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- ItemEngineering Kitaev exchange in stacked iridate layers: Impact of inter-layer species on in-plane magnetism(Cambridge : Royal Society of Chemistry, 2019) Yadav, R.; Eldeeb, M.S.; Ray, R.; Aswartham, S.; Sturza, M.I.; Nishimoto, S.; Van Den Brink, J.; Hozoi, L.Novel functionalities may be achieved in oxide electronics by appropriate stacking of planar oxide layers of different metallic species, MOp and M′Oq. The simplest mechanism allowing the tailoring of the electronic states and physical properties of such heterostructures is of electrostatic nature - charge imbalance between the M and M′ cations. Here we clarify the effect of interlayer electrostatics on the anisotropic Kitaev exchange in H3LiIr2O6, a recently proposed realization of the Kitaev spin liquid. By quantum chemical calculations, we show that the precise position of H+ cations between magnetically active [LiIr2O6]3- honeycomb-like layers has a strong impact on the magnitude of Kitaev interactions. In particular, it is found that stacking with straight interlayer O-H-O links is detrimental to in-plane Kitaev exchange since coordination by a single H-ion of the O ligand implies an axial Coulomb potential at the O site and unfavorable polarization of the O 2p orbitals mediating the Ir-Ir interactions. Our results therefore provide valuable guidelines for the rational design of Kitaev quantum magnets, indicating unprecedented Kitaev interactions of ≈40 meV if the linear interlayer linkage is removed.
- ItemInvestigating the electrochemical stability of Li7La3Zr2O12 solid electrolytes using field stress experiments(London [u.a.] : RSC, 2021) Smetaczek, Stefan; Pycha, Eva; Ring, Joseph; Siebenhofer, Matthäus; Ganschow, Steffen; Berendts, Stefan; Nenning, Andreas; Kubicek, Markus; Rettenwander, Daniel; Limbeck, Andreas; Fleig, JürgenCubic Li7La3Zr2O12 (LLZO) garnets are among the most promising solid electrolytes for solid-state batteries with the potential to exceed conventional battery concepts in terms of energy density and safety. The electrochemical stability of LLZO is crucial for its application, however, controversial reports in the literature show that it is still an unsettled matter. Here, we investigate the electrochemical stability of LLZO single crystals by applying electric field stress via macro- and microscopic ionically blocking Au electrodes in ambient air. Induced material changes are subsequently probed using various locally resolved analysis techniques, including microelectrode electrochemical impedance spectroscopy (EIS), laser induced breakdown spectroscopy (LIBS), laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), and microfocus X-ray diffraction (XRD). Our experiments indicate that LLZO decomposes at 4.1–4.3 V vs. Li+/Li, leading to the formation of Li-poor phases like La2Zr2O7 beneath the positively polarized electrode. The reaction is still on-going even after several days of polarization, indicating that no blocking interfacial layer is formed. The decomposition can be observed at elevated as well as room temperature and suggests that LLZO is truly not compatible with high voltage cathode materials.
- ItemInvestigation of the strain-sensitive superconducting transition of BaFe1.8Co0.2As2 thin films utilizing piezoelectric substrates(Milton Park : Taylor & Francis, 2014) Trommler, S.; Hänisch, J.; Iida, K.; Kurth, F.; Schultz, L.; Holzapfel, B.; Hühne, R.The preparation of biaxially textured BaFe1.8Co0.2As2 thin films has been optimized on MgO single crystals and transfered to piezoelectric (001) Pb(Mg1/3Nb2/3)0.72Ti0.28O3 substrates. By utilizing the inverse piezoelectric effect the lattice parameter of these substrates can be controlled applying an electric field, leading to a induction of biaxial strain into the superconducting layer. High electric fields were used to achieve a total strain of up to 0.05% at low temperatures. A sharpening of the resistive transition and a shift of about 0.6 K to higher temperatures was found at a compressive strain of 0.035%.
