arXiv subjects

F. Stefan Tautz

Publications and source records attributed to F. Stefan Tautz.

At least 37 records · Page 2Linked to original sources

arXiv2024

Scattering makes a difference in circular dichroic angle-resolved photoemission

Recent years have witnessed a steady progress towards blending 2D quantum materials into technology, with future applications often rooted in the electronic structure. Since crossings and inversions of electronic bands with different orbital characters determine intrinsic quantum transport properties, knowledge of the orbital character is essential. Here, we benchmark angle-resolved photoelectron emission spectroscopy (ARPES) as a tool to experimentally derive orbital characters. For this purpose we study the valence electronic structure of two technologically relevant quantum materials, graphene and WSe$_2$, and focus on circular dichroism that is believed to provide sensitivity to the orbital angular momentum. We analyze the contributions related to angular atomic photoionization profiles, interatomic interference, and multiple scattering. Regimes in which initial-state properties could be disentangled from the ARPES maps are critically discussed and the potential of using circular-dichroic ARPES as a tool to investigate the spin polarization of initial bands is explored. For the purpose of generalization, results from two additional materials, GdMn$_6$Sn$_6$ and PtTe$_2$ are presented in addition. This research demonstrates rich complexity of the underlying physics of circular-dichroic ARPES, providing new insights that will shape the interpretation of both past and future circular-dichroic ARPES studies.

cond-mat.mtrl-sci↗

arXiv2023

The electrostatic potential of atomic nanostructures on a metal surface

The discrete and charge-separated nature of matter - electrons and nuclei - results in local electrostatic fields that are ubiquitous in nanoscale structures and are determined by their shape, material, and environment. Such fields are relevant in catalysis, nanoelectronics and quantum nanoscience, and their control will become even more important as the devices in question reach few-nanometres dimensions. Surface-averaging techniques provide only limited experimental access to these potentials at and around individual nanostructures. Here, we use scanning quantum dot microscopy to investigate how electric potentials evolve as nanostructures are built up atom by atom. We image the potential over adatoms, chains, and clusters of Ag and Au atoms on Ag(111) and quantify their surface dipole moments. By focusing on the total charge density, these data establish a new benchmark for ab initio calculations. Indeed, our density functional theory calculations not only show an impressive agreement with experiment, but also allow a deeper analysis of the mechanisms behind the dipole formation, their dependence on fundamental atomic properties and on the atomic configuration of the nanostructures. This allows us to formulate an intuitive picture of the basic mechanisms behind dipole formation, which enables better design choices for future nanoscale systems such as single atom catalysts.

cond-mat.mtrl-sci↗

arXiv2023

Induced Superconductivity in Hybrid Au/YBa2Cu3O7-x Electrodes on Vicinal Substrates

Superconducting electrodes are an integral part of hybrid Josephson junctions used in many applications including quantum technologies. We report on the fabrication and characterization of superconducting hybrid Au/YBa2Cu3O7-x (YBCO) electrodes on vicinal substrates. In these structures, superconducting CuO2-planes face the gold film, resulting in a higher value and smaller variation of the induced energy gap compared to the conventional Au/YBCO electrodes based on films with the c-axis normal to the substrate surface. Using scanning tunneling microscopy, we observe an energy gap of about 10-17 meV at the surface of the 15- nm-thick gold layer deposited in situ atop the YBCO film. To study the origin of this gap, we fabricate nanoconstrictions from the Au/YBCO heterostructure and measure their electrical transport characteristics. The conductance of the nanoconstrictions shows a series of dips due to multiple Andreev reflections in YBCO and gold providing clear evidence of the superconducting nature of the gap in gold. We consider the Au/YBCO electrodes to be a versatile platform for hybrid Josephson devices with a high operating temperature.

cond-mat.supr-con↗

arXiv2023

Suspended dry pick-up and flip-over assembly for van der Waals heterostructures with ultra-clean surfaces

