Dr.jens.brede
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[Report] Composition-matched molecular “solders” for semiconductors
Adsorption and STM imaging of polycyclic aromatic hydrocarbons on graphene
Author(s): Y. J. Dappe, M. Andersen, R. Balog, L. Hornekær, and X. Bouju
The structural characterization of polycyclic aromatic hydrocarbon molecules adsorbed on graphene is of fundamental importance in view of the use of graphene or graphene nanoribbons for electronic applications. Before reaching this point, one has to determine the structure of the adsorbed molecules....
[Phys. Rev. B 91, 045427] Published Thu Jan 22, 2015
Interplay of weak interactions in the atom-by-atom condensation of xenon within quantum boxes
Article
Condensation in the regime of weakly interactions is of fundamental importance. Here, the authors study the condensation process one atom at a time, showing the forces driving the behaviour of xenon atoms as they condense into aggregate structures in nanoscale pores.
Nature Communications doi: 10.1038/ncomms7071
Authors: Sylwia Nowakowska, Aneliia Wäckerlin, Shigeki Kawai, Toni Ivas, Jan Nowakowski, Shadi Fatayer, Christian Wäckerlin, Thomas Nijs, Ernst Meyer, Jonas Björk, Meike Stöhr, Lutz H. Gade, Thomas A. Jung
Alternating Copolymerization of Propylene Oxide with Biorenewable Terpene-Based Cyclic Anhydrides: A Sustainable Route to Aliphatic Polyesters with High Glass Transition Temperatures
Abstract
The alternating copolymerization of propylene oxide with terpene-based cyclic anhydrides catalyzed by chromium, cobalt, and aluminum salen complexes is reported. The use of the Diels–Alder adduct of α-terpinene and maleic anhydride as the cyclic anhydride comonomer results in amorphous polyesters that exhibit glass transition temperatures (Tg) of up to 109 °C. The polymerization conditions and choice of catalyst have a dramatic impact on the molecular weight distribution, the relative stereochemistry of the diester units along the polymer chain, and ultimately the Tg of the resulting polymer. The aluminum salen complex exhibits exceptional selectivity for copolymerization without transesterification or epimerization side reactions. The resulting polyesters are highly alternating and have high molecular weights and narrow polydispersities.
Terpene-based cyclic anhydrides are copolymerized with propylene oxide using metal salen catalysts to provide amorphous aliphatic polyesters with exceptionally high glass transition temperatures (Tg up to 109 °C). The polymerization conditions and choice of catalyst have a dramatic impact on the microstructure and ultimately the Tg value of the resulting polymer.
Many-body transitions in a single molecule visualized by scanning tunnelling microscopy
Nature Physics. doi:10.1038/nphys3212
Authors: Fabian Schulz, Mari Ijäs, Robert Drost, Sampsa K. Hämäläinen, Ari Harju, Ari P. Seitsonen & Peter Liljeroth
Many-body effects arise from the collective behaviour of large numbers of interacting particles, for example, electrons, and the properties of such a system cannot be understood considering only single or non-interacting particles. Despite the generality of the many-body picture, there are only a few examples of experimentally observing such effects in molecular systems. Measurements of the local density of states of single molecules by scanning tunnelling spectroscopy is usually interpreted in terms of single-particle molecular orbitals. Here, we show that the simple single-particle picture fails qualitatively to account for the resonances in the tunnelling spectra of different charge states of cobalt phthalocyanine molecules. Instead, these resonances can be understood as a series of many-body excitations of the different ground states of the molecule. Our theoretical approach opens an accessible route beyond the single-particle picture in quantifying many-body states in molecules.
Direct Observation of Graphene Growth and Associated Copper Substrate Dynamics by in Situ Scanning Electron Microscopy
Synthesis of Large and Few Atomic Layers of Hexagonal Boron Nitride on Melted Copper
Hexagonal boron nitride nanosheets (h-BNNS) have been proposed as an ideal substrate for graphene-based electronic devices, but the synthesis of large and homogeneous h-BNNS is still challenging. In this contribution, we report a facile synthesis of few-layer h-BNNS on melted copper via an atmospheric pressure chemical vapor deposition process. Comparative studies confirm the advantage of using melted copper over solid copper as a catalyst substrate. The former leads to the formation of single crystalline h-BNNS that is several microns in size and mostly in mono- and bi-layer forms, in contrast to the polycrystalline and mixed multiple layers (1–10) yielded by the latter. This difference is likely to be due to the significantly reduced and uniformly distributed nucleation sites on the smooth melted surface, in contrast to the large amounts of unevenly distributed nucleation sites that are associated with grain boundaries and other defects on the solid surface. This synthesis is expected to contribute to the development of large-scale manufacturing of h-BNNS/graphene-based electronics.
