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- ItemLong-range magnetic order in the ~S=1/2 triangular lattice antiferromagnet KCeS2(Amsterdam : SciPost Foundation, 2020) Bastien, Gaël; Rubrecht, Bastian; Haeussler, Ellen; Schlender, Philipp; Zangeneh, Ziba; Avdoshenko, Stanislav; Sarkar, Rajib; Alfonsov, Alexey; Luther, Sven; Onykiienko, Yevhen A.; Walker, Helen C.; Kühne, Hannes; Grinenko, Vadim; Guguchia, Zurab; Kataev, Vladislav; Klauss, Hans-Henning; Hozoi, Liviu; van den Brink, Jeroen; Inosov, Dmytro S.; Büchner, Bernd; Wolter, Anja U.B.; Doert, ThomasRecently, several putative quantum spin liquid (QSL) states were discovered in ~S=1/2 rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS2 and show via low-temperature specific heat and μSR investigations that it yields magnetic order below TN=0.38 K despite the same delafossite structure. We identify a well separated ~S=1/2 ground state for KCeS2 from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane g~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS2.
- ItemRobust Single Molecule Magnet Monolayers on Graphene and Graphite with Magnetic Hysteresis up to 28 K(Weinheim : Wiley-VCH, 2021) Spree, Lukas; Liu, Fupin; Neu, Volker; Rosenkranz, Marco; Velkos, Georgios; Wang, Yaofeng; Schiemenz, Sandra; Dreiser, Jan; Gargiani, Pierluigi; Valvidares, Manuel; Chen, Chia-Hsiang; Büchner, Bernd; Avdoshenko, Stanislav M.; Popov, Alexey A.The chemical functionalization of fullerene single molecule magnet Tb2@C80(CH2Ph) enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite from solution without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K. The use of pyrene terminated linker molecules opens the way to devise integration of spin carrying units encapsulated by fullerene cages on graphitic substrates, be it single-molecule magnets or qubit candidates. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemTailoring Plasmonics of Au@Ag Nanoparticles by Silica Encapsulation(Weinheim : Wiley-VCH, 2021) Schultz, Johannes; Kirner, Felizitas; Potapov, Pavel; Büchner, Bernd; Lubk, Axel; Sturm, Elena V.Hybrid metallic nanoparticles (NPs) encapsulated in oxide shells are currently intensely studied for plasmonic applications in sensing, medicine, catalysis, and photovoltaics. Here, a method for the synthesis of Au@Ag@SiO2 cubes with a uniform silica shell of variable and adjustable thickness in the nanometer range is introduced and their excellent, highly reproducible, and tunable optical response is demonstrated. Varying the silica shell thickness, the excitation energies of the single NP plasmon modes can be tuned in a broad spectral range between 2.55 and 3.25 eV. Most importantly, a strong coherent coupling of the surface plasmons is revealed at the silver–silica interface with Mie resonances at the silica–vacuum interface leading to a significant field enhancement at the encapsulated NP surface in the range of 100% at shell thicknesses t ≃ 20 nm. Consequently, the synthesis method and the field enhancement open pathways to a widespread use of silver NPs in plasmonic applications including photonic crystals and may be transferred to other non-precious metals. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemExciton dispersion in para-quaterphenyl: Significant molecular interactions beyond Coulomb coupling(New York, NY : American Inst. of Physics, 2021) Graf, Lukas; Krupskaya, Yulia; Büchner, Bernd; Knupfer, MartinWe have experimentally determined the momentum dependence of the electronic excitation spectra of para-quaterphenyl single crystals. The parallel arrangement of para-quaterphenyl molecules results in a strong Coulomb coupling of the molecular excitons. Such crystals have been considered to be a very good realization of the Frenkel exciton model, including the formation of H-type aggregates. Our data reveal an unexpected exciton dispersion of the upper Davydov component, which cannot be rationalized in terms of inter-molecular Coulomb coupling of the excitons. A significant reduction of the nearest neighbor coupling due to additional charge-transfer processes is able to provide an explanation of the data. Furthermore, the spectral onset of the excitation spectrum, which represents a heavy exciton resulting from exciton-phonon coupling, also shows a clear dispersion, which had been unknown so far. Finally, an optically forbidden excitation about 1 eV above the excitation onset is observed. © 2021 Author(s).
- ItemSixfold fermion near the Fermi level in cubic PtBi2(Amsterdam : SciPost Foundation, 2021) Thirupathaiah, Setti; Kushnirenko, Yevhen; Koepernik, Klaus; Piening, Boy Roman; Büchner, Bernd; Aswartham, Saicharan; van den Brink, Jeroen; Borisenko, Sergey; Fulga, Ion CosmaWe show that the cubic compound PtBi2, is a topological semimetal hosting a sixfold band touching point in close proximity to the Fermi level. Using angle-resolved photoemission spectroscopy, we map the bandstructure of the system, which is in good agreement with results from density functional theory. Further, by employing a low energy effective Hamiltonian valid close to the crossing point, we study the effect of a magnetic field on the sixfold fermion. The latter splits into a total of twenty Weyl cones for a Zeeman field oriented in the diagonal, [111] direction. Our results mark cubic PtBi2, as an ideal candidate to study the transport properties of gapless topological systems beyond Dirac and Weyl semimetals.
