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- ItemExperimental proof of Joule heating-induced switched-back regions in OLEDs(London : Nature Publishing Group, 2020) Kirch, Anton; Fische, Axel; Liero, Matthias; Fuhrmann, Jürgen; Glitzky, Annegret; Reineke, SebastianOrganic light-emitting diodes (OLEDs) have become a major pixel technology in the display sector, with products spanning the entire range of current panel sizes. The ability to freely scale the active area to large and random surfaces paired with flexible substrates provides additional application scenarios for OLEDs in the general lighting, automotive, and signage sectors. These applications require higher brightness and, thus, current density operation compared to the specifications needed for general displays. As extended transparent electrodes pose a significant ohmic resistance, OLEDs suffering from Joule self-heating exhibit spatial inhomogeneities in electrical potential, current density, and hence luminance. In this article, we provide experimental proof of the theoretical prediction that OLEDs will display regions of decreasing luminance with increasing driving current. With a two-dimensional OLED model, we can conclude that these regions are switched back locally in voltage as well as current due to insufficient lateral thermal coupling. Experimentally, we demonstrate this effect in lab-scale devices and derive that it becomes more severe with increasing pixel size, which implies its significance for large-area, high-brightness use cases of OLEDs. Equally, these non-linear switching effects cannot be ignored with respect to the long-term operation and stability of OLEDs; in particular, they might be important for the understanding of sudden-death scenarios. © 2020, The Author(s).
- ItemDirect molecular-level near-field plasmon and temperature assessment in a single plasmonic hotspot(London : Nature Publishing Group, 2020) Richard-Lacroix, Marie; Deckert, VolkerTip-enhanced Raman spectroscopy (TERS) is currently widely recognized as an essential but still emergent technique for exploring the nanoscale. However, our lack of comprehension of crucial parameters still limits its potential as a user-friendly analytical tool. The tip’s surface plasmon resonance, heating due to near-field temperature rise, and spatial resolution are undoubtedly three challenging experimental parameters to unravel. However, they are also the most fundamentally relevant parameters to explore, because they ultimately influence the state of the investigated molecule and consequently the probed signal. Here we propose a straightforward and purely experimental method to access quantitative information of the plasmon resonance and near-field temperature experienced exclusively by the molecules directly contributing to the TERS signal. The detailed near-field optical response, both at the molecular level and as a function of time, is evaluated using standard TERS experimental equipment by simultaneously probing the Stokes and anti-Stokes spectral intensities. Self-assembled 16-mercaptohexadodecanoic acid monolayers covalently bond to an ultra-flat gold surface were used as a demonstrator. Observation of blinking lines in the spectra also provides crucial information on the lateral resolution and indication of atomic-scale thermally induced morphological changes of the tip during the experiment. This study provides access to unprecedented molecular-level information on physical parameters that crucially affect experiments under TERS conditions. The study thereby improves the usability of TERS in day-to-day operation. The obtained information is of central importance for any experimental plasmonic investigation and for the application of TERS in the field of nanoscale thermometry. © 2020, The Author(s).
- ItemSingle-photon emission from isolated monolayer islands of InGaN(London : Nature Publishing Group, 2020) Sun, Xiaoxiao; Wang, Ping; Wang, Tao; Chen, Ling; Chen, Zhaoying; Gao, Kang; Aoki, Tomoyuki; Li, Mo; Zhang, Jian; Schulz, Tobias; Albrecht, Martin; Ge, Weikun; Arakawa, Yasuhiko; Shen, Bo; Holmes, Mark; Wang, XinqiangWe identify and characterize a novel type of quantum emitter formed from InGaN monolayer islands grown using molecular beam epitaxy and further isolated via the fabrication of an array of nanopillar structures. Detailed optical analysis of the characteristic emission spectrum from the monolayer islands is performed, and the main transmission is shown to act as a bright, stable, and fast single-photon emitter with a wavelength of ~400 nm. © 2020, The Author(s).
