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- ItemHigh Blocking Temperature of Magnetization and Giant Coercivity in the Azafullerene Tb 2 @C 79 N with a Single-Electron Terbium–Terbium Bond(Weinheim : Wiley-VCH, 2019) Velkos, Georgios; Krylov, Denis S.; Kirkpatrick, Kyle; Spree, Lukas; Dubrovin, Vasilii; Büchner, Bernd; Avdoshenko, Stanislav M.; Bezmelnitsyn, Valeriy; Davis, Sean; Faust, Paul; Duchamp, James; Dorn, Harry C.; Popov, Alexey A.The azafullerene Tb 2 @C 79 N is found to be a single-molecule magnet with a high 100-s blocking temperature of magnetization of 24 K and large coercivity. Tb magnetic moments with an easy-axis single-ion magnetic anisotropy are strongly coupled by the unpaired spin of the single-electron Tb−Tb bond. Relaxation of magnetization in Tb 2 @C 79 N below 15 K proceeds via quantum tunneling of magnetization with the characteristic time τ QTM =16 462±1230 s. At higher temperature, relaxation follows the Orbach mechanism with a barrier of 757±4 K, corresponding to the excited states, in which one of the Tb spins is flipped. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemMagnetic properties of individual Co2FeGa Heusler nanoparticles studied at room temperature by a highly sensitive co-resonant cantilever sensor(London : Nature Publishing Group, 2017) Körner, Julia; Reiche, Christopher F.; Ghunaim, Rasha; Fuge, Robert; Hampel, Silke; Büchner, Bernd; Mühl, ThomasThe investigation of properties of nanoparticles is an important task to pave the way for progress and new applications in many fields of research like biotechnology, medicine and magnetic storage techniques. The study of nanoparticles with ever decreasing size is a challenge for commonly employed methods and techniques. It requires increasingly complex measurement setups, often low temperatures and a size reduction of the respective sensors to achieve the necessary sensitivity and resolution. Here, we present results on how magnetic properties of individual nanoparticles can be measured at room temperature and with a conventional scanning force microscopy setup combined with a co-resonant cantilever magnetometry approach. We investigate individual Co2FeGa Heusler nanoparticles with diameters of the order of 35 nm encapsulated in carbon nanotubes. We observed, for the first time, magnetic switching of these nanoparticles in an external magnetic field by simple laser deflection detection. Furthermore, we were able to deduce magnetic properties of these nanoparticles which are in good agreement with previous results obtained with large nanoparticle ensembles in other experiments. In order to do this, we expand the analytical description of the frequency shift signal in cantilever magnetometry to a more general formulation, taking unaligned sensor oscillation directions with respect to the magnetic field into account.
- ItemUniversal electronic structure of polar oxide hetero-interfaces(London : Nature Publishing Group, 2015) Treske, Uwe; Heming, Nadine; Knupfer, Martin; Büchner, Bernd; Di Gennaro, Emiliano; Khare, Amit; Di Uccio, Umberto Scotti; Granozio, Fabio Miletto; Krause, Stefan; Koitzsch, AndreasThe electronic properties of NdGaO3/SrTiO3, LaGaO3/SrTiO3, and LaAlO3/SrTiO3 interfaces, all showing an insulator-to-metal transition as a function of the overlayer-thickness, are addressed in a comparative study based on x-ray absorption, x-ray photoemission and resonant photoemission spectroscopy. The nature of the charge carriers, their concentration and spatial distribution as well as the interface band alignments and the overall interface band diagrams are studied and quantitatively evaluated. The behavior of the three analyzed heterostructures is found to be remarkably similar. The valence band edge of all the three overlayers aligns to that of bulk SrTiO3. The near-interface SrTiO3 layer is affected, at increasing overlayer thickness, by the building-up of a confining potential. This potential bends both the valence and the conduction band downwards. The latter one crossing the Fermi energy in the proximity of the interface and determines the formation of an interfacial band offset growing as a function of thickness. Quite remarkably, but in agreement with previous reports for LaAlO3/SrTiO3, no electric field is detected inside any of the polar overlayers. The essential phenomenology emerging from our findings is discussed on the base of different alternative scenarios regarding the origin of interface carriers and their interaction with an intense photon beam.
