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- ItemSingle molecule magnet with an unpaired electron trapped between two lanthanide ions inside a fullerene(London : Nature Publishing Group, 2017) Liu, F.; Krylov, D.S.; Spree, L.; Avdoshenko, S.M.; Samoylova, N.A.; Rosenkranz, M.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Büchner, B.; Popov, A.A.Increasing the temperature at which molecules behave as single-molecule magnets is a serious challenge in molecular magnetism. One of the ways to address this problem is to create the molecules with strongly coupled lanthanide ions. In this work, endohedral metallofullerenes Y 2 @C 80 and Dy 2 @C 80 are obtained in the form of air-stable benzyl monoadducts. Both feature an unpaired electron trapped between metal ions, thus forming a single-electron metal-metal bond. Giant exchange interactions between lanthanide ions and the unpaired electron result in single-molecule magnetism of Dy 2 @C 80 (CH 2 Ph) with a record-high 100 s blocking temperature of 18 K. All magnetic moments in Dy 2 @C 80 (CH 2 Ph) are parallel and couple ferromagnetically to form a single spin unit of 21 μ B with a dysprosium-electron exchange constant of 32 cm -1. The barrier of the magnetization reversal of 613 K is assigned to the state in which the spin of one Dy centre is flipped.
- ItemAir-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond(London : Nature Publishing Group, 2019) Liu, F.; Velkos, G.; Krylov, D.S.; Spree, L.; Zalibera, M.; Ray, R.; Samoylova, N.A.; Chen, C.-H.; Rosenkranz, M.; Schiemenz, S.; Ziegs, F.; Nenkov, K.; Kostanyan, A.; Greber, T.; Wolter, A.U.B.; Richter, M.; Büchner, B.; Avdoshenko, S.M.; Popov, A.A.Engineering intramolecular exchange interactions between magnetic metal atoms is a ubiquitous strategy for designing molecular magnets. For lanthanides, the localized nature of 4f electrons usually results in weak exchange coupling. Mediating magnetic interactions between lanthanide ions via radical bridges is a fruitful strategy towards stronger coupling. In this work we explore the limiting case when the role of a radical bridge is played by a single unpaired electron. We synthesize an array of air-stable Ln 2 @C 80 (CH 2 Ph) dimetallofullerenes (Ln 2 = Y 2 , Gd 2 , Tb 2 , Dy 2 , Ho 2 , Er 2 , TbY, TbGd) featuring a covalent lanthanide-lanthanide bond. The lanthanide spins are glued together by very strong exchange interactions between 4f moments and a single electron residing on the metal–metal bonding orbital. Tb 2 @C 80 (CH 2 Ph) shows a gigantic coercivity of 8.2 Tesla at 5 K and a high 100-s blocking temperature of magnetization of 25.2 K. The Ln-Ln bonding orbital in Ln 2 @C 80 (CH 2 Ph) is redox active, enabling electrochemical tuning of the magnetism.
- ItemSwitchable magnetic bulk photovoltaic effect in the two-dimensional magnet CrI3(London : Nature Publishing Group, 2019) Zhang, Y.; Holder, T.; Ishizuka, H.; de Juan, F.; Nagaosa, N.; Felser, C.; Yan, B.The bulk photovoltaic effect (BPVE) rectifies light into the dc current in a single-phase material and attracts the interest to design high-efficiency solar cells beyond the pn junction paradigm. Because it is a hot electron effect, the BPVE surpasses the thermodynamic Shockley–Queisser limit to generate above-band-gap photovoltage. While the guiding principle for BPVE materials is to break the crystal centrosymmetry, here we propose a magnetic photogalvanic effect (MPGE) that introduces the magnetism as a key ingredient and induces a giant BPVE. The MPGE emerges from the magnetism-induced asymmetry of the carrier velocity in the band structure. We demonstrate the MPGE in a layered magnetic insulator CrI3, with much larger photoconductivity than any previously reported results. The photocurrent can be reversed and switched by controllable magnetic transitions. Our work paves a pathway to search for magnetic photovoltaic materials and to design switchable devices combining magnetic, electronic, and optical functionalities.
