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- ItemManganese-catalyzed selective C–H activation and deuteration by means of a catalytic transient directing group strategy(London : Royal Society of Chemistry (RSC), 2021) Kopf, Sara; Neumann, Helfried; Beller, MatthiasA novel manganese-catalyzed C-H activation methodology for selective hydrogen isotope exchange of benzaldehydes is presented. Using D2O as a cheap and convenient source of deuterium, the reaction proceeds with excellent functional group tolerance. Highortho-selectivity is achieved in the presence of catalytic amounts of specific amines, whichin situform a transient directing group. © The Royal Society of Chemistry 2021.
- ItemLow-melting manganese(II)-based ionic liquids: Syntheses, structures, properties and influence of trace impurities(Basel : MDPI, 2019) Peppel, Tim; Geppert-Rybczyńska, Monika; Neise, Christin; Kragl, Udo; Köckerling, MartinThe synthesis of more than 10 new magnetic ionic liquids with [MnX4]2− anions, X = Cl, NCS, NCO, is presented. Detailed structural information through single-crystal X-ray diffraction is given for (DMDIm)[Mn(NCS)4], (BnEt3N)2[Mn(NCS)4], and {(Ph3P)2N}2[Mn(NCO4)]·0.6H2O, respectively. All compounds consist of discrete anions and cations with tetrahedrally coordinated Mn(II) atoms. They show paramagnetic behavior as expected for spin-only systems. Melting points are found for several systems below 100 °C classifying them as ionic liquids. Thermal properties are investigated using differential scanning calorimetry (DSC) measurements. The physicochemical properties of density, dynamic viscosity, electrolytic conductivity, and surface tension were measured temperature-dependent of selected samples. These properties are discussed in comparison to similar Co containing systems. An increasing amount of bromide impurity is found to affect the surface tension only up to 3.3%.
- ItemLarge superplastic strain in non-modulated epitaxial Ni-Mn-Ga films(Amsterdam : Elsevier, 2010) Yeduru, S.R.; Backen, A.; Fahler, S.; Schultz, L.; Kohl, M.The phase transformation and superplastic characteristics of free-standing epitaxial Ni-Mn-Ga stripes are reported. The stripes are prepared by micromachining a 1 μm thick Ni-Mn-Ga film sputter-deposited on a single crystalline MgO (100) substrate using optical lithography and a Chromium-based sacrificial layer technology. The stripes are oriented at angles of 0 and 45 degrees with respect to the Ni-Mn-Ga unit cell. Electrical resistance versus temperature characteristics reveal a reversible thermally induced phase transformation between 169°C and 191°C. Stress-strain measurements are performed with the stress applied along the [100]Ni-Mn-Ga as well as [110]Ni-Mn-Ga direction. Depending on the orientation, the twinning stress ranges between 25 and 30 MPa, respectively. For the [100] Ni-Mn-Ga and [110]Ni-Mn-Ga directions, superplastic behaviour with a strain plateau of 12 % and 4% are observed, respectively, indicating stress-induced reorientation of non-modulated martensite variants.
- ItemNanoscale mechanical surface properties of single crystalline martensitic Ni-Mn-Ga ferromagnetic shape memory alloys(Bristol : IOP, 2012) Jakob, A.M.; Müller, M.; Rauschenbach, B.; Mayr, S.G.Located beyond the resolution limit of nanoindentation, contact resonance atomic force microscopy (CR-AFM) is employed for nano-mechanical surface characterization of single crystalline 14M modulated martensitic Ni-Mn-Ga (NMG) thin films grown by magnetron sputter deposition on (001) MgO substrates. Comparing experimental indentation moduli-obtained with CR-AFM-with theoretical predictions based on density functional theory (DFT) indicates the central role of pseudo plasticity and inter-martensitic phase transitions. Spatially highly resolved mechanical imaging enables the visualization of twin boundaries and allows for the assessment of their impact on mechanical behavior at the nanoscale. The CR-AFM technique is also briefly reviewed. Its advantages and drawbacks are carefully addressed.
