TY  - JOUR
A1  - Gabel, Judith
A1  - Pickem, Matthias
A1  - Scheiderer, Philipp
A1  - Dudy, Lenart
A1  - Leikert, Berengar
A1  - Fuchs, Marius
A1  - Stübinger, Martin
A1  - Schmitt, Matthias
A1  - Küspert, Julia
A1  - Sangiovanni, Giorgio
A1  - Tomczak, Jan M.
A1  - Held, Karsten
A1  - Lee, Tien–Lin
A1  - Claessen, Ralph
A1  - Sing, Michael
T1  - Toward Functionalized Ultrathin Oxide Films: The Impact of Surface Apical Oxygen
JF  - Advanced Electronic Materials
N2  - 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.
KW  - transition metal oxides
KW  - correlated oxides
KW  - electronic phase transitions
KW  - photoelectron spectroscopy
KW  - thin films
Y1  - 2022
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-318914
SN  - 2199-160X
VL  - 8
IS  - 4
ER  - 
TY  - JOUR
A1  - Kügel, Jens
A1  - Karolak, Michael
A1  - Krönlein, Andreas
A1  - Serrate, David
A1  - Bode, Matthias
A1  - Sangiovanni, Giorgio
T1  - Reversible magnetic switching of high-spin molecules on a giant Rashba surface
JF  - npj Quantum Materials
N2  - The quantum mechanical screening of a spin via conduction electrons depends sensitively on the environment seen by the magnetic impurity. A high degree of responsiveness can be obtained with metal complexes, as the embedding of a metal ion into an organic molecule prevents intercalation or alloying and allows for a good control by an appropriate choice of the ligands. There are therefore hopes to reach an “on demand” control of the spin state of single molecules adsorbed on substrates. Hitherto one route was to rely on “switchable” molecules with intrinsic bistabilities triggered by external stimuli, such as temperature or light, or on the controlled dosing of chemicals to form reversible bonds. However, these methods constrain the functionality to switchable molecules or depend on access to atoms or molecules. Here, we present a way to induce bistability also in a planar molecule by making use of the environment. We found that the particular “habitat” offered by an antiphase boundary of the Rashba system BiAg2 stabilizes a second structure for manganese phthalocyanine molecules, in which the central Mn ion moves out of the molecular plane. This corresponds to the formation of a large magnetic moment and a concomitant change of the ground state with respect to the conventional adsorption site. The reversible spin switch found here shows how we can not only rearrange electronic levels or lift orbital degeneracies via the substrate, but even sway the effects of many-body interactions in single molecules by acting on their surrounding.
KW  - electronic structure of atoms and molecules
KW  - magnetic properties and materials
KW  - surfaces, interfaces and thin films
Y1  - 2018
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-230866
VL  - 3
ER  -