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- ItemUltrasmall SnO₂ nanocrystals: hot-bubbling synthesis, encapsulation in carbon layers and applications in high capacity Li-ion storage([London] : Macmillan Publishers Limited, part of Springer Nature, 2014) Ding, Liping; He, Shulian; Miao, Shiding; Jorgensen, Matthew R.; Leubner, Susanne; Yan, Chenglin; Hickey, Stephen G.; Eychmüller, Alexander; Xu, Jinzhang; Schmidt, Oliver G.Ultrasmall SnO2 nanocrystals as anode materials for lithium-ion batteries (LIBs) have been synthesized by bubbling an oxidizing gas into hot surfactant solutions containing Sn-oleate complexes. Annealing of the particles in N2 carbonifies the densely packed surface capping ligands resulting in carbon encapsulated SnO2 nanoparticles (SnO2/C). Carbon encapsulation can effectively buffer the volume changes during the lithiation/delithiation process. The assembled SnO2/C thus deliver extraordinarily high reversible capacity of 908 mA·h·g−1 at 0.5 C as well as excellent cycling performance in the LIBs. This method demonstrates the great potential of SnO2/C nanoparticles for the design of high power LIBs.
- ItemNano-biosupercapacitors enable autarkic sensor operation in blood([London] : Nature Publishing Group UK, 2021) Lee, Yeji; Bandari, Vineeth Kumar; Li, Zhe; Medina-Sánchez, Mariana; Maitz, Manfred F.; Karnaushenko, Daniil; Tsurkan, Mikhail V; Karnaushenko, Dmitriy D.; Schmidt, Oliver G.Today’s smallest energy storage devices for in-vivo applications are larger than 3 mm3 and lack the ability to continuously drive the complex functions of smart dust electronic and microrobotic systems. Here, we create a tubular biosupercapacitor occupying a mere volume of 1/1000 mm3 (=1 nanoliter), yet delivering up to 1.6 V in blood. The tubular geometry of this nano-biosupercapacitor provides efficient self-protection against external forces from pulsating blood or muscle contraction. Redox enzymes and living cells, naturally present in blood boost the performance of the device by 40% and help to solve the self-discharging problem persistently encountered by miniaturized supercapacitors. At full capacity, the nano-biosupercapacitors drive a complex integrated sensor system to measure the pH-value in blood. This demonstration opens up opportunities for next generation intravascular implants and microrobotic systems operating in hard-to-reach small spaces deep inside the human body.
- ItemStrong magnetic frustration and anti-site disorder causing spin-glass behavior in honeycomb Li2RhO3([London] : Macmillan Publishers Limited, part of Springer Nature, 2015) Katukuri, Vamshi M.; Nishimoto, Satoshi; Rousochatzakis, Ioannis; Stoll, Hermann; van den Brink, Jeroen; Hozoi, LiviuWith large spin-orbit coupling, the electron configuration in d-metal oxides is prone to highly anisotropic exchange interactions and exotic magnetic properties. In 5d5 iridates, given the existing variety of crystal structures, the magnetic anisotropy can be tuned from antisymmetric to symmetric Kitaev-type, with interaction strengths that outsize the isotropic terms. By many-body electronic-structure calculations we here address the nature of the magnetic exchange and the intriguing spin-glass behavior of Li2RhO3, a 4d5 honeycomb oxide. For pristine crystals without Rh-Li site inversion, we predict a dimerized ground state as in the isostructural 5d5 iridate Li2IrO3, with triplet spin dimers effectively placed on a frustrated triangular lattice. With Rh-Li anti-site disorder, we explain the observed spin-glass phase as a superposition of different, nearly degenerate symmetry-broken configurations.
