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- ItemNanowire-supported plasmonic waveguide for remote excitation of surface-enhanced Raman scattering(London : Nature Publishing Group, 2014) Huang, Y.; Fang, Y.; Zhang, Z.; Zhu, L.; Sun, M.Due to its amazing ability to manipulate light at the nanoscale, plasmonics has become one of the most interesting topics in the field of light-matter interaction. As a promising application of plasmonics, surface-enhanced Raman scattering (SERS) has been widely used in scientific investigations and material analysis. The large enhanced Raman signals are mainly caused by the extremely enhanced electromagnetic field that results from localized surface plasmon polaritons. Recently, a novel SERS technology called remote SERS has been reported, combining both localized surface plasmon polaritons and propagating surface plasmon polaritons (PSPPs, or called plasmonic waveguide), which may be found in prominent applications in special circumstances compared to traditional local SERS. In this article, we review the mechanism of remote SERS and its development since it was first reported in 2009. Various remote metal systems based on plasmonic waveguides, such as nanoparticle-nanowire systems, single nanowire systems, crossed nanowire systems and nanowire dimer systems, are introduced, and recent novel applications, such as sensors, plasmon-driven surface-catalyzed reactions and Raman optical activity, are also presented. Furthermore, studies of remote SERS in dielectric and organic systems based on dielectric waveguides remind us that this useful technology has additional, tremendous application prospects that have not been realized in metal systems.
- ItemPromoting abnormal grain growth in Fe-based shape memory alloys through compositional adjustments(London : Nature Publishing Group, 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.
- ItemDiscovery of TaFeSb-based half-Heuslers with high thermoelectric performance(London : Nature Publishing Group, 2019) Zhu, H.; Mao, J.; Li, Y.; Sun, J.; Wang, Y.; Zhu, Q.; Li, G.; Song, Q.; Zhou, J.; Fu, Y.; He, R.; Tong, T.; Liu, Z.; Ren, W.; You, L.; Wang, Z.; Luo, J.; Sotnikov, A.; Bao, J.; Nielsch, K.; Chen, G.; Singh, D.J.; Ren, Z.Discovery of thermoelectric materials has long been realized by the Edisonian trial and error approach. However, recent progress in theoretical calculations, including the ability to predict structures of unknown phases along with their thermodynamic stability and functional properties, has enabled the so-called inverse design approach. Compared to the traditional materials discovery, the inverse design approach has the potential to substantially reduce the experimental efforts needed to identify promising compounds with target functionalities. By adopting this approach, here we have discovered several unreported half-Heusler compounds. Among them, the p-type TaFeSb-based half-Heusler demonstrates a record high ZT of ~1.52 at 973 K. Additionally, an ultrahigh average ZT of ~0.93 between 300 and 973 K is achieved. Such an extraordinary thermoelectric performance is further verified by the heat-to-electricity conversion efficiency measurement and a high efficiency of ~11.4% is obtained. Our work demonstrates that the TaFeSb-based half-Heuslers are highly promising for thermoelectric power generation.
- 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.
- ItemDivalent EuRh 2 Si 2 as a reference for the Luttinger theorem and antiferromagnetism in trivalent heavy-fermion YbRh 2 Si 2(London : Nature Publishing Group, 2019) Güttler, M.; Generalov, A.; Fujimori, S.I.; Kummer, K.; Chikina, A.; Seiro, S.; Danzenbächer, S.; Koroteev, Y.M.; Chulkov, E.V.; Radovic, M.; Shi, M.; Plumb, N.C.; Laubschat, C.; Allen, J.W.; Krellner, C.; Geibel, C.; Vyalikh, D.V.Application of the Luttinger theorem to the Kondo lattice YbRh 2 Si 2 suggests that its large 4f-derived Fermi surface (FS) in the paramagnetic (PM) regime should be similar in shape and volume to that of the divalent local-moment antiferromagnet (AFM) EuRh 2 Si 2 in its PM regime. Here we show by angle-resolved photoemission spectroscopy that paramagnetic EuRh 2 Si 2 has a large FS essentially similar to the one seen in YbRh 2 Si 2 down to 1 K. In EuRh 2 Si 2 the onset of AFM order below 24.5 K induces an extensive fragmentation of the FS due to Brillouin zone folding, intersection and resulting hybridization of the Fermi-surface sheets. Our results on EuRh 2 Si 2 indicate that the formation of the AFM state in YbRh 2 Si 2 is very likely also connected with similar changes in the FS, which have to be taken into account in the controversial analysis and discussion of anomalies observed at the quantum critical point in this system.
- ItemEmerging 2D-ferromagnetism and strong spin-orbit coupling at the surface of valence-fluctuating EuIr2Si2(London : Nature Publishing Group, 2019) Schulz, S.; Nechaev, I.A.; Güttler, M.; Poelchen, G.; Generalov, A.; Danzenbächer, S.; Chikina, A.; Seiro, S.; Kliemt, K.; Vyazovskaya, A.Y.; Kim, T.K.; Dudin, P.; Chulkov, E.V.; Laubschat, C.; Krasovskii, E.E.; Geibel, C.; Krellner, C.; Kummer, K.; Vyalikh, D.V.The development of materials that are non-magnetic in the bulk but exhibit two-dimensional (2D) magnetism at the surface is at the core of spintronics applications. Here, we present the valence-fluctuating material EuIr2Si2, where in contrast to its non-magnetic bulk, the Si-terminated surface reveals controllable 2D ferromagnetism. Close to the surface the Eu ions prefer a magnetic divalent configuration and their large 4f moments order below 48 K. The emerging exchange interaction modifies the spin polarization of the 2D surface electrons originally induced by the strong Rashba effect. The temperature-dependent mixed valence of the bulk allows to tune the energy and momentum size of the projected band gaps to which the 2D electrons are confined. This gives an additional degree of freedom to handle spin-polarized electrons at the surface. Our findings disclose valence-fluctuating rare-earth based materials as a very promising basis for the development of systems with controllable 2D magnetic properties which is of interest both for fundamental science and applications.
