Browsing by Author "Klingeler, R."
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- ItemComment on 'Oxygen vacancy-induced magnetic moment in edge-sharing CuO2 chains of Li2CuO2'(Bristol : IOP Publishing, 2018) Kuzian, R.O.; Klingeler, R.; Lorenz, W.E.A.; Wizent, N.; Nishimoto, S.; Nitzsche, U.; Rosner, H.; Milosavljevic, D.; Hozoi, L.; Yadav, R.; Richter, J.; Hauser, A.; Geck, J.; Hayn, R.; Yushankhai, V.; Siurakshina, L.; Monney, C.; Schmitt, T.; Schmitt, T.; Roth, G.; Ito, T.; Yamaguchi, H.; Matsuda, M.; Johnston, S.; Málek, J.; Drechsler, S.-L.In a recent work devoted to the magnetism of Li2CuO2, Shu et al (2017 New J. Phys. 19, 023026) have proposed a 'simplified' unfrustrated microscopic model that differs considerably from the models refined through decades of prior work. We show that the proposed model is at odds with known experimental data, including the reported magnetic susceptibility χ(T) data up to 550 K. Using an 8th order high-temperature expansion for χ(T), we show that the experimental data for Li2CuO2 are consistent with the prior model derived from inelastic neutron scattering studies. We also establish the T-range of validity for a Curie–Weiss law for the real frustrated magnetic system. We argue that the knowledge of the long-range ordered magnetic structure for T < T N and of χ(T) in a restricted T-range provides insufficient information to extract all of the relevant couplings in frustrated magnets; the saturation field and INS data must also be used to determine several exchange couplings, including the weak but decisive frustrating antiferromagnetic interchain couplings.
- ItemFilled carbon nanotubes as anode materials for lithium-ion batteries(Basel : MDPI AG, 2020) Thauer, E.; Ottmann, A.; Schneider, P.; Möller, L.; Deeg, L.; Zeus, R.; Wilhelmi, F.; Schlestein, L.; Neef, C.; Ghunaim, R.; Gellesch, M.; Nowka, C.; Scholz, M.; Haft, M.; Wurmehl, S.; Wenelska, K.; Mijowska, E.; Kapoor, A.; Bajpai, A.; Hampel, S.; Klingeler, R.Downsizing well-established materials to the nanoscale is a key route to novel functionalities, in particular if different functionalities are merged in hybrid nanomaterials. Hybrid carbon-based hierarchical nanostructures are particularly promising for electrochemical energy storage since they combine benefits of nanosize effects, enhanced electrical conductivity and integrity of bulk materials. We show that endohedral multiwalled carbon nanotubes (CNT) encapsulating high-capacity (here: conversion and alloying) electrode materials have a high potential for use in anode materials for lithium-ion batteries (LIB). There are two essential characteristics of filled CNT relevant for application in electrochemical energy storage: (1) rigid hollow cavities of the CNT provide upper limits for nanoparticles in their inner cavities which are both separated from the fillings of other CNT and protected against degradation. In particular, the CNT shells resist strong volume changes of encapsulates in response to electrochemical cycling, which in conventional conversion and alloying materials hinders application in energy storage devices. (2) Carbon mantles ensure electrical contact to the active material as they are unaffected by potential cracks of the encapsulate and form a stable conductive network in the electrode compound. Our studies confirm that encapsulates are electrochemically active and can achieve full theoretical reversible capacity. The results imply that encapsulating nanostructures inside CNT can provide a route to new high-performance nanocomposite anode materials for LIB.
- ItemHigh-field ESR studies of the quantum spin magnet CaCu2O 3(Milton Park : Taylor & Francis, 2006) Goiran, M.; Costes, M.; Broto, J.M.; Chou, F.C.; Klingeler, R.; Arushanov, E.; Drechsler, S.-L.; Büchner, B.; Kataev, V.We report an electron spin resonance (ESR) study of the s = 1/2 Heisenberg pseudo-ladder magnet CaCu2O3 in pulsed magnetic fields up to 40 T. At sub-terahertz frequencies we observe an ESR signal originating from a small amount of uncompensated spins residing presumably at the imperfections of the strongly antiferromagnetically correlated host spin lattice. The data give evidence that these few per cent of 'extra' spin states are coupled strongly to the bulk spins and are involved in the antiferromagnetic (AF) ordering at TN = 25 K. By mapping the frequency/resonance field diagram we have determined a small gap for magnetic excitations below TN of the order of ~0.3–0.8 meV. Such a small value of the gap explains the occurrence of the spin-flop transition in CaCu2O3 at weak magnetic fields μ0Hsf ~ 3 T. Qualitative changes of the ESR response with the increasing field strength give indications that strong magnetic fields reduce the AF correlations and may even suppress the long-range magnetic order in CaCu2O3. ESR data support scenarios with a significant role of the 'extra' spin states for the properties of low-dimensional quantum magnets.
