Dr.jens.brede

The key to controlling reactions of molecules induced with the current of a scanning tunneling microscope (STM) tip is the ultrashort intermediate excited ionic state. The initial condition of the excited state is set by the energy and position of the injected current; thereafter, its dynamics determines the reaction outcome. We show that a STM can directly and controllably influence the excited-state dynamics. For the STM-induced desorption of toluene molecules from the Si(111)-7x7 surface, as the tip approaches the molecule, the probability of manipulation drops by two orders of magnitude. A two-channel quenching of the excited state is proposed, consisting of an invariant surface channel and a tip height–dependent channel. We conclude that picometer tip proximity regulates the lifetime of the excited state from 10 femtoseconds to less than 0.1 femtoseconds.

Electron spins in silicon quantum dots provide a promising route towards realising the large number of coupled qubits required for a useful quantum processor. At present, the requisite single-shot spin qubit measurements are performed using on-chip charge sensors, capacitively coupled to the quantum dots. However, as the number of qubits is increased, this approach becomes impractical due to the footprint and complexity of the charge sensors, combined with the required proximity to the quantum dots. Alternatively, the spin state can be measured directly by detecting the complex impedance of spin-dependent electron tunnelling between quantum dots. This can be achieved using radio-frequency reflectometry on a single gate electrode defining the quantum dot itself, significantly reducing gate count and architectural complexity, but thus far it has not been possible to achieve single-shot spin readout using this technique. Here, we detect single electron tunnelling in a double quantum dot and demonstrate that gate-based sensing can be used to read out the electron spin state in a single shot, with an average readout fidelity of 73%. The result demonstrates a key step towards the readout of many spin qubits in parallel, using a compact gate design that will be needed for a large-scale semiconductor quantum processor.

For solid-state spin qubits, single-gate RF readout can help minimise the number of gates required for scale-up to many qubits since the readout sensor can integrate into the existing gates required to manipulate the qubits (Veldhorst 2017, Pakkiam 2018). However, a key requirement for a scalable quantum computer is that we must be capable of resolving the qubit state within single-shot, that is, a single measurement (DiVincenzo 2000). Here we demonstrate single-gate, single-shot readout of a singlet-triplet spin state in silicon, with an average readout fidelity of $82.9\%$ at a $3.3~\text{kHz}$ measurement bandwidth. We use this technique to measure a triplet $T_-$ to singlet $S_0$ relaxation time of $0.62~\text{ms}$ in precision donor quantum dots in silicon. We also show that the use of RF readout does not impact the maximum readout time at zero detuning limited by the $S_0$ to $T_-$ decay, which remained at approximately $2~\text{ms}$. This establishes single-gate sensing as a viable readout method for spin qubits.

Imaging orbital-selective quasiparticles in the Hund’s metal state of FeSe

Imaging orbital-selective quasiparticles in the Hund’s metal state of FeSe, Published online: 03 September 2018; doi:10.1038/s41563-018-0151-0

Orbital-selective quasiparticle interference is imaged in the Hund’s metal parent state of iron-based superconductivity.

Topological band engineering of graphene nanoribbons

Topological band engineering of graphene nanoribbons, Published online: 08 August 2018; doi:10.1038/s41586-018-0376-8

A topologically engineered graphene nanoribbon superlattice is presented that hosts a one-dimensional array of half-filled, in-gap localized electronic states, enabling band engineering.

Engineering the spin couplings in atomically crafted spin chains on an elemental superconductor

Engineering the spin couplings in atomically crafted spin chains on an elemental superconductor, Published online: 14 August 2018; doi:10.1038/s41467-018-05701-8

Magnetic atomic chains assembled on the surface of superconductors are a potential platform for engineering topological superconducting phases. Here the authors step towards this by manipulating magnetic atoms at interstitial sites to tune interatomic interactions and control the Yu-Shiba-Rusinov states that form.

Engineering of robust topological quantum phases in graphene nanoribbons

Engineering of robust topological quantum phases in graphene nanoribbons, Published online: 08 August 2018; doi:10.1038/s41586-018-0375-9

Graphene nanoribbons are used to design robust nanomaterials with controlled periodic coupling of topological boundary states to create quasi-one-dimensional trivial and non-trivial electronic quantum phases.

Topological states engineered in narrow strips of graphene

Topological states engineered in narrow strips of graphene, Published online: 08 August 2018; doi:10.1038/d41586-018-05851-1

In materials known as graphene nanoribbons, topological states can be precisely engineered and probed, providing an experimental platform for studying electronic topology.

