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- ItemShape-adaptive single-molecule magnetism and hysteresis up to 14 K in oxide clusterfullerenes Dy2O@C72 and Dy2O@C74 with fused pentagon pairs and flexible Dy-(μ2-O)-Dy angle(Cambridge : Royal Society of Chemistry, 2020) Velkos, G.; Yang, W.; Yao, Y.-R.; Sudarkova, S.M.; Liu, X.; Büchner, B.; Avdoshenko, S.M.; Chen, N.; Popov, A.A.Dysprosium oxide clusterfullerenes Dy2O@Cs(10528)-C72 and Dy2O@C2(13333)-C74 are synthesized and characterized by single-crystal X-ray diffraction. Carbon cages of both molecules feature two adjacent pentagon pairs. These pentalene units determine positions of endohedral Dy ions hence the shape of the Dy2O cluster, which is bent in Dy2O@C72 but linear in Dy2O@C74. Both compounds show slow relaxation of magnetization and magnetic hysteresis. Nearly complete cancelation of ferromagnetic dipolar and antiferromagnetic exchange Dy⋯Dy interactions leads to unusual magnetic properties. Dy2O@C74 exhibits zero-field quantum tunneling of magnetization and magnetic hysteresis up to 14 K, the highest temperature among Dy-clusterfullerenes.
- ItemUnraveling the Orbital Physics in a Canonical Orbital System KCuF3(College Park, Md. : APS, 2021) Li, Jiemin; Xu, Lei; Garcia-Fernandez, Mirian; Nag, Abhishek; Robarts, H.C.; Walters, A.C.; Liu, X.; Zhou, Jianshi; Wohlfeld, Krzysztof; van den Brink, Jeroen; Ding, Hong; Zhou, Ke-JinWe explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF3 using the Cu L3-edge resonant inelastic x-ray scattering. We show that the nondispersive high-energy peaks result from the Cu2+ dd orbital excitations. These high-energy modes display good agreement with the ab initio quantum chemistry calculation, indicating that the dd excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Müller ansatz calculations. The localized dd excitations and the observation of the strongly dispersive magnetic excitations suggest that the orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong local Jahn-Teller effect in KCuF3, which predominantly drives orbital ordering.
- ItemSpin-orbit-driven magnetic structure and excitation in the 5d pyrochlore Cd2Os2O7(London : Nature Publishing Group, 2016) Calder, S.; Vale, J.G.; Bogdanov, N.A.; Liu, X.; Donnerer, C.; Upton, M.H.; Casa, D.; Said, A.H.; Lumsden, M.D.; Zhao, Z.; Yan, J.-Q.; Mandrus, D.; Nishimoto, S.; van den Brink, J.; Hill, J.P.; McMorrow, D.F.; Christianson, A.D.Much consideration has been given to the role of spin-orbit coupling (SOC) in 5d oxides, particularly on the formation of novel electronic states and manifested metal-insulator transitions (MITs). SOC plays a dominant role in 5d5 iridates (Ir4þ), undergoing MITs both concurrent (pyrochlores) and separated (perovskites) from the onset of magnetic order. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (Os5þ) systems are expected to have an orbital singlet with reduced effective SOC. The pyrochlore Cd2Os2O7 nonetheless exhibits a MIT entwined with magnetic order phenomenologically similar to pyrochlore iridates. Here, we resolve the magnetic structure in Cd2Os2O7 with neutron diffraction and then via resonant inelastic X-ray scattering determine the salient electronic and magnetic energy scales controlling the MIT. In particular, SOC plays a subtle role in creating the electronic ground state but drives the magnetic order and emergence of a multiple spin-flip magnetic excitation.
- ItemElectronic properties of intercalated single-wall carbon nanotubes and C60 peapods(Milton Park : Taylor & Francis, 2003) Pichler, T.; Liu, X.; Knupfer, M.; Fink, J.This paper reviews recent investigations of the electronic structure and the optical properties of intercalated single-wall carbon nanotubes (SWCNTs) and C60 filled SWCNTs (peapods) using electron energy-loss spectroscopy (EELS) in transmission as a probe. The results from these one-dimensional nanostructures are compared to C60 fullerides and intercalated graphite, which are well understood prototypes of carbon-based intercalation compounds. In detail, the structural changes were analysed by electron diffraction and the doping level and the matrix element weighted unoccupied density of states (DOS) by an analysis of the C 1s core-level excitations. Regarding the optical properties, the intercalation gives rise to a charge transfer to the peapods (SWCNTs) which leads to the formation of a free charge carrier plasmon in the loss function which is analysed within the framework of an effective Drude–Lorentz model.
- ItemFree-standing Fe2O3 nanomembranes enabling ultra-long cycling life and high rate capability for Li-ion batteries(London : Nature Publishing Group, 2014) Liu, X.; Si, W.; Zhang, J.; Sun, X.; Deng, J.; Baunack, S.; Oswald, S.; Liu, L.; Yan, C.; Schmidt, O.G.With Fe2O3 as a proof-of-concept, free-standing nanomembrane structure is demonstrated to be highly advantageous to improve the performance of Li-ion batteries. The Fe2O3 nanomembrane electrodes exhibit ultra-long cycling life at high current rates with satisfactory capacity (808 mAh g-1 after 1000 cycles at 2 C and 530 mAh g-1 after 3000 cycles at 6 C) as well as repeatable high rate capability up to 50 C. The excellent performance benefits particularly from the unique structural advantages of the nanomembranes. The mechanical feature can buffer the strain of lithiation/delithiation to postpone the pulverization. The two-dimensional transport pathways in between the nanomembranes can promote the pseudo-capacitive type storage. The parallel-laid nanomembranes, which are coated by polymeric gel-like film and SEI layer with the electrolyte in between layers, electrochemically behave like numerous "mini-capacitors" to provide the pseudo-capacitance thus maintain the capacity at high rate.