- ItemPhotoelectron holography in strong optical and dc electric fields(Bristol : Institute of Physics Publishing, 2014) Stodolna, A.; Huismans, Y.; Rouzée, A.; Lépine, F.; Vrakking, M.J.J.The application of velocity map imaging for the detection of photoelectrons resulting from atomic or molecular ionization allows the observation of interferometric, and in some cases holographic structures that contain detailed information on the target from which the photoelecrons are extracted. In this contribution we present three recent examples of the use of photoelectron velocity map imaging in experiments where atoms are exposed to strong optical and dc electric fields. We discuss (i) observations of the nodal structure of Stark states of hydrogen measured in a dc electric field, (ii) mid-infrared strong-field ionization of metastable Xe atoms and (iii) the reconstruction of helium electronic wavepackets in an attosecond pump-probe experiment. In each case, the interference between direct and indirect electron pathways, reminiscent of the reference and signal waves in holography, is seen to play an important role.
- ItemSTM induced manipulation of azulene-based molecules and nanostructures: the role of the dipole moment(Cambridge : RSC Publ., 2020) Kühne, Tim; Au-Yeung, Kwan Ho; Eisenhut, Frank; Aiboudi, Oumaima; Ryndyk, Dmitry A.; Cuniberti, Gianaurelio; Lissel, Franziska; Moresco, FrancescaAmong the different mechanisms that can be used to drive a molecule on a surface by the tip of a scanning tunneling microscope at low temperature, we used voltage pulses to move azulene-based single molecules and nanostructures on Au(111). Upon evaporation, the molecules partially cleave and form metallo-organic dimers while single molecules are very scarce, as confirmed by simulations. By applying voltage pulses to the different structures under similar conditions, we observe that only one type of dimer can be controllably driven on the surface, which has the lowest dipole moment of all investigated structures. Experiments under different bias and tip height conditions reveal that the electric field is the main driving force of the directed motion. We discuss the different observed structures and their movement properties with respect to their dipole moment and charge distribution on the surface.
- ItemDeterministic positioning of nanophotonic waveguides around single self-assembled quantum dots(Melville, NY : AIP Publishing, 2020) Pregnolato, T.; Chu, X.-L.; Schröder, T.; Schott, R.; Wieck, A.D.; Ludwig, A.; Lodahl, P.; Rotenberg, N.The capability to embed self-assembled quantum dots (QDs) at predefined positions in nanophotonic structures is key to the development of complex quantum-photonic architectures. Here, we demonstrate that QDs can be deterministically positioned in nanophotonic waveguides by pre-locating QDs relative to a global reference frame using micro-photoluminescence (μPL) spectroscopy. After nanofabrication, μPL images reveal misalignments between the central axis of the waveguide and the embedded QD of only (9 ± 46) nm and (1 ± 33) nm for QDs embedded in undoped and doped membranes, respectively. A priori knowledge of the QD positions allows us to study the spectral changes introduced by nanofabrication. We record average spectral shifts ranging from 0.1 nm to 1.1 nm, indicating that the fabrication-induced shifts can generally be compensated by electrical or thermal tuning of the QDs. Finally, we quantify the effects of the nanofabrication on the polarizability, the permanent dipole moment, and the emission frequency at vanishing electric field of different QD charge states, finding that these changes are constant down to QD-surface separations of only 70 nm. Consequently, our approach deterministically integrates QDs into nanophotonic waveguides whose light-fields contain nanoscale structure and whose group index varies at the nanometer level. © 2020 Author(s).
- ItemPhotoemission electron microscopy of magneto-ionic effects in La0.7Sr0.3MnO3(Melville, NY : AIP Publ., 2020) Wilhelm, Marek; Giesen, Margret; Duchoň, Tomáš; Moors, Marco; Mueller, David N.; Hackl, Johanna; Baeumer, Christoph; Hamed, Mai Hussein; Cao, Lei; Zhang, Hengbo; Petracic, Oleg; Glöß, Maria; Cramm, Stefan; Nemšák, Slavomír; Wiemann, Carsten; Dittmann, Regina; Schneider, Claus M.; Müller, MartinaMagneto-ionic control of magnetism is a promising route toward the realization of non-volatile memory and memristive devices. Magneto-ionic oxides are particularly interesting for this purpose, exhibiting magnetic switching coupled to resistive switching, with the latter emerging as a perturbation of the oxygen vacancy concentration. Here, we report on electric-field-induced magnetic switching in a La0.7Sr0.3MnO3 (LSMO) thin film. Correlating magnetic and chemical information via photoemission electron microscopy, we show that applying a positive voltage perpendicular to the film surface of LSMO results in the change in the valence of the Mn ions accompanied by a metal-to-insulator transition and a loss of magnetic ordering. Importantly, we demonstrate that the voltage amplitude provides granular control of the phenomena, enabling fine-tuning of the surface electronic structure. Our study provides valuable insight into the switching capabilities of LSMO that can be utilized in magneto-ionic devices. © 2020 Author(s).