Single-ion magnetic anisotropy in molecular magnets leads to spin flip excitations that can be measured by inelastic scanning tunneling microscope (STM) spectroscopy. Here I present a semi ab initio scheme to compute the spectral features associated with inelastic spin flip excitations and Kondo effect of single molecular magnets. To this end density functional theory calculations of the molecule on the substrate are combined with more sophisticated many-body techniques for solving the Anderson impurity problem of the spin-carrying orbitals of the magnetic molecule coupled to the rest of the system, containing a phenomenological magnetic anisotropy term. For calculating the STM spectra an exact expression for the ##IMG## [http://ej.iop.org/images/0953-8984/30/35/354003/cmaad523ieqn001.gif] in the ideal STM limit, when the coupling to the STM tip becomes negligibly small, is derived. In this limit the ##IMG## [http://ej.iop.o...]

Author(s): S. Weiß, D. Gerbert, A. Stein, A. K. Schenk, X. Yang, C. Brülke, R. Kremring, S. Feldmann, F. C. Bocquet, M. Gille, S. Hecht, M. Sokolowski, P. Tegeder, S. Soubatch, and F. S. Tautz

Comparing the adsorption heights of various graphene nanoribbons on Cu(111) and Au(111) surfaces to those of graphene and π-conjugated planar organic molecules, we observe that two-dimensional graphene adsorbs much further away from the surface than both one-dimensional graphene nanoribbons and π-co...

[Phys. Rev. B 98, 075410] Published Fri Aug 10, 2018

Angewandte Chemie International Edition, Volume 57, Issue 32, August 6, 2018.

We measure singlet-triplet mixing in a precision fabricated double donor dot comprising of 2 and 1 phosphorus atoms separated by $16{\pm}1$ nm. We identify singlet and triplet-minus states by performing sequential independent spin readout of the two electron system and probe its dependence on magnetic field strength. The relaxation of singlet and triplet states are measured to be $12.4{\pm}1.0$ s and $22.1{\pm}1.0$ s respectively at $B_z{=}2.5$ T.

In this work we perform direct single-shot readout of the singlet-triplet states in exchange coupled electrons confined to precision placed donor atoms in silicon. Our method takes advantage of the large energy splitting given by the Pauli-spin blockaded (2,0) triplet states, from which we can achieve a single-shot readout fidelity of 98.4$\pm$0.2%. We measure the triplet-minus relaxation time to be of the order 3s at 2.5T and observe its predicted decrease as a function of magnetic field, reaching 0.5s at 1T.

Modern high-resolution microscopes, such as the scanning tunneling microscope, are commonly used to study specimens that have dense and aperiodic spatial structure. Extracting meaningful information from images obtained from such microscopes remains a formidable challenge. Fourier analysis is commonly used to analyze the underlying structure of fundamental motifs present in an image. However, the Fourier transform fundamentally suffers from severe phase noise when applied to aperiodic images. Here, we report the development of a new algorithm based on nonconvex optimization, applicable to any microscopy modality, that directly uncovers the fundamental motifs present in a real-space image. Apart from being quantitatively superior to traditional Fourier analysis, we show that this novel algorithm also uncovers phase sensitive information about the underlying motif structure. We demonstrate its usefulness by studying scanning tunneling microscopy images of a Co-doped iron arsenide superconductor and prove that the application of the algorithm allows for the complete recovery of quasiparticle interference in this material. Our phase sensitive quasiparticle interference imaging results indicate that the pairing symmetry in optimally doped NaFeAs is consistent with a sign-changing s+- order parameter.

The discretization of the electronic structure of nanometer-size solid systems due to quantum confinement and the concomitant modification of their physical properties is one of the cornerstones for the development of Nanoscience and Nanotechnology. In this letter we demonstrate that Bragg scattering of Cu(111) surface state electrons by the periodic arrangement of tetracyanoquinodimethane (TCNQ) molecules at the edges of self-assembled molecular islands, discretizes the possible values of the electron momentum parallel to the island edge. The electronic structure consists thus of a discrete number of sub-bands which occur in a non-closed space and, therefore, without quantum confinement.

One-dimensional Majorana modes are predicated to form in Josephson junctions based on three-dimensional topological insulators (TIs). While observations of supercurrents in Josephson junctions made on bulk-insulating TI samples are recently reported, the Fraunhofer patters observed in such TI-based Josephson junctions, which sometimes present anomalous features, are still not well understood. Here we report our study of highly gate-tunable TI-based Josephson junctions made of one of the most bulk-insulating TI materials, BiSbTeSe2, and Al. The Fermi level can be tuned by gating across the Dirac point, and the high transparency of the Al/BiSbTeSe2 interface is evinced by a high characteristic voltage and multiple Andreev reflections with peak indices reaching 12. Anomalous Fraunhofer patterns with missing lobes were observed in the entire range of gate voltage. We found that, by employing an advanced fitting procedure to use the maximum entropy method in a Monte Carlo algorithm, the anomalous Fraunhofer patterns are explained as a result of inhomogeneous supercurrent distributions on the TI surface in the junction. Besides establishing a highly promising fabrication technology, this work clarifies one of the important open issues regarding TI-based Josephson junctions.

