Browsing by Author "Knupfer, M."
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- ItemAbsorption and photoemission spectroscopy of rare-earth oxypnictides(Milton Park : Taylor & Francis, 2009) Kroll, T.; Roth, F.; Koitzsch, A.; Kraus, R.; Batchelor, D.R.; Werner, J.; Behr, G.; Büchner, B.; Knupfer, M.The electronic structure of various rare-earth oxypnictides has been investigated by performing Fe L2, 3 x-ray absorption spectroscopy, and Fe 2p and valence band x-ray photoemission spectroscopy. As representative samples the non-superconducting parent compounds LnFeAsO (Ln=La, Ce, Sm and Gd) have been chosen and measured at 25 and 300 K, i.e. below and above the structural and magnetic phase transition at ~150 K. We find no significant change of the electronic structure of the FeAs layers when switching between the different rare-earth ions or when varying the temperature below and above the transition temperatures. Using a simple two-configuration model, we find qualitative agreement with the Fe 2p3/2 core-level spectrum, which allows for a qualitative explanation of the experimental spectral shapes.
- ItemElectronic properties of intercalated single-wall carbon nanotubes and C60 peapods(Milton Park : Taylor & Francis, 2003) Pichler, T.; Liu, X.; Knupfer, M.; Fink, J.This paper reviews recent investigations of the electronic structure and the optical properties of intercalated single-wall carbon nanotubes (SWCNTs) and C60 filled SWCNTs (peapods) using electron energy-loss spectroscopy (EELS) in transmission as a probe. The results from these one-dimensional nanostructures are compared to C60 fullerides and intercalated graphite, which are well understood prototypes of carbon-based intercalation compounds. In detail, the structural changes were analysed by electron diffraction and the doping level and the matrix element weighted unoccupied density of states (DOS) by an analysis of the C 1s core-level excitations. Regarding the optical properties, the intercalation gives rise to a charge transfer to the peapods (SWCNTs) which leads to the formation of a free charge carrier plasmon in the loss function which is analysed within the framework of an effective Drude–Lorentz model.
- ItemEvolution of the charge carrier plasmon in the one-dimensional metal TTF-TCNQ as a function of temperature and momentum(Bristol : Institute of Physics Publishing, 2019) Kovbasa, N.; Graf, L.; Knupfer, M.We have investigated the charge carrier plasmon in the quasi one-dimensional metal TTF-TCNQ using electron energy-loss spectroscopy. Our data reveal a negative plasmon dispersion with a slope that is independent of temperature, which is in agreement to predictions from model calculations and previous room temperature data. A plasmon energy shift upon temperature is observed, and we discuss possible contributions to this shift. The spectral width of the plasmon is rather temperature independent, but increases clearly above a momentum value of about 0.3 Å-1.
- ItemIntertwined electronic and magnetic structure of the van-der-Waals antiferromagnet Fe2P2S6([London] : Nature Publishing Group, 2023) Koitzsch, A.; Klaproth, T.; Selter, S.; Shemerliuk, Y.; Aswartham, S.; Janson, O.; Büchner, B.; Knupfer, M.Many unusual and promising properties have been reported recently for the transition metal trichalcogenides of the type MPS3 (M = V, Mn, Fe, Ni..), such as maintaining magnetic order to the atomically thin limit, ultra-sharp many-body excitons, metal-insulator transitions and, especially for Fe2P2S6, giant linear dichroism among others. Here we conduct a detailed investigation of the electronic structure of Fe2P2S6 using angle-resolved photoemission spectroscopy, q-dependent electron energy loss spectroscopy, optical spectroscopies and density functional theory. Fe2P2S6 is a Mott insulator with a gap of E gap ≈ 1.4 eV and zigzag antiferromagnetism below T N = 119 K. The low energy excitations are dominated by Fe 3d states. Large and sign-changing linear dichroism is observed. We provide a microscopic mechanism explaining key properties of the linear dichroism based on the correlated character of the electronic structure, thereby elucidating the nature of the spin-charge coupling in Fe2P2S6 and related materials.
- ItemMomentum-resolved superconducting gap in the bulk of Ba1-xK xFe2As2 from combined ARPES and μSR measurements(Milton Park : Taylor & Francis, 2009) Evtushinsky, D.V.; Inosov, D.S.; Zabolotnyy, V.B.; Viazovska, M.S.; Khasanov, R.; Amato, A.; Klauss, H.-H.; Luetkens, H.; Niedermayer, Ch.; Sun, G.L.; Hinkov, V.; Lin, C.T.; Varykhalov, A.; Koitzsch, A.; Knupfer, M.; Büchner, B.; Kordyuk, A.A.; Borisenko, S.V.Here we present a calculation of the temperature-dependent London penetration depth, λ(T), in Ba1-xKxFe 2As2 (BKFA) on the basis of the electronic band structure (Zabolotnyy et al 2009 Nature 457 569, Zabolotnyy et al 2009 Physica C 469 448) and momentum-dependent superconducting gap (Evtushinsky et al 2009 Phys. Rev. B 79 054517) extracted from angleresolved photoemission spectroscopy (ARPES) data. The results are compared to the direct measurements of λ(T) by muon spin rotation (μSR) (Khasanov et al 2009 Phys. Rev. Lett. 102 187005). The value of λ(T = 0), calculated with no adjustable parameters, equals 270 nm, while the directly measured one is 320 nm; the temperature dependence λ(T) is also easily reproduced. Such agreement between the two completely different approaches allows us to conclude that ARPES studies of BKFA are bulk-representative. Our review of the available experimental studies of the superconducting gap in the new ironbased superconductors in general allows us to state that most of them bear two nearly isotropic gaps with coupling constants 2ΔkBTc = 2.5±1.5 and 7±2.