- ItemProbing the reconstructed Fermi surface of antiferromagnetic BaFe2As2 in one domain(London : Nature Publishing Group, 2019) Watson, M.D.; Dudin, P.; Rhodes, L.C.; Evtushinsky, D.V.; Iwasawa, H.; Aswartham, S.; Wurmehl, S.; Büchner, B.; Hoesch, M.; Kim, T.K.A fundamental part of the puzzle of unconventional superconductivity in the Fe-based superconductors is the understanding of the magnetic and nematic instabilities of the parent compounds. The issues of which of these can be considered the leading instability, and whether weak- or strong-coupling approaches are applicable, are both critical and contentious. Here, we revisit the electronic structure of BaFe2As2 using angle-resolved photoemission spectroscopy (ARPES). Our high-resolution measurements of samples “detwinned” by the application of a mechanical strain reveal a highly anisotropic 3D Fermi surface in the low-temperature antiferromagnetic phase. By comparison of the observed dispersions with ab initio calculations, we argue that overall it is magnetism, rather than orbital/nematic ordering, which is the dominant effect, reconstructing the electronic structure across the Fe 3d bandwidth. Finally, using a state-of-the-art nano-ARPES system, we reveal how the observed electronic dispersions vary in real space as the beam spot crosses domain boundaries in an unstrained sample, enabling the measurement of ARPES data from within single antiferromagnetic domains, and showing consistence with the effective mono-domain samples obtained by detwinning.
- ItemStrong spin resonance mode associated with suppression of soft magnetic ordering in hole-doped Ba1-xNaxFe2As2(London : Nature Publishing Group, 2019) Waßer, F.; Park, J.T.; Aswartham, S.; Wurmehl, S.; Sidis, Y.; Steffens, P.; Schmalzl, K.; Büchner, B.; Braden, M.Spin-resonance modes (SRM) are taken as evidence for magnetically driven pairing in Fe-based superconductors, but their character remains poorly understood. The broadness, the splitting and the spin-space anisotropies of SRMs contrast with the mostly accepted interpretation as spin excitons. We study hole-doped Ba1−xNaxFe2As2 that displays a spin reorientation transition. This reorientation has little impact on the overall appearance of the resonance excitations with a high-energy isotropic and a low-energy anisotropic mode. However, the strength of the anisotropic low-energy mode sharply peaks at the highest doping that still exhibits magnetic ordering resulting in the strongest SRM observed in any Fe-based superconductor so far. This remarkably strong SRM is accompanied by a loss of about half of the magnetic Bragg intensity upon entering the SC phase. Anisotropic SRMs thus can allow the system to compensate for the loss of exchange energy arising from the reduced antiferromagnetic correlations within the SC state.
- ItemNonlocal dielectric function and nested dark excitons in MoS2(London : Nature Publishing Group, 2019) Koitzsch, A.; Pawlik, A.-S.; Habenicht, C.; Klaproth, T.; Schuster, R.; Büchner, B.; Knupfer, M.Their exceptional optical properties are a driving force for the persistent interest in atomically thin transition metal dichalcogenides such as MoS2. The optical response is dominated by excitons. Apart from the bright excitons, which directly couple to light, it has been realized that dark excitons, where photon absorption or emission is inhibited by the spin state or momentum mismatch, are decisive for many optical properties. However, in particular the momentum dependence is difficult to assess experimentally and often remains elusive or is investigated by indirect means. Here we study the momentum dependent electronic structure experimentally and theoretically. We use angle-resolved photoemission as a one-particle probe of the occupied valence band structure and electron energy loss spectroscopy as a two-particle probe of electronic transitions across the gap to benchmark a single-particle model of the dielectric function ϵ(q, ω) against momentum dependent experimental measurements. This ansatz captures key aspects of the data surprisingly well. In particular, the energy region where substantial nesting occurs, which is at the origin of the strong light–matter interaction of thin transition metal dichalcogenides and crucial for the prominent C-exciton, is described well and spans a more complex exciton landscape than previously anticipated. Its local maxima in (q≠0,ω) space can be considered as dark excitons and might be relevant for higher order optical processes. Our study may lead to a more complete understanding of the optical properties of atomically thin transition metal dichalcogenides.
- ItemUltrafast high-resolution mass spectrometric finger pore imaging in latent finger prints(London : Nature Publishing Group, 2014) Elsner, C.; Abel, B.Latent finger prints (LFPs) are deposits of sweat components in ridge and groove patterns, left after human fingers contact with a surface. Being important targets in biometry and forensic investigations they contain more information than topological patterns. With laser desorption mass spectrometry imaging (LD-MSI) we record 'three-dimensional' finger prints with additional chemical information as the third dimension. Here we show the potential of fast finger pore imaging (FPI) in latent finger prints employing LD-MSI without a classical matrix in a high-spatial resolution mode. Thin films of gold rapidly sputtered on top of the sample are used for desorption. FPI employing an optical image for rapid spatial orientation and guiding of the desorption laser enables the rapid analysis of individual finger pores, and the chemical composition of their excretions. With this approach we rapidly detect metabolites, drugs, and characteristic excretions from the inside of the human organism by a minimally-invasive strategy, and distinguish them from chemicals in contact with fingers without any labeling. The fast finger pore imaging, analysis, and screening approach opens the door for a vast number of novel applications in such different fields as forensics, doping and medication control, therapy, as well as rapid profiling of individuals.
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