Scientific Reports 5 doi: 10.1038/srep07743
Effect of focused ion beam deposition induced contamination on the transport properties of nano devices
Discretized Topological Hall Effect Emerging from Skyrmions in Constricted Geometry. (arXiv:1501.03290v1 [cond-mat.str-el])
We investigate the skyrmion formation process in nano-structured FeGe Hall-bar devices by measurements of topological Hall effect, which extracts the winding number of a spin texture as an emergent magnetic field. Step-wise profiles of topological Hall resistivity are observed in the course of varying the applied magnetic field, which arise from instantaneous changes in the magnetic nano-structure such as creation, annihilation, and jittering motion of skyrmions. The discrete changes in topological Hall resistivity demonstrate the quantized nature of emergent magnetic flux inherent in each skyrmion, which had been indistinguishable in many-skyrmion systems on a macroscopic scale.
Direct observation of electron propagation and dielectric screening on the atomic length scale
Direct observation of electron propagation and dielectric screening on the atomic length scale
Nature 517, 7534 (2015). doi:10.1038/nature14094
Authors: S. Neppl, R. Ernstorfer, A. L. Cavalieri, C. Lemell, G. Wachter, E. Magerl, E. M. Bothschafter, M. Jobst, M. Hofstetter, U. Kleineberg, J. V. Barth, D. Menzel, J. Burgdörfer, P. Feulner, F. Krausz & R. Kienberger
The propagation and transport of electrons in crystals is a fundamental process pertaining to the functioning of most electronic devices. Microscopic theories describe this phenomenon as being based on the motion of Bloch wave packets. These wave packets are superpositions of individual Bloch states with the group velocity determined by the dispersion of the electronic band structure near the central wavevector in momentum space. This concept has been verified experimentally in artificial superlattices by the observation of Bloch oscillations—periodic oscillations of electrons in real and momentum space. Here we present a direct observation of electron wave packet motion in a real-space and real-time experiment, on length and time scales shorter than the Bloch oscillation amplitude and period. We show that attosecond metrology (1 as = 10−18 seconds) now enables quantitative insight into weakly disturbed electron wave packet propagation on the atomic length scale without being hampered by scattering effects, which inevitably occur over macroscopic propagation length scales. We use sub-femtosecond (less than 10−15 seconds) extreme-ultraviolet light pulses to launch photoelectron wave packets inside a tungsten crystal that is covered by magnesium films of varied, well-defined thicknesses of a few ångströms. Probing the moment of arrival of the wave packets at the surface with attosecond precision reveals free-electron-like, ballistic propagation behaviour inside the magnesium adlayer—constituting the semi-classical limit of Bloch wave packet motion. Real-time access to electron transport through atomic layers and interfaces promises unprecedented insight into phenomena that may enable the scaling of electronic and photonic circuits to atomic dimensions. In addition, this experiment allows us to determine the penetration depth of electrical fields at optical frequencies at solid interfaces on the atomic scale.
Cu(110) Surface in Hydrochloric Acid Solution: Potential Dependent Chloride Adsorption and Surface Restructuring
Electronic Interaction between Nitrogen Atoms in Doped Graphene
Reversible Hydrogenation of Graphene on Ni(111)—Synthesis of “Graphone”
Abstract
Understanding the adsorption and reaction between hydrogen and graphene is of fundamental importance for developing graphene-based concepts for hydrogen storage and for the chemical functionalization of graphene by hydrogenation. Recently, theoretical studies of single-sided hydrogenated graphene, so called graphone, predicted it to be a promising semiconductor for applications in graphene-based electronics. Here, we report on the synthesis of graphone bound to a Ni(111) surface. We investigate the formation process by X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption (TPD), and density-functional theory calculations, showing that the hydrogenation of graphene with atomic hydrogen indeed leads to graphone, that is, a hydrogen coverage of 1 ML (4.2 wt %). The dehydrogenation of graphone reveals complex desorption processes that are attributed to coverage-dependent changes in the activation energies for the associative desorption of hydrogen as molecular H2.
Hydrogen on graphene on nickel: The hydrogenation of graphene on a nickel (111) substrate leads to the formation of single-sided graphane, also called graphone (see scheme). The hydrogenation of graphene leading to graphone and the complex dehydrogenation of graphone are investigated by X-ray photoelectron spectroscopy, temperature-programmed desorption and ab initio density functional theory calculations.