- ItemStructure-property relationship of Co 2 MnSi thin films in response to He + -irradiation([London] : Macmillan Publishers Limited, part of Springer Nature, 2019) Hammerath, Franziska; Bali, Rantej; Hübner, René; Brandt, Mira R. D.; Rodan, Steven; Potzger, Kay; Böttger, Roman; Sakuraba, Yuya; Wurmehl, SabineWe investigated the structure-property relationship of Co2MnSi Heusler thin films upon the irradiation with He+ ions. The variation of the crystal structure with increasing ion fluence has been probed using nuclear magnetic resonance (NMR) and transmission electron microscopy (TEM), and associated with the corresponding changes of the magnetic behavior. A decrease of both the structural order and the moment in saturation is observed. Specifically, we detect a direct transition from a highly L21-ordered to a fully A2-disordered structure type and quantify the evolution of the A2 structural contribution as a function of ion fluence. Complementary TEM analysis reveals a spatially-resolved distribution of the L21 and A2 phases showing that the A2 disorder starts at the upper part of the films. The structural degradation in turn leads to a decreasing magnetic moment in saturation in response to the increasing fluence.
- ItemMagnetic patterning of Co/Ni layered systems by plasma oxidation([London] : Macmillan Publishers Limited, part of Springer Nature, 2022) Anastaziak, Błażej; Andrzejewska, Weronika; Schmidt, Marek; Matczak, Michał; Soldatov, Ivan; Schäfer, Rudolf; Lewandowski, Mikołaj; Stobiecki, Feliks; Janzen, Christian; Ehresmann, Arno; Kuświk, PiotrWe studied the structural, chemical, and magnetic properties of Ti/Au/Co/Ni layered systems subjected to plasma oxidation. The process results in the formation of NiO at the expense of metallic Ni, as clearly evidenced by X-ray photoelectron spectroscopy, while not affecting the surface roughness and grain size of the Co/Ni bilayers. Since the decrease of the thickness of the Ni layer and the formation of NiO increase the perpendicular magnetic anisotropy, oxidation may be locally applied for magnetic patterning. Using this approach, we created 2D heterostructures characterized by different combinations of magnetic properties in areas modified by plasma oxidation and in the regions protected from oxidation. As plasma oxidation is an easy to use, low cost, and commonly utilized technique in industrial applications, it may constitute an improvement over other magnetic patterning methods.
- ItemStrong and ductile high temperature soft magnets through Widmanstätten precipitates([London] : Nature Publishing Group UK, 2023) Han, Liuliu; Maccari, Fernando; Soldatov, Ivan; Peter, Nicolas J.; Souza Filho, Isnaldi R.; Schäfer, Rudolf; Gutfleisch, Oliver; Li, Zhiming; Raabe, DierkFast growth of sustainable energy production requires massive electrification of transport, industry and households, with electrical motors as key components. These need soft magnets with high saturation magnetization, mechanical strength, and thermal stability to operate efficiently and safely. Reconciling these properties in one material is challenging because thermally-stable microstructures for strength increase conflict with magnetic performance. Here, we present a material concept that combines thermal stability, soft magnetic response, and high mechanical strength. The strong and ductile soft ferromagnet is realized as a multicomponent alloy in which precipitates with a large aspect ratio form a Widmanstätten pattern. The material shows excellent magnetic and mechanical properties at high temperatures while the reference alloy with identical composition devoid of precipitates significantly loses its magnetization and strength at identical temperatures. The work provides a new avenue to develop soft magnets for high-temperature applications, enabling efficient use of sustainable electrical energy under harsh operating conditions.
- ItemIntegrated molecular diode as 10 MHz half-wave rectifier based on an organic nanostructure heterojunction([London] : Nature Publishing Group UK, 2020) Li, Tianming; Bandari, Vineeth Kumar; Hantusch, Martin; Xin, Jianhui; Kuhrt, Robert; Ravishankar, Rachappa; Xu, Longqian; Zhang, Jidong; Knupfer, Martin; Zhu, Feng; Yan, Donghang; Schmidt, Oliver G.Considerable efforts have been made to realize nanoscale diodes based on single molecules or molecular ensembles for implementing the concept of molecular electronics. However, so far, functional molecular diodes have only been demonstrated in the very low alternating current frequency regime, which is partially due to their extremely low conductance and the poor degree of device integration. Here, we report about fully integrated rectifiers with microtubular soft-contacts, which are based on a molecularly thin organic heterojunction and are able to convert alternating current with a frequency of up to 10 MHz. The unidirectional current behavior of our devices originates mainly from the intrinsically different surfaces of the bottom planar and top microtubular Au electrodes while the excellent high frequency response benefits from the charge accumulation in the phthalocyanine molecular heterojunction, which not only improves the charge injection but also increases the carrier density.