- ItemSelective Earth-Abundant System for CO2 Reduction: Comparing Photo- and Electrocatalytic Processes(Washington, DC : American Chemical Society, 2019) Steinlechner C.; Roesel A.F.; Oberem E.; Päpcke A.; Rockstroh N.; Gloaguen F.; Lochbrunner S.; Ludwig R.; Spannenberg A.; Junge H.; Francke R.; Beller M.The valorization of CO2 via photo- or electrocatalytic reduction constitutes a promising approach toward the sustainable production of fuels or value-added chemicals using intermittent renewable energy sources. For this purpose, molecular catalysts are generally studied independently with respect to the photo- or the electrochemical application, although a unifying approach would be much more effective with respect to the mechanistic understanding and the catalyst optimization. In this context, we present a combined photo- and electrocatalytic study of three Mn diimine catalysts, which demonstrates the synergistic interplay between the two methods. The photochemical part of our study involves the development of a catalytic system containing a heteroleptic Cu photosensitizer and the sacrificial BIH reagent. The system shows exclusive selectivity for CO generation and renders turnover numbers which are among the highest reported thus far within the group of fully earth-abundant photocatalytic systems. The electrochemical part of our investigations complements the mechanistic understanding of the photochemical process and demonstrates that in the present case the sacrificial reagent, the photosensitizer, and the irradiation source can be replaced by the electrode and a weak Brønsted acid. © 2019 American Chemical Society.
- ItemMagnetically induced reorientation of martensite variants in constrained epitaxial Ni-Mn-Ga films grown on MgO(001)(Milton Park : Taylor & Francis, 2008) Thomas, M.; Heczko, O.; Buschbeck, J.; Rößler, U.K.; McCord, J.; Scheerbaum, N.; Schultz, L.; Fähler, S.Magnetically induced reorientation (MIR) is observed in epitaxial orthorhombic Ni-Mn-Ga films. Ni-Mn-Ga films have been grown epitaxially on heated MgO(001) substrates in the cubic austenite state. The unit cell is rotated by 45° relative to the MgO cell. The growth, structure texture and anisotropic magnetic properties of these films are described. The crystallographic analysis of the martensitic transition reveals variant selection dominated by the substrate constraint. The austenite state has low magnetocrystalline anisotropy. In the martensitic state, the magnetization curves reveal an orthorhombic symmetry having three magnetically non-equivalent axes. The existence of MIR is deduced from the typical hysteresis within the first quadrant in magnetization curves and independently by texture measurement without and in the presence of a magnetic field probing micro structural changes. An analytical model is presented, which describes MIR in films with constrained overall extension by the additional degree of freedom of an orthorhombic structure compared to the tetragonal structure used in the standard model.
- ItemMagnetic field-induced twin boundary motion in polycrystalline Ni-Mn-Ga fibres(Milton Park : Taylor & Francis, 2008) Scheerbaum, N.; Heczko, O.; Liu, J.; Hinz, D.; Schultz, L.; Gutfleisch, O.Magnetic field-induced twin boundary motion leading to large magnetic field-induced strain of ~1.0% was established in polycrystalline Ni50.9Mn27.1Ga22.0 (at.%) fibres at room temperature (~60–100 μm in diameter and ~3 mm in length). The fibres' grains are as large as the fibre diameter and of random orientation. At room temperature, a ferromagnetic 5M martensite is found. Magnetic field-induced twin boundary motion was indicated by magnetic measurements and validated by electron backscatter diffraction (EBSD). The application of a magnetic field shifts the equilibrium temperature of martensite and austenite by ~0.4 K T−1, which agrees with calculations using the Clapeyron–Clausius approach.
