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- 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).
- 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.
- ItemCoupled mechanical oscillator enables precise detection of nanowire flexural vibrations(London : Springer Nature, 2023) Sharma, Maneesha; Sathyadharma Prasad, Aniruddha; Freitag, Norbert H.; Büchner, Bernd; Mühl, ThomasThe field of nanowire (NW) technology represents an exciting and steadily growing research area with applications in ultra-sensitive mass and force sensing. Existing detection methods for NW deflection and oscillation include optical and field emission approaches. However, they are challenging for detecting small diameter NWs because of the heating produced by the laser beam and the impact of the high electric field. Alternatively, the deflection of a NW can be detected indirectly by co-resonantly coupling the NW to a cantilever and measuring it using a scanning probe microscope. Here, we prove experimentally that co-resonantly coupled devices are sensitive to small force derivatives similar to standalone NWs. We detect force derivatives as small as 10−9 N/m with a bandwidth of 1 Hz at room temperature. Furthermore, the measured hybrid vibration modes show clear signatures of avoided crossing. The detection technique presented in this work verifies a major step in boosting NW-based force and mass sensing.
- ItemSimultaneous magnetic field and field gradient mapping of hexagonal MnNiGa by quantitative magnetic force microscopy(London : Springer Nature, 2023) Freitag, Norbert H.; Reiche, Christopher F.; Neu, Volker; Devi, Parul; Burkhardt, Ulrich; Felser, Claudia; Wolf, Daniel; Lubk, Axel; Büchner, Bernd; Mühl, ThomasMagnetic force microscopy (MFM) is a scanning microscopy technique that is commonly employed to probe the sample’s magnetostatic stray fields via their interaction with a magnetic probe tip. In this work, a quantitative, single-pass MFM technique is presented that maps one magnetic stray-field component and its spatial derivative at the same time. This technique uses a special cantilever design and a special high-aspect-ratio magnetic interaction tip that approximates a monopole-like moment. Experimental details, such as the control scheme, the sensor design, which enables simultaneous force and force gradient measurements, as well as the potential and limits of the monopole description of the tip moment are thoroughly discussed. To demonstrate the merit of this technique for studying complex magnetic samples it is applied to the examination of polycrystalline MnNiGa bulk samples. In these experiments, the focus lies on mapping and analyzing the stray-field distribution of individual bubble-like magnetization patterns in a centrosymmetric [001] MnNiGa phase. The experimental data is compared to calculated and simulated stray-field distributions of 3D magnetization textures, and, furthermore, bubble dimensions including diameters are evaluated. The results indicate that the magnetic bubbles have a significant spatial extent in depth and a buried bubble top base.
- ItemElastoresistivity of Heavily Hole-Doped 122 Iron Pnictide Superconductors(Lausanne : Frontiers Media, 2022) Hong, Xiaochen; Sykora, Steffen; Caglieris, Federico; Behnami, Mahdi; Morozov, Igor; Aswartham, Saicharan; Grinenko, Vadim; Kihou, Kunihiro; Lee, Chul-Ho; Büchner, Bernd; Hess, ChristianNematicity in heavily hole-doped iron pnictide superconductors remains controversial. Sizeable nematic fluctuations and even nematic orders far from magnetic instability were declared in RbFe2As2 and its sister compounds. Here, we report a systematic elastoresistance study of a series of isovalent- and electron-doped KFe2As2 crystals. We found divergent elastoresistance on cooling for all the crystals along their [110] direction. The amplitude of elastoresistivity diverges if K is substituted with larger ions or if the system is driven toward a Lifshitz transition. However, we conclude that none of them necessarily indicates an independent nematic critical point. Instead, the increased nematicity can be associated with another electronic criticality. In particular, we propose a mechanism for how elastoresistivity is enhanced at a Lifshitz transition.
- ItemInterplay of charge density waves, disorder, and superconductivity in 2H-TaSe2 elucidated by NMR([London] : IOP, 2022) Baek, Seung-Ho; Sur, Yeahan; Kim, Kee Hoon; Vojta, Matthias; Büchner, BerndSingle crystals of pristine and 6% Pd-intercalated 2H‐TaSe2 have been studied by means of 77Se nuclear magnetic resonance. The temperature dependence of the 77Se spectrum, with an unexpected line narrowing upon Pd intercalation, unravels the presence of correlated local lattice distortions far above the transition temperature of the charge density wave (CDW) order, thereby supporting a strong-coupling CDW mechanism in 2H‐TaSe2. While, the Knight shift data suggest that the incommensurate CDW transition involves a partial Fermi surface gap opening. As for spin dynamics, the 77Se spin-lattice relaxation rate T1-1 as a function of temperature shows that a pseudogap behavior dominates the low-energy spin excitations even within the CDW phase, and gets stronger along with superconductivity in the Pd-6% sample. We discuss that CDW fluctuations may be responsible for the pseudogap as well as superconductivity, although the two phenomena are unlikely to be directly linked each other.