Van der Waals heterostructures are an excellent platform for studying intriguing interface phenomena, such as moiré and proximity effects. Surface science techniques like scanning tunneling microscopy (STM) have proven a powerful tool to study such heterostructures but have so far been hampered because of their high sensitivity to surface contamination. Here, we report a dry polymer-based assembly technique to fabricate van der Waals heterostructures with atomically clean surfaces. The key features of our suspended dry pick-up and flip-over technique are 1) the heterostructure surface never comes into contact with polymers, 2) it is entirely solvent-free, 3) it is entirely performed in a glovebox, and 4) it only requires temperatures below 130$^{\circ}$. By performing ambient atomic force microscopy and atomically-resolved scanning tunneling microscopy on example heterostructures, we demonstrate that we can fabricate air-sensitive heterostructures with ultra-clean interfaces and surfaces. Due to the lack of polymer melting, the technique is further compatible with heterostructure assembly under ultra-high vacuum conditions, which promises ultimate heterostructure quality.

cond-mat.mes-hall↗

arXiv2023

One-dimensional topological superconductivity in a van der Waals heterostructure

One-dimensional (1D) topological superconductivity is a state of matter that is not found in nature. However, it can be realised, for example, by inducing superconductivity into the quantum spin Hall edge state of a two-dimensional topological insulator. Because topological superconductors are proposed to host Majorana zero modes, they have been suggested as a platform for topological quantum computing. Yet, conclusive proof of 1D topological superconductivity has remained elusive. Here, we employ low-temperature scanning tunnelling microscopy to show 1D topological superconductivity in a van der Waals heterostructure by directly probing its superconducting properties, instead of relying on the observation of Majorana zero modes at its boundary. We realise this by placing the two-dimensional topological insulator monolayer WTe$_2$ on the superconductor NbSe$_2$. We find that the superconducting topological edge state is robust against magnetic fields, a hallmark of its triplet pairing. Its topological protection is underpinned by a lateral self-proximity effect, which is resilient against disorder in the monolayer edge. By creating this exotic state in a van der Waals heterostructure, we provide an adaptable platform for the future realization of Majorana bound states. Finally, our results more generally demonstrate the power of Abrikosov vortices as effective experimental probes for superconductivity in nanostructures.

cond-mat.mes-hall↗

arXiv2023

Electron spin secluded inside a bottom-up assembled standing metal-molecule nanostructure

Artificial nanostructures, fabricated by placing building blocks such as atoms or molecules in well-defined positions, are a powerful platform in which quantum effects can be studied and exploited on the atomic scale. Here, we report a strategy to significantly reduce the electron-electron coupling between a large planar aromatic molecule and the underlying metallic substrate. To this end, we use the manipulation capabilities of a scanning tunneling microscope (STM) and lift the molecule into a metastable upright geometry on a pedestal of two metal atoms. Measurements at millikelvin temperatures and magnetic fields reveal that the bottom-up assembled standing metal-molecule nanostructure has an $S = \frac{1}{2}$ spin which is screened by the substrate electrons, resulting in a Kondo temperature of only $291 \pm 13$ mK. We extract the Landé $g$-factor of the molecule and the exchange coupling $Jρ$ to the substrate by modeling the differential conductance spectra using a third-order perturbation theory in the weak coupling and high-field regimes. Furthermore, we show that the interaction between the STM tip and the molecule can tune the exchange coupling to the substrate, which suggests that the bond between the standing metal-molecule nanostructure and the surface is mechanically soft.

cond-mat.mes-hall↗

arXiv2022

How cold is the junction of a millikelvin scanning tunnelling microscope?