- ItemRelativistic-intensity near-single-cycle light waveforms at kHz repetition rate(London : Nature Publishing Group, 2020) Ouillé, Marie; Vernier, Aline; Böhle, Frederik; Bocoum, Maïmouna; Jullien, Aurélie; Lozano, Magali; Rousseau, Jean-Philippe; Cheng, Zhao; Gustas, Dominykas; Blumenstein, Andreas; Simon, Peter; Haessler, Stefan; Faure, Jérôme; Nagy, Tamas; Lopez-Martens, RodrigoThe development of ultra-intense and ultra-short light sources is currently a subject of intense research driven by the discovery of novel phenomena in the realm of relativistic optics, such as the production of ultrafast energetic particle and radiation beams for applications. It has been a long-standing challenge to unite two hitherto distinct classes of light sources: those achieving relativistic intensity and those with pulse durations approaching a single light cycle. While the former class traditionally involves large-scale amplification chains, the latter class places high demand on the spatiotemporal control of the electromagnetic laser field. Here, we present a light source producing waveform-controlled 1.5-cycle pulses with a 719 nm central wavelength that can be focused to relativistic intensity at a 1 kHz repetition rate based on nonlinear post-compression in a long hollow-core fiber. The unique capabilities of this source allow us to observe the first experimental indications of light waveform effects in laser wakefield acceleration of relativistic energy electrons. © 2020, The Author(s).
- ItemObservation of giant spin-split Fermi-arc with maximal Chern number in the chiral topological semimetal PtGa(London : Nature Publishing Group, 2020) Yao, M.; Manna, K.; Yang, Q.; Fedorov, A.; Voroshnin, V.; Valentin Schwarze, B.; Hornung, J.; Chattopadhyay, S.; Sun, Z.; Guin, S.N.; Wosnitza, J.; Borrmann, H.; Shekhar, C.; Kumar, N.; Fink, J.; Sun, Y.; Felser, C.Non-symmorphic chiral topological crystals host exotic multifold fermions, and their associated Fermi arcs helically wrap around and expand throughout the Brillouin zone between the high-symmetry center and surface-corner momenta. However, Fermi-arc splitting and realization of the theoretically proposed maximal Chern number rely heavily on the spin-orbit coupling (SOC) strength. In the present work, we investigate the topological states of a new chiral crystal, PtGa, which has the strongest SOC among all chiral crystals reported to date. With a comprehensive investigation using high-resolution angle-resolved photoemission spectroscopy, quantum-oscillation measurements, and state-of-the-art ab initio calculations, we report a giant SOC-induced splitting of both Fermi arcs and bulk states. Consequently, this study experimentally confirms the realization of a maximal Chern number equal to ±4 in multifold fermionic systems, thereby providing a platform to observe large-quantized photogalvanic currents in optical experiments.
- ItemSeparate tuning of nematicity and spin fluctuations to unravel the origin of superconductivity in FeSe(London : Nature Publishing Group, 2020) Baek, S.-H.; Ok, J.M.; Kim, J.S.; Aswartham, S.; Morozov, I.; Chareev, D.; Urata, T.; Tanigaki, K.; Tanabe, Y.; Büchner, B.; Efremov, D.V.The interplay of orbital and spin degrees of freedom is the fundamental characteristic in numerous condensed matter phenomena, including high-temperature superconductivity, quantum spin liquids, and topological semimetals. In iron-based superconductors (FeSCs), this causes superconductivity to emerge in the vicinity of two other instabilities: nematic and magnetic. Unveiling the mutual relationship among nematic order, spin fluctuations, and superconductivity has been a major challenge for research in FeSCs, but it is still controversial. Here, by carrying out 77Se nuclear magnetic resonance (NMR) measurements on FeSe single crystals, doped by cobalt and sulfur that serve as control parameters, we demonstrate that the superconducting transition temperature Tc increases in proportion to the strength of spin fluctuations, while it is independent of the nematic transition temperature Tnem. Our observation therefore directly implies that superconductivity in FeSe is essentially driven by spin fluctuations in the intermediate coupling regime, while nematic fluctuations have a marginal impact on Tc.
- ItemTurning charge-density waves into Cooper pairs(London : Nature Publishing Group, 2020) Chikina, A.; Fedorov, A.; Bhoi, D.; Voroshnin, V.; Haubold, E.; Kushnirenko, Y.; Kim, K.H.; Borisenko, S.The relationship between charge-density waves (CDWs) and superconductivity is a long-standing debate. Often observed as neighbors in phase diagrams, it is still unclear whether they cooperate, compete, or simply coexist. Using angle-resolved photoemission spectroscopy, we demonstrate here that by tuning the energy position of the van Hove singularity in Pd-doped 2H-TaSe2, one is able to suppress CDW and enhance superconductivity by more than an order of magnitude. We argue that it is particular fermiology of the material that is responsible for each phenomenon, thus explaining their persistent proximity as phases.