- ItemCollapse of layer dimerization in the photo-induced hidden state of 1T-TaS2([London] : Nature Publishing Group UK, 2020) Stahl, Quirin; Kusch, Maximilian; Heinsch, Florian; Garbarino, Gaston; Kretzschmar, Norman; Hanff, Kerstin; Rossnagel, Kai; Geck, Jochen; Ritschel, TobiasPhoto-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently, very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2, where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here, we characterize the hidden quantum state of 1T-TaS2 by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of interlayer molecular orbital dimers as a key mechanism for this non-thermal collective transition between two truly long-range ordered electronic crystals.
- ItemUltrathin positively charged electrode skin for durable anion-intercalation battery chemistries([London] : Nature Publishing Group UK, 2023) Sabaghi, Davood; Wang, Zhiyong; Bhauriyal, Preeti; Lu, Qiongqiong; Morag, Ahiud; Mikhailovia, Daria; Hashemi, Payam; Li, Dongqi; Neumann, Christof; Liao, Zhongquan; Dominic, Anna Maria; Nia, Ali Shaygan; Dong, Renhao; Zschech, Ehrenfried; Turchanin, Andrey; Heine, Thomas; Yu, Minghao; Feng, XinliangThe anion-intercalation chemistries of graphite have the potential to construct batteries with promising energy and power breakthroughs. Here, we report the use of an ultrathin, positively charged two-dimensional poly(pyridinium salt) membrane (C2DP) as the graphite electrode skin to overcome the critical durability problem. Large-area C2DP enables the conformal coating on the graphite electrode, remarkably alleviating the electrolyte. Meanwhile, the dense face-on oriented single crystals with ultrathin thickness and cationic backbones allow C2DP with high anion-transport capability and selectivity. Such desirable anion-transport properties of C2DP prevent the cation/solvent co-intercalation into the graphite electrode and suppress the consequent structure collapse. An impressive PF6−-intercalation durability is demonstrated for the C2DP-covered graphite electrode, with capacity retention of 92.8% after 1000 cycles at 1 C and Coulombic efficiencies of > 99%. The feasibility of constructing artificial ion-regulating electrode skins with precisely customized two-dimensional polymers offers viable means to promote problematic battery chemistries.
- ItemEvidence of two-dimensional flat band at the surface of antiferromagnetic kagome metal FeSn([London] : Nature Publishing Group UK, 2021) Han, Minyong; Inoue, Hisashi; Fang, Shiang; John, Caolan; Ye, Linda; Chan, Mun K.; Graf, David; Suzuki, Takehito; Ghimire, Madhav Prasad; Cho, Won Joon; Kaxiras, Efthimios; Checkelsky, Joseph G.The kagome lattice has long been regarded as a theoretical framework that connects lattice geometry to unusual singularities in electronic structure. Transition metal kagome compounds have been recently identified as a promising material platform to investigate the long-sought electronic flat band. Here we report the signature of a two-dimensional flat band at the surface of antiferromagnetic kagome metal FeSn by means of planar tunneling spectroscopy. Employing a Schottky heterointerface of FeSn and an n-type semiconductor Nb-doped SrTiO3, we observe an anomalous enhancement in tunneling conductance within a finite energy range of FeSn. Our first-principles calculations show this is consistent with a spin-polarized flat band localized at the ferromagnetic kagome layer at the Schottky interface. The spectroscopic capability to characterize the electronic structure of a kagome compound at a thin film heterointerface will provide a unique opportunity to probe flat band induced phenomena in an energy-resolved fashion with simultaneous electrical tuning of its properties. Furthermore, the exotic surface state discussed herein is expected to manifest as peculiar spin-orbit torque signals in heterostructure-based spintronic devices.