- ItemLarge thermoelectric power factor from crystal symmetry-protected non-bonding orbital in half-Heuslers(London : Nature Publishing Group, 2018) Zhou, J.; Zhu, H.; Liu, T.-H.; Song, Q.; He, R.; Mao, J.; Liu, Z.; Ren, W.; Liao, B.; Singh, D.J.; Ren, Z.; Chen, G.Modern society relies on high charge mobility for efficient energy production and fast information technologies. The power factor of a material-the combination of electrical conductivity and Seebeck coefficient-measures its ability to extract electrical power from temperature differences. Recent advancements in thermoelectric materials have achieved enhanced Seebeck coefficient by manipulating the electronic band structure. However, this approach generally applies at relatively low conductivities, preventing the realization of exceptionally high-power factors. In contrast, half-Heusler semiconductors have been shown to break through that barrier in a way that could not be explained. Here, we show that symmetry-protected orbital interactions can steer electron-acoustic phonon interactions towards high mobility. This high-mobility regime enables large power factors in half-Heuslers, well above the maximum measured values. We anticipate that our understanding will spark new routes to search for better thermoelectric materials, and to discover high electron mobility semiconductors for electronic and photonic applications.
- ItemUniaxial stress flips the natural quantization axis of a quantum dot for integrated quantum photonics(London : Nature Publishing Group, 2018) Yuan, X.; Weyhausen-Brinkmann, F.; Martín-Sánchez, J.; Piredda, G.; Křápek, V.; Huo, Y.; Huang, H.; Schimpf, C.; Schmidt, O.G.; Edlinger, J.; Bester, G.; Trotta, R.; Rastelli, A.The optical selection rules in epitaxial quantum dots are strongly influenced by the orientation of their natural quantization axis, which is usually parallel to the growth direction. This configuration is well suited for vertically emitting devices, but not for planar photonic circuits because of the poorly controlled orientation of the transition dipoles in the growth plane. Here we show that the quantization axis of gallium arsenide dots can be flipped into the growth plane via moderate in-plane uniaxial stress. By using piezoelectric strain-actuators featuring strain amplification, we study the evolution of the selection rules and excitonic fine structure in a regime, in which quantum confinement can be regarded as a perturbation compared to strain in determining the symmetry-properties of the system. The experimental and computational results suggest that uniaxial stress may be the right tool to obtain quantum-light sources with ideally oriented transition dipoles and enhanced oscillator strengths for integrated quantum photonics.
- ItemEvolution of the Kondo lattice and non-Fermi liquid excitations in a heavy-fermion metal(London : Nature Publishing Group, 2018) Seiro, S.; Jiao, L.; Kirchner, S.; Hartmann, S.; Friedemann, S.; Krellner, C.; Geibel, C.; Si, Q.; Steglich, F.; Wirth, S.Strong electron correlations can give rise to extraordinary properties of metals with renormalized Landau quasiparticles. Near a quantum critical point, these quasiparticles can be destroyed and non-Fermi liquid behavior ensues. YbRh2Si2 is a prototypical correlated metal exhibiting the formation of quasiparticle and Kondo lattice coherence, as well as quasiparticle destruction at a field-induced quantum critical point. Here we show how, upon lowering the temperature, Kondo lattice coherence develops at zero field and finally gives way to non-Fermi liquid electronic excitations. By measuring the single-particle excitations through scanning tunneling spectroscopy, we find the Kondo lattice peak displays a non-trivial temperature dependence with a strong increase around 3.3 K. At 0.3 K and with applied magnetic field, the width of this peak is minimized in the quantum critical regime. Our results demonstrate that the lattice Kondo correlations have to be sufficiently developed before quantum criticality can set in.