- ItemComprehensive scan for nonmagnetic Weyl semimetals with nonlinear optical response(London : Nature Publishing Group, 2020) Xu, Q.; Zhang, Y.; Koepernik, K.; Shi, W.; van den Brink, J.; Felser, C.; Sun, Y.First-principles calculations have recently been used to develop comprehensive databases of nonmagnetic topological materials that are protected by time-reversal or crystalline symmetry. However, owing to the low symmetry requirement of Weyl points, a symmetry-based approach to identifying topological states cannot be applied to Weyl semimetals (WSMs). To date, WSMs with Weyl points in arbitrary positions are absent from the well-known databases. In this work, we develop an efficient algorithm to search for Weyl points automatically and establish a database of nonmagnetic WSMs with Weyl points near the Fermi level based on the experimental non-centrosymmetric crystal structures in the Inorganic Crystal Structure Database (ICSD). In total, 46 Weyl semimetals were discovered to have nearly clean Fermi surfaces and Weyl points within 300 meV of the Fermi level. Nine of them are chiral structures which may exhibit the quantized circular photogalvanic effect. In addition, the nonlinear optical response is studied and the giant shift current is explored. Besides nonmagnetic WSMs, our powerful tools can also be used in the discovery of magnetic topological materials.
- ItemImproved kinetic behaviour of Mg(NH2)2-2LiH doped with nanostructured K-modified-LixTiyOz for hydrogen storage(London : Nature Publishing Group, 2020) Gizer, G.; Puszkiel, J.; Riglos, M.V.C.; Pistidda, C.; Ramallo-López, J.M.; Mizrahi, M.; Santoru, A.; Gemming, T.; Tseng, J.-C.; Klassen, T.; Dornheim, M.The system Mg(NH2)2 + 2LiH is considered as an interesting solid-state hydrogen storage material owing to its low thermodynamic stability of ca. 40 kJ/mol H2 and high gravimetric hydrogen capacity of 5.6 wt.%. However, high kinetic barriers lead to slow absorption/desorption rates even at relatively high temperatures (>180 °C). In this work, we investigate the effects of the addition of K-modified LixTiyOz on the absorption/desorption behaviour of the Mg(NH2)2 + 2LiH system. In comparison with the pristine Mg(NH2)2 + 2LiH, the system containing a tiny amount of nanostructured K-modified LixTiyOz shows enhanced absorption/desorption behaviour. The doped material presents a sensibly reduced (∼30 °C) desorption onset temperature, notably shorter hydrogen absorption/desorption times and reversible hydrogen capacity of about 3 wt.% H2 upon cycling. Studies on the absorption/desorption processes and micro/nanostructural characterizations of the Mg(NH2)2 + 2LiH + K-modified LixTiyOz system hint to the fact that the presence of in situ formed nanostructure K2TiO3 is the main responsible for the observed improved kinetic behaviour.
- ItemIncreased static dielectric constant in ZnMnO and ZnCoO thin films with bound magnetic polarons(London : Nature Publishing Group, 2020) Vegesna, S.V.; Bhat, V.J.; Bürger, D.; Dellith, J.; Skorupa, I.; Schmidt, O.G.; Schmidt, H.A novel small signal equivalent circuit model is proposed in the inversion regime of metal/(ZnO, ZnMnO, and ZnCoO) semiconductor/Si3N4 insulator/p-Si semiconductor (MSIS) structures to describe the distinctive nonlinear frequency dependent capacitance (C-F) and conductance (G-F) behaviour in the frequency range from 50 Hz to 1 MHz. We modelled the fully depleted ZnO thin films to extract the static dielectric constant (εr) of ZnO, ZnMnO, and ZnCoO. The extracted enhancement of static dielectric constant in magnetic n-type conducting ZnCoO (εr ≥ 13.0) and ZnMnO (εr ≥ 25.8) in comparison to unmagnetic ZnO (εr = 8.3–9.3) is related to the electrical polarizability of donor-type bound magnetic polarons (BMP) in the several hundred GHz range (120 GHz for CdMnTe). The formation of donor-BMP is enabled in n-type conducting, magnetic ZnO by the s-d exchange interaction between the electron spin of positively charged oxygen vacancies Vo+ in the BMP center and the electron spins of substitutional Mn2+ and Co2+ ions in ZnMnO and ZnCoO, respectively. The BMP radius scales with the Bohr radius which is proportional to the static dielectric constant. Here we show how BMP overlap can be realized in magnetic n-ZnO by increasing its static dielectric constant and guide researchers in the field of transparent spintronics towards ferromagnetism in magnetic, n-ZnO.