- ItemTuning the spin coherence time of Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes by advanced ESR pulse protocols(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017-4-27) Zaripov, Ruslan; Vavilova, Evgeniya; Khairuzhdinov, Iskander; Salikhov, Kev; Voronkova, Violeta; Abdulmalic, Mohammad A.; Meva, Francois E.; Weheabby, Saddam; Rüffer, Tobias; Büchner, Bernd; Kataev, VladislavWe have investigated with the pulsed ESR technique at X- and Q-band frequencies the coherence and relaxation of Cu spins S = 1/2 in single crystals of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opba)] (1%) in the host lattice of [n-Bu4N]2[Ni(opba)] (99%, opba = o-phenylenebis(oxamato)) and of diamagnetically diluted mononuclear [n-Bu4N]2[Cu(opbon-Pr2)] (1%) in the host lattice of [n-Bu4N]2[Ni(opbon-Pr2)] (99%, opbon-Pr2 = o-phenylenebis(N(propyl)oxamidato)). For that we have measured the electron spin dephasing time Tm at different temperatures with the two-pulse primary echo and with the special Carr–Purcell–Meiboom–Gill (CPMG) multiple microwave pulse sequence. Application of the CPMG protocol has led to a substantial increase of the spin coherence lifetime in both complexes as compared to the primary echo results. It shows the efficiency of the suppression of the electron spin decoherence channel in the studied complexes arising due to spectral diffusion induced by a random modulation of the hyperfine interaction with the nuclear spins. We argue that this method can be used as a test for the relevance of the spectral diffusion for the electron spin decoherence. Our results have revealed a prominent role of the opba4– and opbon-Pr24– ligands for the dephasing of the Cu spins. The presence of additional 14N nuclei and protons in [Cu(opbon-Pr2)]2– as compared to [Cu(opba)]2– yields significantly shorter Tm times. Such a detrimental effect of the opbon-Pr24− ligands has to be considered when discussing a potential application of the Cu(II)−(bis)oxamato and Cu(II)−(bis)oxamidato complexes as building blocks of more complex molecular structures in prototype spintronic devices. Furthermore, in our work we propose an improved CPMG pulse protocol that enables elimination of unwanted echoes that inevitably appear in the case of inhomogeneously broadened ESR spectra due to the selective excitation of electron spins.
- ItemProbing the magnetic superexchange couplings between terminal CuII ions in heterotrinuclear bis(oxamidato) type complexes(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017-4-6) Abdulmalic, Mohammad A.; Weheabby, Saddam; Meva, Francois E.; Aliabadi, Azar; Kataev, Vladislav; Büchner, Bernd; Schleife, Frederik; Kersting, Berthold; Rüffer, TobiasThe reaction of one equivalent of [n-Bu4N]2[Ni(opboR2)] with two equivalents of [Cu(pmdta)(X)2] afforded the heterotrinuclear CuIINiIICuII containing bis(oxamidato) type complexes [Cu2Ni(opboR2)(pmdta)2]X2 (R = Me, X = NO3– (1); R = Et, X = ClO4– (2); R = n-Pr, X = NO3– (3); opboR2 = o-phenylenebis(NR-substituted oxamidato); pmdta = N,N,N’,N”,N”-pentamethyldiethylenetriamine). The identities of the heterotrinuclear complexes 1–3 were established by IR spectroscopy, elemental analysis and single-crystal X-ray diffraction studies, which revealed the cationic complex fragments [Cu2Ni(opboR2)(pmdta)2]2+ as not involved in any further intermolecular interactions. As a consequence thereof, the complexes 1–3 possess terminal paramagnetic [Cu(pmdta)]2+ fragments separated by [NiII(opboR2)]2– bridging units representing diamagnetic SNi = 0 states. The magnetic field dependence of the magnetization M(H) of 1–3 at T = 1.8 K has been determined and is shown to be highly reproducible with the Brillouin function for an ideal paramagnetic spin = 1/2 system, verifying experimentally that no magnetic superexchange couplings exists between the terminal paramagnetic [Cu(pmdta)]2+ fragments. Susceptibility measurements versus temperature of 1–3 between 1.8–300 K were performed to reinforce the statement of the absence of magnetic superexchange couplings in these three heterotrinuclear complexes.