We employ a scanning tunnelling microscope (STM) cooled to millikelvin temperatures by an adiabatic demagnetization refrigerator (ADR) to perform scanning tunnelling spectroscopy (STS) on an atomically clean surface of Al(100) in a superconducting state using normal-metal and superconducting STM tips. Varying the ADR temperatures between 30 mK and 1.2 K, we show that the temperature of the STM junction $T$ is decoupled from the temperature of the surrounding environment $T_{\mathrm{env}}$. Simulating the STS data with the $P(E)$ theory, we determine that $T_{\mathrm{env}} \approx 1.5$ K, while the fitting of the superconducting gap spectrum yields the lowest $T=77$ mK.

cond-mat.mes-hall↗

arXiv2022

Benchmarking theoretical electronic structure methods with photoemission orbital tomography

In the past decade, photoemission orbital tomography (POT) has evolved into a powerful tool to investigate the electronic structure of organic molecules adsorbed on (metallic) surfaces. By measuring the angular distribution of photoelectrons as a function of binding energy and making use of the momentum-space signature of molecular orbitals, POT leads to an orbital-resolved picture of the electronic density of states at the organic/metal interface. In this combined experimental and theoretical work, we apply POT to the prototypical organic $π$-conjugated molecule bisanthene (C$_{28}$H$_{14}$) which forms a highly oriented monolayer on a Cu(110) surface. Experimentally, we identify an unprecedented number of 13 $π$ and 12 $σ$ orbitals of bisanthene and measure their respective binding energies and spectral lineshapes at the bisanthene/Cu(110) interface. Theoretically, we perform density functional calculations for this interface employing four widely used exchange-correlation functionals from the families of the generalized gradient approximations as well as global and range-separated hybrid functionals. By analyzing the electronic structure in terms of orbital-projected density of states, we arrive at a detailed orbital-by-orbital assessment of theory vs. experiment. This allows us to benchmark the performance of the investigated functionals with regards to their capability of accounting for the orbital energy alignment at organic/metal interfaces.

cond-mat.mtrl-sci↗

arXiv2022

Vertical structure of Sb-intercalated quasifreestanding graphene on SiC(0001)

Using the normal incidence x-ray standing wave technique as well as low energy electron microscopy we have investigated the structure of quasi-freestanding monolayer graphene (QFMLG) obtained by intercalation of antimony under the $\left(6\sqrt{3}\times6\sqrt{3}\right)R30^\circ$ reconstructed graphitized 6H-SiC(0001) surface, also known as zeroth-layer graphene. We found that Sb intercalation decouples the QFMLG well from the substrate. The distance from the QFMLG to the Sb layer almost equals the expected van der Waals bonding distance of C and Sb. The Sb intercalation layer itself is mono-atomic, flat, and located much closer to the substrate, at almost the distance of a covalent Sb-Si bond length. All data is consistent with Sb located on top of the uppermost Si atoms of the SiC bulk.

cond-mat.mtrl-sci↗

arXiv2022

Portrait of locally driven quantum phase transition cascades in a molecular monolayer

Strongly interacting electrons in layered materials give rise to a plethora of emergent phenomena, such as unconventional superconductivity. heavy fermions, and spin textures with non-trivial topology. Similar effects can also be observed in bulk materials, but the advantage of two dimensional (2D) systems is the combination of local accessibility by microscopic techniques and tuneability. In stacks of 2D materials, for example, the twist angle can be employed to tune their properties. However, while material choice and twist angle are global parameters, the full complexity and potential of such correlated 2D electronic lattices will only reveal itself when tuning their parameters becomes possible on the level of individual lattice sites. Here, we discover a lattice of strongly correlated electrons in a perfectly ordered 2D supramolecular network by driving this system through a cascade of quantum phase transitions using a movable atomically sharp electrostatic gate. As the gate field is increased, the molecular building blocks change from a Kondo-screened to a paramagnetic phase one-by-one, enabling us to reconstruct their complex interactions in detail. We anticipate that the supramolecular nature of the system will in future allow to engineer quantum correlations in arbitrary patterned structures.

cond-mat.mes-hall↗

arXiv2022

Disentangling the Complex Electronic Structure of an Adsorbed Nanographene: Cycloarene C108

