Dr.jens.brede

Author(s): Michael Ruby, Yang Peng, Felix von Oppen, Benjamin W. Heinrich, and Katharina J. Franke

We investigate the nature of Yu-Shiba-Rusinov (YSR) subgap states induced by single manganese (Mn) atoms adsorbed on different surface orientations of superconducting lead (Pb). Depending on the adsorption site, we detect a distinct number and characteristic patterns of YSR states around the Mn atom…

[Phys. Rev. Lett. 117, 186801] Published Mon Oct 24, 2016

Nematic quantum fluids with wave functions that break the underlying crystalline symmetry can form in interacting electronic systems. We examined the quantum Hall states that arise in high magnetic fields from anisotropic hole pockets on the Bi(111) surface. Spectroscopy performed with a scanning tunneling microscope showed that a combination of single-particle effects and many-body Coulomb interactions lift the six-fold Landau level (LL) degeneracy to form three valley-polarized quantum Hall states. We imaged the resulting anisotropic LL wave functions and found that they have a different orientation for each broken-symmetry state. The wave functions correspond to those expected from pairs of hole valleys and provide a direct spatial signature of a nematic electronic phase. Authors: Benjamin E. Feldman, Mallika T. Randeria, András Gyenis, Fengcheng Wu, Huiwen Ji, R. J. Cava, Allan H. MacDonald, Ali Yazdani

Author(s): D. Van Tuan, J. M. Marmolejo-Tejada, X. Waintal, B. K. Nikolić, S. O. Valenzuela, and S. Roche

Recent experiments reporting an unexpectedly large spin Hall effect (SHE) in graphene decorated with adatoms have raised a fierce controversy. We apply numerically exact Kubo and Landauer-Büttiker formulas to realistic models of gold-decorated disordered graphene (including adatom clustering) to obt…

[Phys. Rev. Lett. 117, 176602] Published Thu Oct 20, 2016

Nature Materials. doi:10.1038/nmat4760

Authors: Allegra A. Latimer, Ambarish R. Kulkarni, Hassan Aljama, Joseph H. Montoya, Jong Suk Yoo, Charlie Tsai, Frank Abild-Pedersen, Felix Studt & Jens K. Nørskov

While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C–H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.

Author(s): Yu Zhang, Si-Yu Li, Huaqing Huang, Wen-Tian Li, Jia-Bin Qiao, Wen-Xiao Wang, Long-Jing Yin, Ke-Ke Bai, Wenhui Duan, and Lin He

Pristine graphene is strongly diamagnetic. However, graphene with single carbon atom defects could exhibit paramagnetism. Theoretically, the π magnetism induced by the monovacancy in graphene is characteristic of two spin-split density-of-states (DOS) peaks close to the Dirac point. Since its predic…

[Phys. Rev. Lett. 117, 166801] Published Mon Oct 10, 2016

This book chapter reviews the experimental evidence for magnetic phenomena at the LaAlO3/SrTiO3 interface. We argue that essentially all of the signatures of magnetism can be sorted into two distinct categories: (1) magnetic phases (e.g., ferromagnetic or Kondo) involving local magnetic moments and their coupling to itinerant electrons; (2) metamagnetic effects that are mediated by attractive electron-electron interactions that do not involve local moments. We review possible candidates for the local moments that give rise to the ferromagnetic phases and focus on arguments for one potential source: oxygen vacancies. For the metamagnetic transport signatures, band-structure effects (e.g., Lifshitz transition) and strong attractive electron-electron interaction can help consolidate disparate experimental findings.

Nature advance online publication 03 October 2016. doi:10.1038/nature19765

Authors: Hiroshi Imada, Kuniyuki Miwa, Miyabi Imai-Imada, Shota Kawahara, Kensuke Kimura & Yousoo Kim

Given its central role in photosynthesis and artificial energy-harvesting devices, energy transfer has been widely studied using optical spectroscopy to monitor excitation dynamics and probe the molecular-level control of energy transfer between coupled molecules. However, the spatial resolution of conventional optical spectroscopy is limited to a few hundred nanometres and thus cannot reveal the nanoscale spatial features associated with such processes. In contrast, scanning tunnelling luminescence spectroscopy has revealed the energy dynamics associated with phenomena ranging from single-molecule electroluminescence, absorption of localized plasmons and quantum interference effects to energy delocalization and intervalley electron scattering with submolecular spatial resolution in real space. Here we apply this technique to individual molecular dimers that comprise a magnesium phthalocyanine and a free-base phthalocyanine (MgPc and H2Pc) and find that locally exciting MgPc with the tunnelling current of the scanning tunnelling microscope generates a luminescence signal from a nearby H2Pc molecule as a result of resonance energy transfer from the former to the latter. A reciprocating resonance energy transfer is observed when exciting the second singlet state (S2) of H2Pc, which results in energy transfer to the first singlet state (S1) of MgPc and final funnelling to the S1 state of H2Pc. We also show that tautomerization of H2Pc changes the energy transfer characteristics within the dimer system, which essentially makes H2Pc a single-molecule energy transfer valve device that manifests itself by blinking resonance energy transfer behaviour.