Adatoms underneath Single Porphyrin Molecules on Au(111)
Electromechanical response at polar zigzag boundaries in hybrid monolayers
Author(s): Rafael Martinez-Gordillo and Miguel Pruneda
First-principles calculations are used to demonstrate electromechanical control of charge and spin at zigzag-edged interfaces between graphene and boron-nitride domains in hybrid monolayers. We show how, through a direct piezoelectric effect, the interfacial bound charges and associated electric fie...
[Phys. Rev. B 91, 045411] Published Fri Jan 09, 2015
Probing of valley polarization in graphene via optical second-harmonic generation
Author(s): T. O. Wehling, A. Huber, A. I. Lichtenstein, and M. I. Katsnelson
Valley polarization in graphene breaks inversion symmetry and therefore leads to second-harmonic generation. We present a complete theory of this effect within a single-particle approximation. It is shown that this may be a sensitive tool to measure the valley polarization created, e.g., by polarize...
[Phys. Rev. B 91, 041404] Published Fri Jan 09, 2015
Stabilizing CuPc Coordination Networks on Ag(100) by Ag Atoms
High-Resolution Model for Noncontact Atomic Force Microscopy with a Flexible Molecule on the Tip Apex
Confinement of massless Dirac fermions in the graphene matrix induced by the B/N heteroatoms
DOI: 10.1039/C4CP05193A, Paper
The p-/n-type massless Dirac fermions are confined around an extended 1-D defect in graphene.
The content of this RSS Feed (c) The Royal Society of Chemistry
The O-P-O bridged Mn2(salen)2 chains showing coexistence of single chain magnet and metamagnet behaviour
DOI: 10.1039/C4DT03888F, Paper
Three chain compounds in which the Mn2(salen)2 dimers are bridged by O-P-O units are reported, two of which display coexistence of SCM behavior and metamagnetism at low temperature.
The content of this RSS Feed (c) The Royal Society of Chemistry
Atomistic mechanisms for bilayer growth of graphene on metal substrates
Author(s): Wei Chen, Ping Cui, Wenguang Zhu, Efthimios Kaxiras, Yanfei Gao, and Zhenyu Zhang
Epitaxial growth on metal substrates has been shown to be the most powerful approach in producing large-scale high-quality monolayer graphene, yet it remains a major challenge to realize uniform bilayer graphene growth. Here we carry out a comparative study of the atomistic mechanisms for bilayer gr...
[Phys. Rev. B 91, 045408] Published Thu Jan 08, 2015
Strain engineering Dirac surface states in heteroepitaxial topological crystalline insulator thin films. (arXiv:1501.01299v1 [cond-mat.mes-hall])
In newly discovered topological crystalline insulators (TCIs), the unique crystalline protection of the surface state (SS) band structure has led to a series of intriguing predictions of strain generated phenomena, from the appearance of pseudo-magnetic fields and helical flat bands, to the tunability of the Dirac SS by strain that may be used to construct "straintronic" nanoswitches. However, practical realization of this exotic phenomenology via strain engineering is experimentally challenging and is yet to be achieved. In this work, we have designed an experiment to not only generate and measure strain locally, but to also directly measure the resulting effects on the Dirac SS. We grow heteroepitaxial thin films of TCI SnTe in-situ and measure them by using high-resolution scanning tunneling microscopy (STM). Large STM images were analyzed to determine picoscale changes in the atomic positions which reveal regions of both tensile and compressive strain. Simultaneous Fourier-transform STM was then used to determine the effects of strain on the Dirac electrons. We find that strain continuously tunes the momentum space position of the Dirac points, consistent with theoretical predictions. Our work demonstrates the fundamental mechanism necessary for using TCIs in strain-based applications, and establishes these systems as highly tunable platforms for nanodevices.
Probing dynamics and pinning of single vortices in superconductors at nanometer scales
The dynamics of quantized magnetic vortices and their pinning by materials defects determine electromagnetic properties of superconductors, particularly their ability to carry non-dissipative currents. Despite recent advances in the understanding of the complex physics of vortex matter, the behavior of vortices driven by current through a multi-scale potential of the actual materials defects is still not well understood, mostly due to the scarcity of appropriate experimental tools capable of tracing vortex trajectories on nanometer scales. Using a novel scanning superconducting quantum interference microscope we report here an investigation of controlled dynamics of vortices in lead films with sub-Angstrom spatial resolution and unprecedented sensitivity. We measured, for the first time, the fundamental dependence of the elementary pinning force of multiple defects on the vortex displacement, revealing a far more complex behavior than has previously been recognized, including striking spring softening and broken-spring depinning, as well as spontaneous hysteretic switching between cellular vortex trajectories. Our results indicate the importance of thermal fluctuations even at 4.2 K and of the vital role of ripples in the pinning potential, giving new insights into the mechanisms of magnetic relaxation and electromagnetic response of superconductors.