We combine low-temperature scanning tunneling spectroscopy, CO functionalized tips and algorithmic data analysis to investigate the electronic structure of the molecular cycloarene C108 (graphene nanoring) adsorbed on a Au(111) surface. We demonstrate that CO functionalized tips enhance the visibility of molecular resonances, both in differential conductance spectra and in real-space topographic images without introducing spurious artifacts. Comparing our experimental data with ab-initio density functional theory reveals a remarkably precise agreement of the molecular orbitals and enables us to disentangle close-lying molecular states only separated by 50 meV at an energy of 2 eV below the Fermi level. We propose this combination of techniques as a promising new route for a precise characterization of complex molecules and other physical entities which have electronic resonances in the tip-sample junction.

cond-mat.mes-hall↗

arXiv2022

Boron nitride on SiC(0001)

In the field of van der Waals heterostructures, the twist angle between stacked two-dimensional (2D) layers has been identified to be of utmost importance for the properties of the heterostructures. In this context, we previously reported the growth of a single layer of unconventionally oriented epitaxial graphene that forms in a surfactant atmosphere [F. C. Bocquet, et al., Phys. Rev. Lett. 125, 106102 (2020)]. The resulting G-R0$^\circ$ layer is aligned with the SiC lattice, and hence represents an important milestone towards high quality twisted bilayer graphene (tBLG), a frequently investigated model system in this field. Here, we focus on the surface structures obtained in the same surfactant atmosphere, but at lower preparation temperatures at which a boron nitride template layer forms on SiC(0001). In a comprehensive study based on complementary experimental and theoretical techniques, we find -- in contrast to the literature -- that this template layer is a hexagonal B$_x$N$_y$ layer, but not high-quality hBN. It is aligned with the SiC lattice and gradually replaced by low-quality graphene in the 0$^\circ$ orientation of the B$_x$N$_y$ template layer upon annealing.

cond-mat.mtrl-sci↗

arXiv2022

Probing edge state conductance in ultra-thin topological insulator films

Quantum spin Hall (QSH) insulators have unique electronic properties, comprising a band gap in their two-dimensional interior and one-dimensional spin-polarized edge states in which current flows ballistically. In scanning tunneling microscopy (STM), the edge states manifest themselves as a localized density of states. However, there is a significant research gap between the observation of edge states in nanoscale spectroscopy, and the detection of ballistic transport in edge channels which typically relies on transport experiments with microscale lithographic contacts. Here, we study few-layer films of the three-dimensional topological insulator (Bi$_{x}$Sb$_{1-x})_2$Te$_3$, for which a topological transition to a two-dimensional topological QSH insulator phase has been proposed. Indeed, an edge state in the local density of states is observed within the band gap. Yet, in nanoscale transport experiments with a four-tip STM, 2 and 3 quintuple layer films do not exhibit a ballistic conductance in the edge channels. This demonstrates that the detection of edge states in spectroscopy can be misleading with regard to the identification of a QSH phase. In contrast, nanoscale multi-tip transport experiments are a robust method for effectively pinpointing ballistic edge channels, as opposed to trivial edge states, in quantum materials.

cond-mat.mes-hall↗

arXiv2021

Momentum-space imaging of σ-orbitals for chemical analysis

Tracing the modifications of molecules in surface chemical reactions benefits from the possibility to image their orbitals. While delocalized frontier orbitals with π-character are imaged routinely with photoemission orbital tomography, they are not always sensitive to local chemical modifications, particularly the making and breaking of bonds at the molecular periphery. For such bonds, σ-orbitals would be far more revealing. Here, we show that these orbitals can indeed be imaged in a remarkably broad energy range, and that the plane wave approximation, an important ingredient of photoemission orbital tomography, is also well fulfilled for these orbitals. This makes photoemission orbital tomography a unique tool for the detailed analysis of surface chemical reactions. We demonstrate this by identifying the reaction product of a dehalogenation and cyclodehydrogenation reaction.

physics.chem-ph↗

arXiv2021

Resolving Ambiguity of the Kondo Temperature Determination in Mechanically Tunable Single-Molecule Kondo Systems

