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Instruments / Technical Area	Publication Details	Published
I09-Surface and Interface Structural Analysis	Toward functionalized ultrathin oxide films: the impact of surface apical oxygen Judith Gabel , Matthias Pickem , Philipp Scheiderer , Lenart Dudy , Berengar Leikert , Marius Fuchs , Martin Stübinger , Matthias Schmitt , Julia Kuespert , Giorgio Sangiovanni , Jan M. Tomczak , Karsten Held , Tien-Lin Lee , Ralph Claessen , Michael Sing Advanced Electronic Materials 102 DOI: 10.1002/aelm.202101006 Diamond Proposal Number(s): [23737, 25151] Open Access Show Abstract ▼ 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 SrVO3 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.	Dec 2021
I09-Surface and Interface Structural Analysis	Hard x-ray photoemission spectroscopy of LaVO3/SrTiO3 : Band alignment and electronic reconstruction M. Stübinger , J. Gabel , Philipp Scheiderer , M. Zapf , M. Schmitt , P. Schütz , B. Leikert , J. Küspert , M. Kamp , P. K. Thakur , T.-L. Lee , P. Potapov , A. Lubk , B. Büchner , M. Sing , R. Claessen Physical Review B 103 DOI: 10.1103/PhysRevB.103.235128 Diamond Proposal Number(s): [17499, 23737] Show Abstract ▼ Abstract: A heterostructure consisting of the Mott insulator LaVO3 and the band insulator SrTiO3 is considered a promising candidate for future photovoltaic applications. Not only does the (direct) excitation gap of LaVO3 match well the solar spectrum, but its correlated nature and predicted built-in potential, owing to the nonpolar/polar interface when integrated with SrTiO3, also offer remarkable advantages over conventional solar cells. However, experimental data beyond the observation of a thickness-dependent metal-insulator transition are scarce and a profound, microscopic understanding of the electronic properties is still lacking. By means of soft and hard x-ray photoemission spectroscopy as well as resistivity and Hall effect measurements we study the electrical properties, band bending, and band alignment of LaVO3/SrTiO3 heterostructures. We find a critical LaVO3 thickness of five unit cells, confinement of the conducting electrons to exclusively Ti 3d states at the interface, and a potential gradient in the film. From these findings we conclude on electronic reconstruction as the driving mechanism for the formation of the metallic interface in LaVO3/SrTiO3.	Jun 2021
I09-Surface and Interface Structural Analysis	Controlling the electronic interface properties of AlOx / SrTiO3 heterostructures Berengar Leikert , Judith Gabel , Matthias Schmitt , Martin Stuebinger , Philipp Scheiderer , Louis Veyrat , Tien-Lin Lee , Michael Sing , Ralph Claessen Physical Review Materials 5 DOI: 10.1103/PhysRevMaterials.5.065003 Diamond Proposal Number(s): [15856] Show Abstract ▼ Abstract: Depositing disordered Al on top of Sr Ti O 3 is a cheap and easy way to create a two-dimensional electron system in the Sr Ti O 3 surface layers. To facilitate future device applications, we passivate the heterostructure by a disordered La Al O 3 capping layer to study the electronic properties by complementary x-ray photoemission spectroscopy and transport measurements on the very same samples. We also tune the electronic interface properties by adjusting the oxygen pressure during film growth.	Jun 2021
I09-Surface and Interface Structural Analysis	Tailoring materials for Mottronics: Excess oxygen doping of a prototypical Mott insulator Philipp Scheiderer , Matthias Schmitt , Judith Gabel , Michael Zapf , Martin Stuebinger , Philipp Schütz , Lenart Dudy , Christoph Schlueter , Tien-Lin Lee , Michael Sing , Ralph Claessen Advanced Materials 327 DOI: 10.1002/adma.201706708 Diamond Proposal Number(s): [14106, 15200, 15856, 18372] Show Abstract ▼ Abstract: The Mott transistor is a paradigm for a new class of electronic devices—often referred to by the term Mottronics—which are based on charge correlations between the electrons. Since correlation‐induced insulating phases of most oxide compounds are usually very robust, new methods have to be developed to push such materials right to the boundary to the metallic phase in order to enable the metal–insulator transition to be switched by electric gating. Here, it is demonstrated that thin films of the prototypical Mott insulator LaTiO3 grown by pulsed laser deposition under oxygen atmosphere are readily tuned by excess oxygen doping across the line of the band‐filling controlled Mott transition in the electronic phase diagram. The detected insulator to metal transition is characterized by a strong change in resistivity of several orders of magnitude. The use of suitable substrates and capping layers to inhibit oxygen diffusion facilitates full control of the oxygen content and renders the films stable against exposure to ambient conditions. These achievements represent a significant advancement in control and tuning of the electronic properties of LaTiO3+x thin films making it a promising channel material in future Mottronic devices.	May 2018
	In situ control of separate electronic phases on SrTiO3 surfaces by oxygen dosing Lenart Dudy , Michael Sing , Philipp Scheiderer , Jonathan D. Denlinger , Philipp Schütz , Judith Gabel , Mathias Buchwald , Christoph Schlueter , Tien-Lin Lee , Ralph Claessen Advanced Materials 28, 7443 - 7449 DOI: 10.1002/adma.201600046 Show Abstract ▼ Abstract: Insulating SrTiO3 (STO) can host 2D electron systems (2DESs) on its surfaces, caused by oxygen defects. This study shows that the STO surface exhibits phase separation once the 2DES is formed and relates this inhomogeneity to recently reported magnetic order at STO surfaces and interfaces. The results open pathways to exploit oxygen defects for engineering the electronic and magnetic properties of oxides.	Sep 2016

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