Conventional logic and memory devices are built out of deterministic units such as transistors, or magnets with energy barriers in excess of 40-60 kT. We show that stochastic units, p-bits, can be interconnected to create robust correlations that implement Boolean functions with impressive accuracy, comparable to standard circuits. Also they are invertible, a unique property that is absent in digital circuits. When operated in the direct mode, the input is clamped, and the network provides the correct output. In the inverted mode, the output is clamped, and the network fluctuates among possible inputs consistent with that output. We present an implementation of an invertible gate to bring out the key role of a three-terminal building block to enable the construction of correlated p-bit networks. The results for this implementation agree well with those from a universal model, showing that p-bits need not be magnet-based: any three-terminal tunable random bit generator should be suitable. We present an algorithm for designing a Boltzmann machine (BM) with symmetric connections that implements a given truth table. We then show how BM Full Adders can be interconnected in a partially directed manner to implement large operations such as 32-bit addition. Hundreds of p-bits get precisely correlated such that the correct answer out of 2^33 possibilities can be extracted by looking at the mode of a number of time samples. With perfect directivity a small number of samples is enough, while for less directed connections more samples are needed, but even in the former case invertibility is largely preserved. This combination of accuracy and invertibility is enabled by the hybrid design that uses bidirectional units to construct circuits with partially directed connections. We establish this result with examples including a 4-bit multiplier which in inverted mode functions as a factorizer.

We investigate long-range chiral magnetic interactions among adatoms mediated by surface states spin-splitted by spin-orbit coupling. Using the Rashba model, the tensor of exchange interactions is extracted wherein a pseudo-dipolar interaction is found besides the usual isotropic exchange interaction and the Dzyaloshinskii-Moriya interaction. We find that, despite the latter interaction, collinear magnetic states can still be stabilized by the pseudo-dipolar interaction. The inter-adatom distance controls the strength of these terms, which we exploit to design chiral magnetism in Fe nanostructures deposited on Au(111) surface. We demonstrate that these magnetic interactions are related to superpositions of the out-of-plane and in-plane components of the skyrmionic magnetic waves induced by the adatoms in the surrounding electron gas. We show that, even if the inter-atomic distance is large, the size and shape of the nanostructures dramatically impacts on the strength of the magnetic interactions, thereby affecting the magnetic ground state. We also derive an appealing connection between the isotropic exchange interaction and the Dzyaloshinskii-Moriya interaction, which relates the latter to the first order change of the former with respect to the spin-orbit coupling. This implies that the chirality defined by the direction of the Dzyaloshinskii-Moriya vector is driven by the variation of the isotropic exchange interaction due to the spin-orbit interaction.

We present a robust but still efficient simulation approach for high-resolution scanning tunneling microscopy with a flexible tip apex showing sharp submolecular features. The approach takes into account the electronic structure of sample and tip and relaxation of the tip apex. We validate our model by achieving good agreement with various experimental images which allows us to explain the origin of several observed features. Namely, we have found that high-resolution STM mechanism consists of the standard STM imaging, convolving electronic states of the sample and the tip apex orbital structure, with the contrast heavily distorted by the relaxation of the flexible apex caused by interaction with the substrate.

Superconductors containing magnetic impurities exhibit intriguing phenomena derived from the competition between Cooper pairing and Kondo screening. At the heart of this competition are the Yu-Shiba-Rusinov (Shiba) states which arise from the pair breaking effects a magnetic impurity has on a superconducting host. Hybrid superconductor-molecular junctions offer unique access to these states but the added complexity in fabricating such devices has kept their exploration to a minimum. Here, we report on the successful integration of a model spin 1/2 impurity, in the form of a neutral and stable all organic radical molecule, in proximity-induced superconducting break-junctions. Our measurements reveal excitations which are characteristic of a spin-induced Shiba state due to the radical's unpaired spin strongly coupled to a superconductor. By virtue of a variable molecule-electrode coupling, we access both the singlet and doublet ground states of the hybrid system which give rise to the doublet and singlet Shiba excited states, respectively. Our results show that Shiba states are a robust feature of the interaction between a paramagnetic impurity and a proximity-induced superconductor where the excited state is mediated by correlated electron-hole (Andreev) pairs instead of Cooper pairs.

Sub-molecular modulation of a 4<i>f</i> driven Kondo resonance by surface-induced asymmetry

Nature Communications, Published online: 26 September 2016; doi:10.1038/ncomms12785

In the Kondo effect, a bath of conduction electrons screens a localized magnetic moment. Here, the authors demonstrate Kondo screening of a normally isolated 4f-like moment in a magnetic molecule on a Cu(001) surface that is modulated by strong ligand-mediated coupling.

SrTiO 3 plays a central role in oxide electronics. It is the substrate of choice for functional oxide heterostructures based on perovskite-structure thin-film stacks, and its surface or interface with a polar oxide such as LaAlO 3 can become a 2D conductor because of electronic reconstruction or the presence of oxygen defects. Inconsistent reports of magnetic order in SrTiO 3 abound in the literature. Here, we report a systematic experimental study aimed at establishing how and when SrTiO 3 can develop a magnetic moment at room temperature. Polished (1 0 0), (1 1 0) or (1 1 1) crystal slices from four different suppliers are characterized before and after vacuum annealing at 750 °C, both in single-crystal and powdered form. Impurity content is analysed at the surface and in the bulk. Besides the underlying intrinsic diamagnetism of SrTiO 3 , magnetic signals are of three types—a Curie law susceptibility due to dilute magnetic impu...