Scientific Reports 5 doi: 10.1038/srep07598
Shot Noise as a Probe of Spin-Polarized Transport through Single Atoms
Author(s): Andreas Burtzlaff, Alexander Weismann, Mads Brandbyge, and Richard Berndt
Measurements of the shot noise through a gold STM tip contacted to a gold adatom reveal the open spin-polarized transport channels between the tip and the surface underneath.
[Phys. Rev. Lett. 114, 016602] Published Tue Jan 06, 2015
Control of quantum magnets by atomic exchange bias
Nature Nanotechnology 10, 40 (2015). doi:10.1038/nnano.2014.281
Authors: Shichao Yan, Deung-Jang Choi, Jacob A. J. Burgess, Steffen Rolf-Pissarczyk & Sebastian Loth
Mixing of discretized states in quantum magnets has a radical impact on their properties. Managing this effect is key for spintronics in the quantum limit. Magnetic fields can modify state mixing and, for example, mitigate destabilizing effects in single-molecule magnets. The exchange bias field has been proposed as a mechanism for localized control of individual nanomagnets. Here, we demonstrate that exchange coupling with the magnetic tip of a scanning tunnelling microscope provides continuous tuning of spin state mixing in an individual nanomagnet. By directly measuring spin relaxation time with electronic pump–probe spectroscopy, we find that the exchange interaction acts analogously to a local magnetic field that can be applied to a specific atom. It can be tuned in strength by up to several tesla and cancel external magnetic fields, thereby demonstrating the feasibility of complete control over individual quantum magnets with atomically localized exchange coupling.
Multipartite Einstein–Podolsky–Rosen steering and genuine tripartite entanglement with optical networks
Nature Physics. doi:10.1038/nphys3202
Authors: Seiji Armstrong, Meng Wang, Run Yan Teh, Qihuang Gong, Qiongyi He, Jiri Janousek, Hans-Albert Bachor, Margaret D. Reid & Ping Koy Lam
Einstein, Podolsky and Rosen (EPR) pointed out in their famous paradox that two quantum-entangled particles can have perfectly correlated positions and momenta. Such correlations give evidence for the nonlocality of quantum mechanics and form the basis for quantum cryptography and teleportation. EPR steering is the nonlocality associated with the EPR paradox and has traditionally been investigated between only two parties. Using optical networks and efficient detection, we present experimental observations of multiparty EPR steering and of the genuine entanglement of three intense optical beams. We entangle the quadrature phase amplitudes of distinct fields, in analogy to the position–momentum entanglement of the original paradox. Our experiments complement tests of quantum mechanics that have entangled small systems or have demonstrated tripartite inseparability. Our methods establish principles for the development of multiparty quantum communication protocols with asymmetric observers, and can be extended to qubits, whether photonic, atomic, superconducting, or otherwise.
[Review] Graphene, related two-dimensional crystals, and hybrid systems for energy conversion and storage
Temperature-Driven Changes of the Graphene Edge Structure on Ni(111): Substrate vs Hydrogen Passivation
Modeling Ferro- and Antiferromagnetic Interactions in Metal–Organic Coordination Networks
Tuning the magnetic anisotropy of single molecules. (arXiv:1412.7454v2 [cond-mat.mes-hall] UPDATED)
The magnetism of single atoms and molecules is governed by the atomic scale environment. In general, the reduced symmetry of the surrounding splits the $d$ states and aligns the magnetic moment along certain favorable directions. Here, we show that we can reversibly modify the magnetocrystalline anisotropy by manipulating the environment of single iron(II) porphyrin molecules adsorbed on Pb(111) with the tip of a scanning tunneling microscope. When we decrease the tip--molecule distance, we first observe a small increase followed by an exponential decrease of the axial anisotropy on the molecules. This is in contrast to the monotonous increase observed earlier for the same molecule with an additional axial Cl ligand. We ascribe the changes in the anisotropy of both species to a deformation of the molecules in the presence of the attractive force of the tip, which leads to a change in the $d$ level alignment. These experiments demonstrate the feasibility of a precise tuning of the magnetic anisotropy of an individual molecule by mechanical control.







