symmetry and on the in-plane orientation of the structures themselves along the planar directions. By comparing the etching evolution at two different length scales, we distinguish two regimes for the propagation of the etching front: an intrinsic one, owning to a specific lattice direction, and a macroscopic one, resulting from the mixing of different etching fronts. We report the morphologies of the etched SrTiO3 surfaces and the geometries of the underetched regions as well as of the microbridge clamping zones. The reported analysis will enable the design of complex MEMS devices by allowing to model the evolution of the etching process required for the release of arbitrary structures made of oxide thin films deposited on top of STO.
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