- ItemEnhancement of switching speed of BiFeO3 capacitors by magnetic fields(New York : American Institute of Physics, 2014) Guo, E.J.; Das, S.; Herklotz, A.The effect of a magnetic field on the ferroelectric switching kinetics of BiFeO3 (BFO) capacitors with La0.8Ca0.2MnO3 (LCMO) bottom electrode and Pt top contact has been investigated. We find a strong dependence of the remnant polarization and coercive field on the magnetic field. The switching time can be systematically tuned by magnetic field and reaches a tenfold reduction around the Curie temperature of LCMO at 4 T. We attribute this behavior to the splitting of the voltage drops across the BFO film and the LCMO bottom electrode, which can be strongly influenced by an external magnetic field due to the magnetoresistance. Further experiments on the BFO capacitors with SrRuO3 bottom electrodes show little magnetic field dependence of ferroelectric switching confirming our interpretation. Our results provide an efficient route to control the ferroelectric switching speed through the magnetic field, implying potential application in multifunctional devices.
- ItemCoupled mechanical oscillator enables precise detection of nanowire flexural vibrations(London : Springer Nature, 2023) Sharma, Maneesha; Sathyadharma Prasad, Aniruddha; Freitag, Norbert H.; Büchner, Bernd; Mühl, ThomasThe field of nanowire (NW) technology represents an exciting and steadily growing research area with applications in ultra-sensitive mass and force sensing. Existing detection methods for NW deflection and oscillation include optical and field emission approaches. However, they are challenging for detecting small diameter NWs because of the heating produced by the laser beam and the impact of the high electric field. Alternatively, the deflection of a NW can be detected indirectly by co-resonantly coupling the NW to a cantilever and measuring it using a scanning probe microscope. Here, we prove experimentally that co-resonantly coupled devices are sensitive to small force derivatives similar to standalone NWs. We detect force derivatives as small as 10−9 N/m with a bandwidth of 1 Hz at room temperature. Furthermore, the measured hybrid vibration modes show clear signatures of avoided crossing. The detection technique presented in this work verifies a major step in boosting NW-based force and mass sensing.
- ItemSurface- and tip-enhanced Raman spectroscopy reveals spin-waves in iron oxide nanoparticles(Cambridge : RSC Publ., 2015) Rodriguez, Raul D.; Sheremet, Evgeniya; Deckert-Gaudig, Tanja; Chaneac, Corinne; Hietschold, Michael; Deckert, Volker; Zahn, Dietrich R. T.Nanomaterials have the remarkable characteristic of displaying physical properties different from their bulk counterparts. An additional degree of complexity and functionality arises when oxide nanoparticles interact with metallic nanostructures. In this context the Raman spectra due to plasmonic enhancement of iron oxide nanocrystals are here reported showing the activation of spin-waves. Iron oxide nanoparticles on gold and silver tips are found to display a band around 1584 cm−1 attributed to a spin-wave magnon mode. This magnon mode is not observed for nanoparticles deposited on silicon (111) or on glass substrates. Metal–nanoparticle interaction and the strongly localized electromagnetic field contribute to the appearance of this mode. The localized excitation that generates this mode is confirmed by tip-enhanced Raman spectroscopy (TERS). The appearance of the spin-waves only when the TERS tip is in close proximity to a nanocrystal edge suggests that the coupling of a localized plasmon with spin-waves arises due to broken symmetry at the nanoparticle border and the additional electric field confinement. Beyond phonon confinement effects previously reported in similar systems, this work offers significant insights on the plasmon-assisted generation and detection of spin-waves optically induced.