- ItemEnergy-level alignment at interfaces between manganese phthalocyanine and C60(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017-4-25) Waas, Daniel; Rückerl, Florian; Knupfer, Martin; Büchner, BerndWe have used photoelectron spectroscopy to determine the energy-level alignment at organic heterojunctions made of manganese phthalocyanine (MnPc) and the fullerene C60. We show that this energy-level alignment depends upon the preparation sequence, which is explained by different molecular orientations. Moreover, our results demonstrate that MnPc/C60 interfaces are hardly suited for application in organic photovoltaic devices, since the energy difference of the two lowest unoccupied molecular orbitals (LUMOs) is rather small.
- ItemMagnetic Nanoparticle Chains in Gelatin Ferrogels: Bioinspiration from Magnetotactic Bacteria(Weinheim : Wiley-VCH, 2019) Sturm, Sebastian; Siglreitmeier, Maria; Wolf, Daniel; Vogel, Karin; Gratz, Micha; Faivre, Damien; Lubk, Axel; Büchner, Bernd; Sturm, Elena V.; Cölfen, HelmutInspired by chains of ferrimagnetic nanocrystals (NCs) in magnetotactic bacteria (MTB), the synthesis and detailed characterization of ferrimagnetic magnetite NC chain-like assemblies is reported. An easy green synthesis route in a thermoreversible gelatin hydrogel matrix is used. The structure of these magnetite chains prepared with and without gelatin is characterized by means of transmission electron microscopy, including electron tomography (ET). These structures indeed bear resemblance to the magnetite assemblies found in MTB, known for their mechanical flexibility and outstanding magnetic properties and known to crystallographically align their magnetite NCs along the strongest <111> magnetization easy axis. Using electron holography (EH) and angular dependent magnetic measurements, the magnetic interaction between the NCs and the generation of a magnetically anisotropic material can be shown. The electro- and magnetostatic modeling demonstrates that in order to precisely determine the magnetization (by means of EH) inside chain-like NCs assemblies, their exact shape, arrangement and stray-fields have to be considered (ideally obtained using ET). © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemMethane as a selectivity booster in the arc-discharge synthesis of endohedral fullerenes: Selective synthesis of the single-molecule magnet Dy2TiC@C80and Its Congener Dy2TiC2@C80(Hoboken, NJ : Wiley, 2015) Junghans, Katrin; Schlesier, Christin; Kostanyan, Aram; Samoylova, Nataliya A.; Deng, Qingming; Rosenkranz, Marco; Schiemenz, Sandra; Westerström, Rasmus; Greber, Thomas; Büchner, Bernd; Greber, Thomas; Popov, Alexey A.The use of methane as a reactive gas dramatically increases the selectivity of the arc‐discharge synthesis of M‐Ti‐carbide clusterfullerenes (M=Y, Nd, Gd, Dy, Er, Lu). Optimization of the process parameters allows the synthesis of Dy2TiC@C80‐I and its facile isolation in a single chromatographic step. A new type of cluster with an endohedral acetylide unit, M2TiC2@C80, is discovered along with the second isomer of M2TiC@C80. Dy2TiC@C80‐(I,II) and Dy2TiC2@C80‐I are shown to be single‐molecule magnets (SMM), but the presence of the second carbon atom in the cluster Dy2TiC2@C80 leads to substantially poorer SMM properties.