Determination of the molecular Kondo temperature $T_K$ poses a challenge in most cases when the experimental temperature cannot be tuned to a sufficient extent. We show how this ambiguity can be resolved if additional control parameters are present, such as magnetic field and mechanical gating. We record the evolution of the differential conductance by lifting an individual molecule from the metal surface with the tip of a scanning tunneling microscope. By fitting the measured conductance spectra with the single impurity Anderson model we are able to demonstrate that the lifting tunes the junction continuously from the strongly correlated Kondo-singlet to the free spin $1/2$ ground state. In the crossover regime, where $T_K$ is similar to the temperature of experiment, the fitting yields ambiguous estimates of $T_K$ varying by an order of magnitude. We show that analysis of the conductance measured in two distinct external magnetic fields can be used to resolve this problem.

cond-mat.mes-hall↗

arXiv2021

Lifting the spin-momentum locking in ultra-thin topological insulator films

Three-dimensional (3D) topological insulators (TIs) are known to carry 2D Dirac-like topological surface states in which spin-momentum locking prohibits backscattering. When thinned down to a few nanometers, the hybridization between the topological surface states at the top and bottom surfaces results in a topological quantum phase transition, which can lead to the emergence of a quantum spin Hall phase. Here, we study the thickness-dependent transport properties across the quantum phase transition on the example of (Bi$_{0.16}$Sb$_{0.84}$)$_2$Te$_3$ films, with a four-tip scanning tunnelling microscope. Our findings reveal an exponential drop of the conductivity below the critical thickness. The steepness of this drop indicates the presence of spin-conserving backscattering between the top and bottom surface states, effectively lifting the spin-momentum locking and resulting in the opening of a gap at the Dirac point. Our experiments provide crucial steps towards the detection of quantum spin Hall states in transport measurements.

cond-mat.mes-hall↗

arXiv2021

The Vertical Position of Sr Dopants in the Sr$_x$Bi$_2$Se$_3$ Superconductor

The discovery of topological superconductivity in doped Bi$_2$Se$_3$ made this class of materials highly important for the field of condensed matter physics. However, the structural origin of the superconducting state remained elusive, despite being investigated intensively in recent years. We use scanning tunneling microscopy and the normal incidence x-ray standing wave (NIXSW) technique in order to determine the vertical position of the dopants -- one of the key parameters for understanding topological superconductivity in this material -- for the case of Sr$_{x}$Bi$_2$Se$_3$. In a novel approach we analyze the NIXSW data in consideration of the inelastic mean free path of the photoemitted electrons, which allows us to distinguish between symmetry equivalent sites. We find that Sr-atoms are not situated inside the van der Waals gap between the Bi$_2$Se$_3$ quintuple layers but rather in the quintuple layer close to the outer Se planes.

cond-mat.supr-con↗

arXiv2021

A millikelvin scanning tunneling microscope in ultra-high vacuum with adiabatic demagnetization refrigeration

We present the design and performance of an ultra-high vacuum (UHV) scanning tunneling microscope (STM) that uses adiabatic demagnetization of electron magnetic moments for controlling its operating temperature in the range between 30 mK and 1 K with the accuracy of up to 7 $μ$K. The time available for STM experiments at 50 mK is longer than 20 h, at 100 mK about 40 h. The single-shot adiabatic demagnetization refrigerator (ADR) can be regenerated automatically within 7 hours while keeping the STM temperature below 5 K. The whole setup is located in a vibrationally isolated, electromagnetically shielded laboratory with no mechanical pumping lines penetrating through its isolation walls. The 1K pot of the ADR cryostat can be operated silently for more than 20 days in a single-shot mode using a custom-built high-capacity cryopump. A high degree of vibrational decoupling together with the use of a specially-designed minimalistic STM head provides an outstanding mechanical stability, demonstrated by the tunneling current noise, STM imaging, and scanning tunneling spectroscopy measurements all performed on atomically clean Al(100) surface.

physics.ins-det↗