The Ba\~{n}ados-Teitelboim-Zanelli (BTZ) black hole model corresponds to a solution of (2+1)-dimensional Einstein gravity with negative cosmological constant, and by a conformal rescaling its metric can be mapped onto the hyperbolic pseudosphere surface (Beltrami trumpet) with negative curvature. Beltrami trumpet shaped graphene sheets have been predicted to emit Hawking radiation that is experimentally detectable by a scanning tunnelling microscope. Here, for the first time we present an analytical algorithm that allows variational solutions to the Dirac Hamiltonian of graphene pseudoparticles in BTZ black hole gravitational field by using an approach based on the formalism of pseudo-Hermitian Hamiltonians within a discrete-basis-set method. We show that our model not only reproduces the exact results for the real part of quasinormal mode frequencies of (2+1)-dimensional spinless BTZ black hole, but also provides analytical results for the real part of quasinormal modes of spinning BTZ black hole, and also offers some predictions for the observable effects with a view to gravity-like phenomena in a curved graphene sheet.

Electronic wave functions of planar molecules can be reconstructed via inverse Fourier transform of angle-resolved photoelectron spectroscopy (ARPES) data, provided the phase of the electron wave in the detector plane is known. Since the recorded intensity is proportional to the absolute square of the Fourier transform of the initial state wave function, information about the phase distribution is lost in the measurement. It was shown that the phase can be retrieved in some cases by iterative algorithms using a priori information about the object such as its size and symmetry. We suggest a more generalized and robust approach for the reconstruction of molecular orbitals based on state-of-the-art phase-retrieval algorithms currently used in coherent diffraction imaging (CDI). We draw an analogy between the phase problem in molecular orbital imaging by ARPES and of that in optical CDI by performing an optical analogue experiment on micrometer-sized structures. We successful...

Nature Chemistry 8, 935 (2016). doi:10.1038/nchem.2552

Authors: Janina N. Ladenthin, Thomas Frederiksen, Mats Persson, John C. Sharp, Sylwester Gawinkowski, Jacek Waluk & Takashi Kumagai

Force-induced tautomerization in a single porphycene molecule is investigated on a Cu(110) surface at 5 K by using non-contact atomic force microscopy. The force needed to trigger the tautomerization process is quantified by force spectroscopy and theoretical calculations reveal the atomistic mechanism behind the reaction.

Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic

Nature 537, 7621 (2016). doi:10.1038/nature19343

Authors: Julia A. Mundy, Charles M. Brooks, Megan E. Holtz, Jarrett A. Moyer, Hena Das, Alejandro F. Rébola, John T. Heron, James D. Clarkson, Steven M. Disseler, Zhiqi Liu, Alan Farhan, Rainer Held, Robert Hovden, Elliot Padgett, Qingyun Mao, Hanjong Paik, Rajiv Misra, Lena F. Kourkoutis, Elke Arenholz, Andreas Scholl, Julie A. Borchers, William D. Ratcliff, Ramamoorthy Ramesh, Craig J. Fennie, Peter Schiffer, David A. Muller & Darrell G. Schlom

Materials that exhibit simultaneous order in their electric and magnetic ground states hold promise for use in next-generation memory devices in which electric fields control magnetism. Such materials are exceedingly rare, however, owing to competing requirements for displacive ferroelectricity and magnetism. Despite the recent identification of several new multiferroic materials and magnetoelectric coupling mechanisms, known single-phase multiferroics remain limited by antiferromagnetic or weak ferromagnetic alignments, by a lack of coupling between the order parameters, or by having properties that emerge only well below room temperature, precluding device applications. Here we present a methodology for constructing single-phase multiferroic materials in which ferroelectricity and strong magnetic ordering are coupled near room temperature. Starting with hexagonal LuFeO3—the geometric ferroelectric with the greatest known planar rumpling—we introduce individual monolayers of FeO during growth to construct formula-unit-thick syntactic layers of ferrimagnetic LuFe2O4 (refs 17, 18) within the LuFeO3 matrix, that is, (LuFeO3)m/(LuFe2O4)1 superlattices. The severe rumpling imposed by the neighbouring LuFeO3 drives the ferrimagnetic LuFe2O4 into a simultaneously ferroelectric state, while also reducing the LuFe2O4 spin frustration. This increases the magnetic transition temperature substantially—from 240 kelvin for LuFe2O4 (ref. 18) to 281 kelvin for (LuFeO3)9/(LuFe2O4)1. Moreover, the ferroelectric order couples to the ferrimagnetism, enabling direct electric-field control of magnetism at 200 kelvin. Our results demonstrate a design methodology for creating higher-temperature magnetoelectric multiferroics by exploiting a combination of geometric frustration, lattice distortions and epitaxial engineering.