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Promoting abnormal grain growth in Fe-based shape memory alloys through compositional adjustments

2019, Vollmer, M., Arold, T., Kriegel, M.J., Klemm, V., Degener, S., Freudenberger, J., Niendorf, T.

Iron-based shape memory alloys are promising candidates for large-scale structural applications due to their cost efficiency and the possibility of using conventional processing routes from the steel industry. However, recently developed alloy systems like Fe–Mn–Al–Ni suffer from low recoverability if the grains do not completely cover the sample cross-section. To overcome this issue, here we show that small amounts of titanium added to Fe–Mn–Al–Ni significantly enhance abnormal grain growth due to a considerable refinement of the subgrain sizes, whereas small amounts of chromium lead to a strong inhibition of abnormal grain growth. By tailoring and promoting abnormal grain growth it is possible to obtain very large single crystalline bars. We expect that the findings of the present study regarding the elementary mechanisms of abnormal grain growth and the role of chemical composition can be applied to tailor other alloy systems with similar microstructural features.

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Air-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond

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.

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Highly-efficient extraction of entangled photons from quantum dots using a broadband optical antenna

2018, Chen, Y., Zopf, M., Keil, R., Ding, F., Schmidt, O.G.

Many quantum photonic technologies require the efficient generation of entangled pairs of photons, but to date there have been few ways to produce them reliably. Sources based on parametric down conversion operate at very low efficiency per pulse due to the probabilistic generation process. Semiconductor quantum dots can emit single pairs of entangled photons deterministically but they fall short due to the extremely low-extraction efficiency. Strategies for extracting single photons from quantum dots, such as embedding them in narrowband optical cavities, are difficult to translate to entangled photons. Here, we build a broadband optical antenna with an extraction efficiency of 65% ± 4% and demonstrate a highly-efficient entangled-photon source by collecting strongly entangled photons (fidelity of 0.9) at a pair efficiency of 0.372 ± 0.002 per pulse. The high brightness achieved by our source represents a step forward in the development of optical quantum technologies.

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A diuranium carbide cluster stabilized inside a C80 fullerene cage

2018, Zhang, X., Li, W., Feng, L., Chen, X., Hansen, A., Grimme, S., Fortier, S., Sergentu, D.-C., Duignan, T.J., Autschbach, J., Wang, S., Wang, Y., Velkos, G., Popov, A.A., Aghdassi, N., Duhm, S., Li, X., Li, J., Echegoyen, L., Schwarz, W.H.E., Chen, N.

Unsupported non-bridged uranium-carbon double bonds have long been sought after in actinide chemistry as fundamental synthetic targets in the study of actinide-ligand multiple bonding. Here we report that, utilizing I h(7)-C80 fullerenes as nanocontainers, a diuranium carbide cluster, U=C=U, has been encapsulated and stabilized in the form of UCU@I h(7)-C80. This endohedral fullerene was prepared utilizing the Krätschmer-Huffman arc discharge method, and was then co-crystallized with nickel(II) octaethylporphyrin (NiII-OEP) to produce UCU@I h(7)-C80·[NiII-OEP] as single crystals. X-ray diffraction analysis reveals a cage-stabilized, carbide-bridged, bent UCU cluster with unexpectedly short uranium-carbon distances (2.03 Å) indicative of covalent U=C double-bond character. The quantum-chemical results suggest that both U atoms in the UCU unit have formal oxidation state of +5. The structural features of UCU@I h(7)-C80 and the covalent nature of the U(f1)=C double bonds were further affirmed through various spectroscopic and theoretical analyses.

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Tailor-made nanostructures bridging chaos and order for highly efficient white organic light-emitting diodes

2019, Li, Y., Kovačič, M., Westphalen, J., Oswald, S., Ma, Z., Hänisch, C., Will, P.-A., Jiang, L., Junghaehnel, M., Scholz, R., Lenk, S., Reineke, S.

Organic light-emitting diodes (OLEDs) suffer from notorious light trapping, resulting in only moderate external quantum efficiencies. Here, we report a facile, scalable, lithography-free method to generate controllable nanostructures with directional randomness and dimensional order, significantly boosting the efficiency of white OLEDs. Mechanical deformations form on the surface of poly(dimethylsiloxane) in response to compressive stress release, initialized by reactive ions etching with periodicity and depth distribution ranging from dozens of nanometers to micrometers. We demonstrate the possibility of independently tuning the average depth and the dominant periodicity. Integrating these nanostructures into a two-unit tandem white organic light-emitting diode, a maximum external quantum efficiency of 76.3% and a luminous efficacy of 95.7 lm W−1 are achieved with extracted substrate modes. The enhancement factor of 1.53 ± 0.12 at 10,000 cd m−2 is obtained. An optical model is built by considering the dipole orientation, emitting wavelength, and the dipole position on the sinusoidal nanotexture.

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Tuning the interplay between nematicity and spin fluctuations in Na1-x Li x FeAs superconductors

2018, Baek, S.-H., Bhoi, D., Nam, W., Lee, B., Efremov, D.V., Büchner, B., Kim, K.H.

Strong interplay of spin and charge/orbital degrees of freedom is the fundamental characteristic of the iron-based superconductors (FeSCs), which leads to the emergence of a nematic state as a rule in the vicinity of the antiferromagnetic state. Despite intense debate for many years, however, whether nematicity is driven by spin or orbital fluctuations remains unsettled. Here, by use of transport, magnetization, and 75As nuclear magnetic resonance (NMR) measurements, we show a striking transformation of the relationship between nematicity and spin fluctuations (SFs) in Na1-x Li x FeAs; For x ≤ 0.02, the nematic transition promotes SFs. In contrast, for x ≥ 0.03, the system undergoes a non-magnetic phase transition at a temperature T 0 into a distinct nematic state that suppresses SFs. Such a drastic change of the spin fluctuation spectrum associated with nematicity by small doping is highly unusual, and provides insights into the origin and nature of nematicity in FeSCs.

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Large magneto-Seebeck effect in magnetic tunnel junctions with half-metallic Heusler electrodes

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.

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Switchable magnetic bulk photovoltaic effect in the two-dimensional magnet CrI3

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.

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Uniaxial stress flips the natural quantization axis of a quantum dot for integrated quantum photonics

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.

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Giant thermal expansion and α-precipitation pathways in Ti-Alloys

2017, Bönisch, M., Panigrahi, A., Stoica, M., Calin, M., Ahrens, E., Zehetbauer, M., Skrotzki, W., Eckert, J.

Ti-Alloys represent the principal structural materials in both aerospace development and metallic biomaterials. Key to optimizing their mechanical and functional behaviour is in-depth know-how of their phases and the complex interplay of diffusive vs. displacive phase transformations to permit the tailoring of intricate microstructures across a wide spectrum of configurations. Here, we report on structural changes and phase transformations of Ti-Nb alloys during heating by in situ synchrotron diffraction. These materials exhibit anisotropic thermal expansion yielding some of the largest linear expansion coefficients (+ 163.9×10-6 to-95.1×10-6 °C-1) ever reported. Moreover, we describe two pathways leading to the precipitation of the α-phase mediated by diffusion-based orthorhombic structures, α″lean and α″iso. Via coupling the lattice parameters to composition both phases evolve into α through rejection of Nb. These findings have the potential to promote new microstructural design approaches for Ti-Nb alloys and β-stabilized Ti-Alloys in general.