- ItemTopological Electronic Structure and Intrinsic Magnetization in MnBi4Te7: A Bi2Te3 Derivative with a Periodic Mn Sublattice(College Park, MD : American Physical Society, 2019) Vidal, R.C.; Zeugner, A.; Facio, J.I.; Ray, R.; Haghighi, M.H.; Wolter, A.U.B.; Corredor, Bohorquez, L.T.; Caglieris, F.; Moser, S.; Figgemeier, T.; Peixoto, T.R.F.; Vasili, H.B.; Valvidares, M.; Jung, S.; Cacho, C.; Alfonsov, A.; Mehlawat, K.; Kataev, V.; Hess, C.; Richter, M.; Büchner, B.; Van Den Brink, J.; Ruck, M.; Reinert, F.; Bentmann, H.; Isaeva, A.Combinations of nontrivial band topology and long-range magnetic order hold promise for realizations of novel spintronic phenomena, such as the quantum anomalous Hall effect and the topological magnetoelectric effect. Following theoretical advances, material candidates are emerging. Yet, so far a compound that combines a band-inverted electronic structure with an intrinsic net magnetization remains unrealized. MnBi2Te4 has been established as the first antiferromagnetic topological insulator and constitutes the progenitor of a modular (Bi2Te3)n(MnBi2Te4) series. Here, for n=1, we confirm a nonstoichiometric composition proximate to MnBi4Te7. We establish an antiferromagnetic state below 13 K followed by a state with a net magnetization and ferromagnetic-like hysteresis below 5 K. Angle-resolved photoemission experiments and density-functional calculations reveal a topologically nontrivial surface state on the MnBi4Te7(0001) surface, analogous to the nonmagnetic parent compound Bi2Te3. Our results establish MnBi4Te7 as the first band-inverted compound with intrinsic net magnetization providing a versatile platform for the realization of magnetic topological states of matter.
- ItemElectronic transitions and dielectric function tensor of a YMnO3 single crystal in the NIR-VUV spectral range(London [u.a.] : Royal Society of Chemistry, 2014) Schmidt-Grund, R.; Richter, S.; Ebbinghaus, S.G.; Lorenz, M.; Bundesmann, C.; Grundmann, M.We present optical properties in the near-infrared to vacuum-ultraviolet spectral range of hexagonal YMnO3. The high-quality (110)-oriented bulk single crystal was grown by the optical floating zone technique. We have determined the tensor of the dielectric function by means of Mueller matrix ellipsometry in the wide spectral range (0.5-9.15) eV. For the spectral range below 5.4 eV, we present much more precise data compared to previous reports. For higher energies no experimental reports were given previously. The experimental dielectric function of YMnO3 agrees generally with theoretical calculations. We found the well known transitions involving hybridized oxygen-Mn states and Mn-3d states to be spectrally localized with a homogeneous Lorentzian lineshape. At energies above these transitions, we observe pseudo-transparent points where for each of the principal diagonal elements of the dielectric function tensor the imaginary part approaches zero but at different photon energies. These are followed at the onset of the high-absorption spectral range by parabolic direct band-band transitions which have not been reported so far.
- ItemTransformation of epitaxial NiMnGa/InGaAs nanomembranes grown on GaAs substrates into freestanding microtubes(Cambridge : Royal Society of Chemistry, 2016) Müller, C.; Neckel, I.; Monecke, M.; Dzhagan, V.; Salvan, G.; Schulze, S.; Baunack, S.; Gemming, T.; Oswald, S.; Engemaiere, V.; Mosca, D.H.We report the fabrication of Ni2.7Mn0.9Ga0.4/InGaAs bilayers on GaAs (001)/InGaAs substrates by molecular beam epitaxy. To form freestanding microtubes the bilayers have been released from the substrate by strain engineering. Microtubes with up to three windings have been successfully realized by tailoring the size and strain of the bilayer. The structure and magnetic properties of both, the initial films and the rolled-up microtubes, are investigated by electron microscopy, X-ray techniques and magnetization measurements. A tetragonal lattice with c/a = 2.03 (film) and c/a = 2.01 (tube) is identified for the Ni2.7Mn0.9Ga0.4 alloy. Furthermore, a significant influence of the cylindrical geometry and strain relaxation induced by roll-up on the magnetic properties of the tube is found.