- ItemMagnetoelastic coupling and ferromagnetic-type in-gap spin excitations in multiferroic α-Cu2V2O7(Bristol : Institute of Physics Publishing, 2018) Wang, L.; Werner, J.; Ottmann, A.; Weis, R.; Abdel-Hafiez, M.; Sannigrahi, J.; Majumdar, S.; Koo, C.; Klingeler, R.We investigate magnetoelectric coupling and low-energy magnetic excitations in multiferroic α-Cu2V2O7 by detailed thermal expansion, magnetostriction, specific heat and magnetization measurements in magnetic fields up to 15 T and by high-field/high-frequency electron spin resonance studies. Our data show negative thermal expansion in the temperature range ≤200 K under study. Well-developed anomalies associated with the onset of multiferroic order (canted antiferromagnetism with a significant magnetic moment and ferroelectricity) imply pronounced coupling to the structure. We detect anomalous entropy changes in the temperature regime up to ∼80 K which significantly exceed the spin entropy. Failure of Grüneisen scaling further confirms that several dominant ordering phenomena are concomitantly driving the multiferroic order. By applying external magnetic fields, anomalies in the thermal expansion and in the magnetization are separated. Noteworthy, the data clearly imply the development of a canted magnetic moment at temperatures above the structural anomaly. Low-field magnetostriction supports the scenario of exchange-striction driven multiferroicity. We observe low-energy magnetic excitations well below the antiferromagnetic gap, i.e., a ferromagnetic-type resonance branch associated with the canted magnetic moment arising from Dzyaloshinsii-Moriya (DM) interactions. The anisotropy parameter meV indicates a sizeable ratio of DM- and isotropic magnetic exchange.
- ItemOrbital order induced ferromagnetic insulating properties(Milton Park : Taylor & Francis, 2004) Geck, J.; Wochner, P.; Kiele, S.; Klingeler, R.; Revcolevschi, A.; v. Zimmermann, M.; Büchner, B.; Reutler, P.At temperatures below the metal-insulator transition of La 1-xSrxMnO3 with 0.1 < x < 0.15, a peculiar ferromagnetic and insulating phase is observed which has been intensively discussed over the last few years. We present a detailed investigation of this phase by means of resonant and high energy x-ray scattering along with measurements of the electrical resistivity, thermal expansion, magnetization, and specific heat. Interestingly, the data show that the metal-insulator transition of lightly doped manganites is accompanied by an orbital rearrangement. The microscopic information provided by the x-ray scattering studies together with the analysis of the macroscopic properties implies that the orbital reordering maximizes the gain of double exchange energy and, at the same time, induces an insulating behaviour. The relevance of the double-exchange mechanism for the stabilization of the ferromagnetic insulating phase is further substantiated by studies of (La1-yPr y)7/8Sr1/8MnO3: with increasing praseodymium content, the metal-insulator transition is dramatically suppressed which can naturally be explained by a reduction of the band width upon praseodymium doping.
- ItemSingle-crystalline FeCo nanoparticle-filled carbon nanotubes: Synthesis, structural characterization and magnetic properties(Frankfurt am Main : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2018) Ghunaim, R.; Scholz, M.; Damm, C.; Rellinghaus, B.; Klingeler, R.; Büchner, B.; Mertig, M.; Hampel, S.In the present work, we demonstrate different synthesis procedures for filling carbon nanotubes (CNTs) with equimolar binary nanoparticles of the type Fe-Co. The CNTs act as templates for the encapsulation of magnetic nanoparticles and provide a protective shield against oxidation as well as prevent nanoparticle agglomeration. By variation of the reaction parameters, we were able to tailor the sample purity, degree of filling, the composition and size of the filling particles, and therefore, the magnetic properties. The samples were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), superconducting quantum interference device (SQUID) and thermogravimetric analysis (TGA). The Fe-Co-filled CNTs show significant enhancement in the coercive field as compared to the corresponding bulk material, which make them excellent candidates for several applications such as magnetic storage devices.
- ItemStrong effects of uniaxial pressure and short-range correlations in Cr2Ge2Te6(College Park, MD : APS, 2022) Spachmann, S.; Elghandour, A.; Selter, S.; Büchner, B.; Aswartham, S.; Klingeler, R.Cr2Ge2Te6 is a quasi-two-dimensional semiconducting van der Waals ferromagnet down to the bilayer with great potential for technological applications. Engineering the critical temperature to achieve room-temperature applications is one of the critical next steps on this path. Here, we report high-resolution capacitance dilatometry studies on Cr2Ge2Te6 single crystals which directly prove significant magnetoelastic coupling and provide quantitative values of the large uniaxial pressure effects on long-range magnetic order (∂TC/∂pc=24.7 K/GPa and ∂TC/∂pab=−15.6 K/GPa) derived from thermodynamic relations. Moderate in-plane strain is thus sufficient to strongly enhance ferromagnetism in Cr2Ge2Te6 up to room temperature. Moreover, unambiguous signs of short-range magnetic order up to 200 K are found.