@article{GabelPickemScheidereretal.2022, author = {Gabel, Judith and Pickem, Matthias and Scheiderer, Philipp and Dudy, Lenart and Leikert, Berengar and Fuchs, Marius and St{\"u}binger, Martin and Schmitt, Matthias and K{\"u}spert, Julia and Sangiovanni, Giorgio and Tomczak, Jan M. and Held, Karsten and Lee, Tien-Lin and Claessen, Ralph and Sing, Michael}, title = {Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen}, series = {Advanced Electronic Materials}, volume = {8}, journal = {Advanced Electronic Materials}, number = {4}, issn = {2199-160X}, doi = {10.1002/aelm.202101006}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-318914}, year = {2022}, abstract = {Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO\(_{3}\) as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which are present even if the films are kept in an ultrahigh vacuum environment and not explicitly exposed to air, are shown to severely affect the intrinsic electronic structure of a transition metal oxide film. Their presence leads to the formation of an electronically dead surface layer but also alters the band filling and the electron correlations in the thin films. These findings highlight that it is important to take into account surface apical oxygen or—mutatis mutandis—the specific oxygen configuration imposed by a capping layer to predict the behavior of ultrathin films of transition metal oxides near the single unit-cell limit.}, language = {en} } @phdthesis{Gabel2019, author = {Gabel, Judith}, title = {Interface Engineering of Functional Oxides: A Photoemission Study}, doi = {10.25972/OPUS-19227}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-192275}, school = {Universit{\"a}t W{\"u}rzburg}, year = {2019}, abstract = {Due to their complex chemical structure transition metal oxides display many fascinating properties which conventional semiconductors lack. For this reason transition metal oxides hold a lot of promise for novel electronic functionalities. Just as in conventional semiconductor heterostructures, the interfaces between different materials play a key role in oxide electronics. The textbook example is the (001) interface between the band insulators LaAlO\(_3\) and SrTiO\(_3\) at which a two-dimensional electron system (2DES) forms. In order to utilize such a 2DES in prospective electronic devices, it is vital that the electronic properties of the interface can be controlled and manipulated at will. Employing photoelectron spectroscopy as well as electronic transport measurements, this thesis examines how such interface engineering can be realized in the case of the LaAlO\(_3\)/SrTiO\(_3\) heterostructure: By photoemission we manage to unambiguously distinguish the different mechanisms by which SrTiO\(_3\) can be doped with electrons. An electronic reconstruction is identified as the driving mechanism to render stoichiometric LaAlO\(_3\)/SrTiO\(_3\) interfaces metallic. The doping of the LaAlO\(_3\)/SrTiO\(_3\) heterointerface can furthermore be finely adjusted by changing the oxygen vacancy \(V_{\mathrm{O}}\) concentration in the heterostructure. Combining intense x-ray irradiation with oxygen dosing, we even achieve control over the \(V_{\mathrm{O}}\) concentration and, consequently, the doping in the photoemission experiment itself. Exploiting this method, we investigate how the band diagram of SrTiO\(_3\)-based heterostructures changes as a function of the \(V_{\mathrm{O}}\) concentration and temperature by hard x-ray photoemission spectroscopy. With the band bending in the SrTiO\(_3\) substrate changing as a function of the \(V_{\mathrm{O}}\) concentration, the interfacial band alignment is found to vary as well. The relative permittivity of the SrTiO\(_3\) substrate and, in particular, its dependence on temperature and electric field is identified as one of the essential parameters determining the electronic interface properties. That is also why the sample temperature affects the charge carrier distribution. The mobile charge carriers are shown to shift toward the SrTiO\(_3\) bulk when the sample temperature is lowered. This effect is, however, only pronounced if the total charge carrier concentration is small. At high charge carrier concentrations the charge carriers are always confined to the interface, independent of the sample temperature. The dependence of the electronic interface properties on the \(V_{\mathrm{O}}\) concentration is also investigated by a complementary method, viz. by electronic transport measurements. These experiments confirm that the mobile charge carrier concentration increases concomitantly to the \(V_{\mathrm{O}}\) concentration. The mobility of the charge carriers changes as well depending on the \(V_{\mathrm{O}}\) concentration. Comparing spectroscopy and transport results, we are able to draw conclusions about the processes limiting the mobility in electronic transport. We furthermore build a memristor device from our LaAlO\(_3\)/SrTiO\(_3\) heterostructures and demonstrate how interface engineering is used in practice in such novel electronic applications. This thesis furthermore investigates how the electronic structure of the 2DES is affected by the interface topology: We show that, akin to the (001) LaAlO\(_3\)/SrTiO\(_3\) heterointerface, an electronic reconstruction also renders the (111) interface between LaAlO\(_3\) and SrTiO\(_3\) metallic. The change in interface topology becomes evident in the Fermi surface of the buried 2DES which is probed by soft x-ray photoemission. Based on the asymmetry in the Fermi surface, we estimate the extension of the conductive layer in the (111)-oriented LaAlO\(_3\)/SrTiO\(_3\) heterostructure. The spectral function measured furthermore identifies the charge carriers at the interface as large polarons.}, subject = {{\"U}bergangsmetalloxide}, language = {en} }