- ItemCharge transfer characteristics of F6TCNNQ–gold interface(Chichester [u.a.] : Wiley, 2020) Kuhrt, Robert; Hantusch, Martin; Knupfer, Martin; Büchner, BerndThe metal–organic interface between polycrystalline gold and hexafluorotetracyanonaphthoquinodimethane (F6TCNNQ) was investigated by photoelectron spectroscopy with the focus on the charge transfer characteristics from the metal to the molecule. The valence levels, as well as the core levels of the heterojunction, indicate a full electron transfer and a change in the chemical environment. The changes are observed in the first F6TCNNQ layers, whereas for further film growth, only neutral F6TCNNQ molecules could be detected. New occupied states below the Fermi level were observed in the valence levels, indicating a lowest unoccupied molecular orbital (LUMO) occupation due to the charge transfer. A fitting of the spectra reveals the presence of a neutral and a charged F6TCNNQ molecules, but no further species were present.
- ItemAxion Mie theory of electron energy loss spectroscopy in topological insulators(Amsterdam : SciPost Foundation, 2021) Schultz, Johannes; Nogueira, Flavio S.; Büchner, Bernd; van den Brink, Jeroen; Lubk, AxelElectronic topological states of matter exhibit novel types of responses to electromagnetic fields. The response of strong topological insulators, for instance, is characterized by a so-called axion term in the electromagnetic Lagrangian which is ultimately due to the presence of topological surface states. Here we develop the axion Mie theory for the electromagnetic response of spherical particles including arbitrary sources of fields, i.e., charge and current distributions. We derive an axion induced mixing of transverse magnetic and transverse electric modes which are experimentally detectable through small induced rotations of the field vectors. Our results extend upon previous analyses of the problem. Our main focus is on the experimentally relevant problem of electron energy loss spectroscopy in topological insulators, a technique that has so far not yet been used to detect the axion electromagnetic response in these materials.
- ItemSuppression of nematicity by tensile strain in multilayer FeSe/SrTiO3 films(College Park, MD : APS, 2023) Lou, Rui; Suvorov, Oleksandr; Grafe, Hans-Joachim; Kuibarov, Andrii; Krivenkov, Maxim; Rader, Oliver; Büchner, Bernd; Borisenko, Sergey; Fedorov, AlexanderThe nematicity in multilayer FeSe/SrTiO3 films has been previously suggested to be enhanced with decreasing film thickness. Motivated by this, there have been many discussions about the competing relation between nematicity and superconductivity. However, the criterion for determining the nematicity strength in FeSe remains highly debated. The understanding of nematicity as well as its relation to superconductivity in FeSe films is therefore still controversial. Here, we fabricate multilayer FeSe/SrTiO3 films using molecular beam epitaxy and study the nematic properties by combining angle-resolved photoemission spectroscopy, Se77 nuclear magnetic resonance, and scanning tunneling microscopy experiments. We unambiguously demonstrate that, near the interface, the nematic order is suppressed by the SrTiO3-induced tensile strain; in the bulk region further away from the interface, the strength of nematicity recovers to the bulk value. Our results not only solve the recent controversy about the nematicity in multilayer FeSe films, but also offer valuable insights into the relationship between nematicity and superconductivity.
- ItemAutocorrected off-axis holography of two-dimensional materials(College Park, ML : American Physical Society, 2020) Kern, Felix; Linck, Martin; Wolf, Daniel; Alem, Nasim; Arora, Himani; Gemming, Sibylle; Erbe, Artur; Zettl, Alex; Büchner, Bernd; Lubk, AxelThe reduced dimensionality in two-dimensional materials leads to a wealth of unusual properties, which are currently explored for both fundamental and applied sciences. In order to study the crystal structure, edge states, the formation of defects and grain boundaries, or the impact of adsorbates, high-resolution microscopy techniques are indispensable. Here we report on the development of an electron holography (EH) transmission electron microscopy (TEM) technique, which facilitates high spatial resolution by an automatic correction of geometric aberrations. Distinguished features of EH beyond conventional TEM imaging are gap-free spatial information signal transfer and higher dose efficiency for certain spatial frequency bands as well as direct access to the projected electrostatic potential of the two-dimensional material. We demonstrate these features with the example of h-BN, for which we measure the electrostatic potential as a function of layer number down to the monolayer limit and obtain evidence for a systematic increase of the potential at the zig-zag edges.
- ItemChirality coupling in topological magnetic textures with multiple magnetochiral parameters([London] : Nature Publishing Group UK, 2023) Volkov, Oleksii M.; Wolf, Daniel; Pylypovskyi, Oleksandr V.; Kákay, Attila; Sheka, Denis D.; Büchner, Bernd; Fassbender, Jürgen; Lubk, Axel; Makarov, DenysChiral effects originate from the lack of inversion symmetry within the lattice unit cell or sample’s shape. Being mapped onto magnetic ordering, chirality enables topologically non-trivial textures with a given handedness. Here, we demonstrate the existence of a static 3D texture characterized by two magnetochiral parameters being magnetic helicity of the vortex and geometrical chirality of the core string itself in geometrically curved asymmetric permalloy cap with a size of 80 nm and a vortex ground state. We experimentally validate the nonlocal chiral symmetry breaking effect in this object, which leads to the geometric deformation of the vortex string into a helix with curvature 3 μm−1 and torsion 11 μm−1. The geometric chirality of the vortex string is determined by the magnetic helicity of the vortex texture, constituting coupling of two chiral parameters within the same texture. Beyond the vortex state, we anticipate that complex curvilinear objects hosting 3D magnetic textures like curved skyrmion tubes and hopfions can be characterized by multiple coupled magnetochiral parameters, that influence their statics and field- or current-driven dynamics for spin-orbitronics and magnonics.