- ItemX-ray imaging of chemically active valence electrons during a pericyclic reaction(London : Nature Publishing Group, 2014) Bredtmann, T.; Ivanov, M.; Dixit, G.Time-resolved imaging of chemically active valence electron densities is a long-sought goal, as these electrons dictate the course of chemical reactions. However, X-ray scattering is always dominated by the core and inert valence electrons, making time-resolved X-ray imaging of chemically active valence electron densities extremely challenging. Here we demonstrate an effective and robust method, which emphasizes the information encoded in weakly scattered photons, to image chemically active valence electron densities. The degenerate Cope rearrangement of semibullvalene, a pericyclic reaction, is used as an example to visually illustrate our approach. Our work also provides experimental access to the long-standing problem of synchronous versus asynchronous bond formation and breaking during pericyclic reactions.
- ItemLarge magneto-Seebeck effect in magnetic tunnel junctions with half-metallic Heusler electrodes(London : Nature Publishing Group, 2017) Boehnke, A.; Martens, U.; Sterwerf, C.; Niesen, A.; Huebner, T.; Von Der Ehe, M.; Meinert, M.; Kuschel, T.; Thomas, A.; Heiliger, C.; Münzenberg, M.; Reiss, G.Spin caloritronics studies the interplay between charge-, heat- and spin-currents, which are initiated by temperature gradients in magnetic nanostructures. A plethora of new phenomena has been discovered that promises, e.g., to make wasted heat in electronic devices useable or to provide new read-out mechanisms for information. However, only few materials have been studied so far with Seebeck voltages of only some microvolt, which hampers applications. Here, we demonstrate that half-metallic Heusler compounds are hot candidates for enhancing spin-dependent thermoelectric effects. This becomes evident when considering the asymmetry of the spin-split density of electronic states around the Fermi level that determines the spin-dependent thermoelectric transport in magnetic tunnel junctions. We identify Co2FeAl and Co2FeSi Heusler compounds as ideal due to their energy gaps in the minority density of states, and demonstrate devices with substantially larger Seebeck voltages and tunnel magneto-Seebeck effect ratios than the commonly used Co-Fe-B-based junctions.
- ItemCorrelation induced electron-hole asymmetry in quasi- two-dimensional iridates(London : Nature Publishing Group, 2017) Pärschke, E.M.; Wohlfeld, K.; Foyevtsova, K.; Van Den Brink, J.The resemblance of crystallographic and magnetic structures of the quasi-two-dimensional iridates Ba2IrO4 and Sr2IrO4 to La2CuO4 points at an analogy to cuprate high-Tc superconductors, even if spin-orbit coupling is very strong in iridates. Here we examine this analogy for the motion of a charge (hole or electron) added to the antiferromagnetic ground state. We show that correlation effects render the hole and electron case in iridates very different. An added electron forms a spin polaron, similar to the cuprates, but the situation of a removed electron is far more complex. Many-body 5d 4 configurations form which can be singlet and triplet states of total angular momentum that strongly affect the hole motion. This not only has ramifications for the interpretation of (inverse-)photoemission experiments but also demonstrates that correlation physics renders electron- and hole-doped iridates fundamentally different.
- ItemSolar spectral conversion for improving the photosynthetic activity in algae reactors(London : Nature Publishing Group, 2013) Wondraczek, L.; Batentschuk, M.; Schmidt, M.A.; Borchardt, R.; Scheiner, S.; Seemann, B.; Schweizer, P.; Brabec, C.J.Sustainable biomass production is expected to be one of the major supporting pillars for future energy supply, as well as for renewable material provision. Algal beds represent an exciting resource for biomass/biofuel, fine chemicals and CO2 storage. Similar to other solar energy harvesting techniques, the efficiency of algal photosynthesis depends on the spectral overlap between solar irradiation and chloroplast absorption. Here we demonstrate that spectral conversion can be employed to significantly improve biomass growth and oxygen production rate in closed-cycle algae reactors. For this purpose, we adapt a photoluminescent phosphor of the type Ca 0.59Sr0.40Eu0.01S, which enables efficient conversion of the green part of the incoming spectrum into red light to better match the Qy peak of chlorophyll b. Integration of a Ca 0.59Sr0.40Eu0.01S backlight converter into a flat panel algae reactor filled with Haematococcus pluvialis as a model species results in significantly increased photosynthetic activity and algae reproduction rate.