- ItemNesting-driven multipolar order in CeB6 from photoemission tomography(London : Nature Publishing Group, 2016) Koitzsch, A.; Heming, N.; Knupfer, M.; Büchner, B.; Portnichenko, P.Y.; Dukhnenko, A.V.; Shitsevalova, N.Y.; Filipov, V.B.; Lev, L.L.Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order.
- 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.
- ItemOrbital and spin effects for the upper critical field in As-deficient disordered Fe pnictide superconductors(Milton Park : Taylor & Francis, 2009) Fuchs, G.; Drechsler, S.-L.; Kozlova, N.; Bartkowiak, M.; Hamann-Borrero, J.E.; Behr, G.; Nenkov, K.; Klauss, H.-H.; Maeter, H.; Amato, A.; Luetkens, H.; Kwadrin, A.; Khasanov, R.; Freudenberger, J.; Köhler, A.; Knupfer, M.; Arushanov, E.; Rosner, H.; Büchner, B.; Schultz, L.We report upper critical field Bc2(T) data for LaO0.9F0.1FeAs1- δ in a wide temperature and field range up to 60 T. The large slope of Bc2≈- 5.4 to -6.6 T K-1 near an improved Tc≈28.5 K of the in-plane Bc2(T) contrasts with a flattening starting near 23 K above 30 T we regard as the onset of Pauli-limited behaviour (PLB) with Bc2(0)≈63–68 T. We interpret a similar hitherto unexplained flattening of the Bc2(T) curves reported for at least three other disordered closely related systems, Co-doped BaFe2As2, (Ba,K) Fe2As2 and NdO0.7F0.3FeAs (all single crystals), for applied fields H∥(a,b), also as a manifestation of PLB. Their Maki parameters have been estimated by analysing their Bc2(T) data within the Werthamer–Helfand–Hohenberg approach. The pronounced PLB of (Ba, K)Fe2As2 single crystals obtained from an Sn flux is attributed also to a significant As deficiency detected by wavelength dispersive x-ray spectroscopy as reported by Ni et al (2008 Phys. Rev. B 78 014507). Consequences of our results are discussed in terms of disorder effects within conventional superconductivity (CSC) and unconventional superconductivity (USC). USC scenarios with nodes on individual Fermi surface sheets (FSS), e.g. p- and d-wave SC, can be discarded for our samples. The increase of dBc2/dT|Tc by sizeable disorder provides evidence for an important intraband (intra-FSS) contribution to the orbital upper critical field. We suggest that it can be ascribed either to an impurity-driven transition from s± USC to CSC of an extended s++-wave state or to a stabilized s±-state provided As-vacancies cause predominantly strong intraband scattering in the unitary limit. We compare our results with Bc2 data from the literature, which often show no PLB for fields below 60–70 T probed so far. A novel disorder-related scenario of a complex interplay of SC with two different competing magnetic instabilities is suggested.
- ItemSpectromicroscopic measurements of electronic structure variations in atomically thin WSe2(2020) Klaproth, T.; Habenicht, C.; Schuster, R.; Büchner, B.; Knupfer, M.; Koitzsch, A.Atomically thin transition metal dichalcogenides (TMDCs) are promising candidates for implementation in next generation semiconducting devices, for which laterally homogeneous behavior is needed. Here, we study the electronic structure of atomically thin exfoliated WSe2, a prototypical TMDC with large spin–orbit coupling, by photoemission electron microscopy, electron energy-loss spectroscopy, and density functional theory. We resolve the inhomogeneities of the doping level by the varying energy positions of the valence band. There appear to be different types of inhomogeneities that respond differently to electron doping, introduced by potassium intercalation. In addition, we find that the doping process itself is more complex than previously anticipated and entails a distinct orbital and thickness dependence that needs to be considered for effective band engineering. In particular, the density of selenium vs tungsten states depends on the doping level, which leads to changes in the optical response beyond increased dielectric screening. Our work gives insight into the inhomogeneity of the electron structure of WSe2 and the effects of electron doping, provides microscopic understanding thereof, and improves the basis for property engineering of 2D materials.
- ItemTunable charge transfer properties in metal-phthalocyanine heterojunctions(Cambridge : Royal Society of Chemistry, 2016) Siles, P.F.; Hahn, T.; Salvan, G.; Knupfer, M.; Zhu, F.; Zahn, D.R.T.; Schmidt, O.G.Organic materials such as phthalocyanine-based systems present a great potential for organic device applications due to the possibility of integrating films of different organic materials to create organic heterostructures which combine the electrical capabilities of each material. This opens the possibility to precisely engineer and tune new electrical properties. In particular, similar transition metal phthalocyanines demonstrate hybridization and charge transfer properties which could lead to interesting physical phenomena. Although, when considering device dimensions, a better understanding and control of the tuning of the transport properties still remain in the focus of research. Here, by employing conductive atomic force microscopy techniques, we provide an insight about the nanoscale electrical properties and transport mechanisms of MnPc and fluorinated phthalocyanines such as F16CuPc and F16CoPc. We report a transition from typical diode-like transport mechanisms for pure MnPc thin films to space-charge-limited current transport regime (SCLC) for Pc-based heterostructures. The controlled addition of fluorinated phthalocyanine also provides highly uniform and symmetric-polarized transport characteristics with conductance enhancements up to two orders of magnitude depending on the polarization. We present a method to spatially map the mobility of the MnPc/F16CuPc structures with a nanoscale resolution and provide theoretical calculations to support our experimental findings. This well-controlled nanoscale tuning of the electrical properties for metal transition phthalocyanine junctions stands as key step for future phthalocyanine-based electronic devices, where the low dimension charge transfer, mediated by transition metal atoms could be intrinsically linked to a transfer of magnetic moment or spin.