- ItemMagnetic superexchange interactions: Trinuclear bis(oxamidato) versus bis(oxamato) type complexes(Cambridge : Royal Society of Chemistry, 2015) Abdulmalic, Mohammad A.; Aliabadi, Azar; Petr, Andreas; Krupskaya, Yulia; Kataev, Vladislav; Büchner, Bernd; Zaripov, Ruslan; Vavilova, Evgeniya; Voronkova, Violeta; Salikov, Kev; Hahn, Torsten; Kortus, Jens; Meva, Francois Eya’ane; Schaarschmidt, Dieter; Rüffer, TobiasThe diethyl ester of o-phenylenebis(oxamic acid) (opbaH2Et2) was treated with an excess of RNH2 in MeOH to cause the exclusive formation of the respective o-phenylenebis(N(R)-oxamides) (opboH4R2, R = Me 1, Et 2, nPr 3) in good yields. Treatment of 1–3 with half an equivalent of [Cu2(AcO)4(H2O)2] or one equivalent of [Ni(AcO)2(H2O)4] followed by the addition of four equivalents of [nBu4N]OH resulted in the formation of mononuclear bis(oxamidato) type complexes [nBu4N]2[M(opboR2)] (M = Ni, R = Me 4, Et 5, nPr 6; M = Cu, R = Me 7, Et 8, nPr 9). By addition of two equivalents of [Cu(pmdta)(NO3)2] to MeCN solutions of 7–9, novel trinuclear complexes [Cu3(opboR2)(L)2](NO3)2 (L = pmdta, R = Me 10, Et 11, nPr 12) could be obtained. Compounds 4–12 have been characterized by elemental analysis and NMR/IR spectroscopy. Furthermore, the solid state structures of 4–10 and 12 have been determined by single-crystal X-ray diffraction studies. By controlled cocrystallization, diamagnetically diluted 8 and 9 (1%) in the host lattice of 5 and 6 (99%) (8@5 and 9@6), respectively, in the form of single crystals have been made available, allowing single crystal ESR studies to extract all components of the g-factor and the tensors of onsite CuA and transferred NA hyperfine (HF) interaction. From these studies, the spin density distribution of the [Cu(opboEt2)]2− and [Cu(opbonPr2)]2− complex fragments of 8 and 9, respectively, could be determined. Additionally, as a single crystal ENDOR measurement of 8@5 revealed the individual HF tensors of the N donor atoms to be unequal, individual estimates of the spin densities on each N donor atom were made. The magnetic properties of 10–12 were studied by susceptibility measurements versus temperature to give J values varying from −96 cm−1 (10) over −104 cm−1 (11) to −132 cm−1 (12). These three trinuclear CuII-containing bis(oxamidato) type complexes exhibit J values which are comparable to and slightly larger in magnitude than those of related bis(oxamato) type complexes. In a summarizing discussion involving experimentally obtained ESR results (spin density distribution) of 8 and 9, the geometries of the terminal [Cu(pmdta)]2+ fragments of 12 determined by crystallographic studies, together with accompanying quantum chemical calculations, an approach is derived to explain these phenomena and to conclude if the spin density distribution of mononuclear bis(oxamato)/bis(oxamidato) type complexes could be a measure of the J couplings of corresponding trinuclear complexes.
- ItemMagnetization Dynamics of an Individual Single-Crystalline Fe-Filled Carbon Nanotube(Weinheim : Wiley-VCH, 2019) Lenz, Kilian; Narkowicz, Ryszard; Wagner, Kai; Reiche, Christopher F.; Körner, Julia; Schneider, Tobias; Kákay, Attila; Schultheiss, Helmut; Weissker, Uhland; Wolf, Daniel; Suter, Dieter; Büchner, Bernd; Fassbender, Jürgen; Mühl, Thomas; Lindner, JürgenThe magnetization dynamics of individual Fe-filled multiwall carbon-nanotubes (FeCNT), grown by chemical vapor deposition, are investigated by microresonator ferromagnetic resonance (FMR) and Brillouin light scattering (BLS) microscopy and corroborated by micromagnetic simulations. Currently, only static magnetometry measurements are available. They suggest that the FeCNTs consist of a single-crystalline Fe nanowire throughout the length. The number and structure of the FMR lines and the abrupt decay of the spin-wave transport seen in BLS indicate, however, that the Fe filling is not a single straight piece along the length. Therefore, a stepwise cutting procedure is applied in order to investigate the evolution of the ferromagnetic resonance lines as a function of the nanowire length. The results show that the FeCNT is indeed not homogeneous along the full length but is built from 300 to 400 nm long single-crystalline segments. These segments consist of magnetically high quality Fe nanowires with almost the bulk values of Fe and with a similar small damping in relation to thin films, promoting FeCNTs as appealing candidates for spin-wave transport in magnonic applications. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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