The performance requirements for fault-tolerant quantum computing are very stringent. Qubits must be manipulated, coupled, and measured with error rates well below 1%. For semiconductor implementations, silicon quantum dot spin qubits have demonstrated average single-qubit Clifford gate error rates that approach this threshold, notably with error rates of 0.14% in isotopically enriched $^{28}$Si/SiGe devices. This gate performance, together with high-fidelity two-qubit gates and measurements, is only known to meet the threshold for fault-tolerant quantum computing in some architectures when assuming that the noise is incoherent, and still lower error rates are needed to reduce overhead. Here we experimentally show that pulse engineering techniques, widely used in magnetic resonance, improve average Clifford gate error rates for silicon quantum dot spin qubits to 0.043%,a factor of 3 improvement on previous best results for silicon quantum dot devices. By including tomographically complete measurements in randomised benchmarking, we infer a higher-order feature of the noise called the unitarity, which measures the coherence of noise. This in turn allows us to theoretically predict that average gate error rates as low as 0.026% may be achievable with further pulse improvements. These fidelities are ultimately limited by Markovian noise, which we attribute to charge noise emanating from the silicon device structure itself, or the environment.

We report on the magnetic properties of HoCo dimers as a model system for the smallest intermetallic transition metal-lanthanide compound. The dimers are adsorbed on ultrathin MgO(100) films grown on Ag(100). New for $4f$ elements, we detect inelastic excitations with scanning tunneling microscopy and prove by their behaviour in applied magnetic field that they are spin-excitations. In combination with density functional theory and spin Hamiltonian analysis we determine the magnetic level distribution, as well as sign and magnitude of the exchange interaction between the two atoms. In contrast to typical $4f-3d$ bulk compounds, we find ferromagnetic coupling in the dimer.

Author(s): Matthias Koch, Zhi Li, Christophe Nacci, Takashi Kumagai, Ignacio Franco, and Leonhard Grill

Molecular defects can improve the mechanical flexibility of graphene nanoribbons without affecting their electrical properties, new experiments show.

[Phys. Rev. Lett. 121, 047701] Published Tue Jul 24, 2018

Probing optical Stark effect at the single-molecule or atomic scale is crucial for understanding many photo-induced chemical and physical processes on surfaces. Here we report a study about optical Stark effect of single atomic defects on TiO2(110) surface with photo-assisted scanning tunneling spectroscopy. When a laser is coupled into the tunneling junction, the mid-gap state of OH-O2 defects changes remarkably in the differential conductance spectra. As laser power gradually increases, the energy of the mid-gap state shifts away from the Fermi level with increase in intensity and broadening of peak width. The observation can be explained as optical Stark effect with the Autler-Townes formula. This large optical Stark effect is due to the tip-enhancement and the strong dipole moment in the transient charged state during electron tunneling. Our study provides new aspects in exploring electron-photon interactions at the microscopic scale.

In the scanning tunnelling microscope, the many-body Kondo effect leads to a zero-bias feature of the differential conductance spectra of magnetic adsorbates on surfaces. The intrinsic line shape of this Kondo resonance and its temperature dependence in principle contain valuable information. We use measurements on a molecular Kondo system, all-trans retinoic acid on Au(111), and model calculations to discuss the role of instrumental broadening. The modulation voltage used for the lock-in detection, noise on the sample voltage, and the temperature of the microscope tip are considered. These sources of broadening affect the apparent line shapes and render difficult a determination of the intrinsic line width, in particular when variable temperatures are involved.

Magnetic resonance imaging (MRI) revolutionized diagnostic medicine and biomedical research by allowing a noninvasive access to spin ensembles. To enhance MRI resolution to the nanometer scale, new approaches including scanning probe methods have been used in recent years, which culminated in detection of individual spins. This allowed three-dimensional (3D) visualization of organic samples and of sophisticated spin-structures. Here, we demonstrate for the first time MRI of individual atoms on a surface. The setup, implemented in a cryogenic scanning tunneling microscope (STM), uses single-atom electron spin resonance (ESR) to achieve sub-{\AA}ngstr\"om resolution exceeding the spatial resolution of previous experiments by one to two orders of magnitude. We find that MRI scans of different atomic species and probe tips lead to unique signatures in the resonance images. These signatures reveal the magnetic interactions between the tip and the atom, in particular magnetic dipolar and exchange interaction.

We describe the development and performance of an ultra-high vacuum scanning tunneling microscope working under combined extreme conditions of ultra-low temperatures and high magnetic fields. We combined a top-loading dilution refrigerator and a standard bucket dewar with a bottom-loading superconducting magnet to achieve 4.5 days operating time, which is long enough to perform various spectroscopic-imaging measurements. To bring the effective electron temperature closer to the mixing-chamber temperature, we paid particular attention to filtering out the radio-frequency noise, as well as enhancing the thermal link between the microscope unit and the mixing chamber. We estimated the lowest effective electron temperature to be below 90 mK by measuring the superconducting-gap spectrum of aluminum. We confirmed the long-term stability of the spectroscopic-imaging measurement by visualizing superconducting vortices in the cuprate superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$.