arXiv subjects

Franz J. Giessibl

Publications and source records attributed to Franz J. Giessibl.

At least 19 recordsLinked to original sources

arXiv2026

Local probing of superconductivity at oxide interfaces with atomic force microscopy

Superconductivity in strontium titanate has remained enigmatic for more than 50 years. The LaAlO$_3$/SrTiO$_3$ (LAO/STO) heterointerface enables systematic dimensional confinement, from a two-dimensional electron gas to quasi-one-dimensional nanostructures, providing access to this quantum state. Transport measurements in patterned devices reveal puzzling phenomena, including width-independent critical currents and anomalous pairing suggestive of one-dimensional behavior, but direct local probes of the patterned interface and its superconducting response have been lacking. Here we use ultralow-temperature non-contact atomic force microscopy, dissipation spectroscopy, and Kelvin probe force microscopy to locally probe signatures of superconductivity in patterned LAO/STO devices. Spatially resolved energy-dissipation measurements reveal superconducting signatures, with features confined in some devices to edge channels approximately 200 nm wide. Dissipation spectra exhibit a characteristic nonlinear bias dependence that provides a local diagnostic of superconductivity, consistent with the intermediate carrier-density regime near the superconducting dome, and persisting up to the critical field. These results establish atomic force microscopy as a local probe of superconductivity in patterned LAO/STO structures and provide a route to addressing longstanding questions about quantum confinement and transport anomalies in correlated oxide nanostructures.

cond-mat.supr-con↗

arXiv2025

Measurement and Qualitative Explanation of Decay Lengths of Attractive and Repulsive Forces between Natural and Artificial Atoms

Artificial atoms, such as quantum corrals, offer an excellent platform to study fundamental interactions between localized quantum states and nanoscale probes. We performed atomic force microscopy measurements inside square quantum corrals on Cu(111) using CO- and metal-terminated tips. Using chemically unreactive CO-terminated tips repulsive Pauli forces can be probed, while metallic tips are attracted to the localized quantum states due to chemical bonding. We found distinct exponential decay constants of 46 pm for the repulsive and 66 pm for the attractive forces. Attractive and repulsive interactions between two natural atoms show significantly shorter decay lengths. While natural atoms feature states with a broad range of decay lengths, including very short ones from deeply bound states, quantum corrals are lacking such deeply bound and highly localized states, resulting in longer decay lengths. These results offer a new route to understand and design atomic-scale interactions in low-dimensional quantum structures and devices.

cond-mat.mes-hall↗

arXiv2025

Attosecond charge transfer in atomic-resolution scanning tunnelling microscopy

Electrons in atoms and molecules move on attosecond time scales. Deciphering their quantum dynamics in space and time calls for high-resolution microscopy at this speed. While scanning tunnelling microscopy (STM) driven with terahertz pulses has visualized sub-picosecond motion of single atoms, the advent of attosecond light pulses has provided access to the much faster electron dynamics. Yet, combining direct atomic spatial and attosecond temporal resolution remained challenging. Here, we reveal atomic-scale quantum motion of single electrons in attosecond lightwave-driven STM. Near-infrared single-cycle waveforms from phase-controlled optical pulse synthesis steer and clock electron tunnelling. By keeping the thermal load of the tip-sample junction stable, thereby eliminating thermal artifacts, we detect waveform-dependent currents on sub-cycle time scales. Our joint theory-experiment campaign shows that single-cycle near-infrared pulses can drive isolated electronic wave packets shorter than 1 fs. The angstrom-scale decay of the tunnelling current earmarks a fascinating interplay of multi-photon and field-driven dynamics. By balancing these effects, we sharply image a single copper adatom on a silver surface with lightwave-driven currents. This long-awaited fusion of attosecond science with atomic-scale STM makes elementary dynamics of electrons inside atoms, molecules and solids accessible to direct spatio-temporal videography and atom-scale petahertz electronics.

physics.optics↗

arXiv2024

Probing the Electronic Structure at the Boundary of Topological Insulators in the $\mathrm{Bi}_2\mathrm{Se}_3$ Family by Combined STM and AFM

We develop a numerical scheme for the calculation of tunneling current $I$ and differential conductance $\mathsf{d}I/\mathsf{d}V$ of metal and CO-terminated STM tips on the topological insulators $\mathrm{Bi}_2\mathrm{Se}_3$, $\mathrm{Bi}_2\mathrm{Te}_2\mathrm{Se}$ and $\mathrm{Bi}_2\mathrm{Te}_3$ and find excellent agreement with experiment. The calculation is an application of Chen's derivative rule, whereby the Bloch functions are obtained from Wannier interpolated tight-binding Hamiltonians and maximally localized Wannier functions from first-principle DFT+$GW$ calculations. We observe signatures of the topological boundary modes, their hybridization with bulk bands, Van Hove singularities of the bulk bands and characterize the orbital character of these electronic modes using the high spatial resolution of STM and AFM. Bare DFT calculations are insufficient to explain the experimental data, which are instead accurately reproduced by many-body corrected $GW$ calculations.

cond-mat.mes-hall↗

arXiv2024

Unexpected Gaussian line shapes reveal electron-adsorbate interaction as dominant broadening mechanism in quantum corrals

Understanding the factors influencing the lifetime of electronic states in artificial quantum structures is of great significance for advancing quantum technologies. This study focuses on CO-based quantum corrals on Cu(111). Tunneling spectroscopy measurements reveal a strong correlation between the size of the quantum corral and spectral width, characterized by a predominant Gaussian line shape. We attribute this dominant Gaussian-shaped lifetime broadening to the interaction of surface state electrons with the corral boundary. To further investigate this phenomenon, we constructed corrals of varying wall densities. Our findings indicate that elastic processes, such as tunneling, are more sensitive to wall density than coupling to the bulk.

cond-mat.mes-hall↗

arXiv2023

A Next-Generation qPlus-Sensor-Based AFM Setup: Resolving Archaeal S-layer Protein Structures in Air and Liquid

Surface-layer (S-layer) proteins form the outermost envelope in many bacteria and most archaea and arrange in 2D quasi-crystalline structures via self-assembly. We investigated S-layer proteins extracted from the archaeon Pyrobaculum aerophilium with a qPlus sensor-based atomic force microscope (AFM) in both liquid and ambient conditions and compared it to transmission electron microscopy (TEM) images under vacuum conditions. For AFM scanning, a next-generation liquid cell and a new protocol for creating long and sharp sapphire tips was introduced. Initial AFM images showed only layers of residual detergent molecules (SDS), which are used to isolate the S-layer proteins from the cells. SDS was not visible in the TEM images, requiring a more thorough sample preparation for AFM measurements. These improvements allowed us to resolve the crystal-like structure of the S-layer samples with frequency-modulation AFM in both air and liquid.

cond-mat.mtrl-sci↗

arXiv2023

On the origin and elimination of cross coupling between tunneling current and excitation in scanning probe experiments that utilize the qPlus sensor

The qPlus sensor allows simultaneous measurements of scanning tunneling microscopy (STM) and atomic force microscopy (AFM). Its design for use in frequency modulation AFM (FM-AFM) involves separate electrodes, applied on an oscillating quartz cantilever, for the detection of an electronic tunneling current and the deflection signal. Cable resistance and capacities in the electronic setup can induce cross talk phenomena. We report a tunneling current-induced cross coupling observed in a combined STM/AFM setup which uses the qPlus sensor. This cross coupling can induce a positive or negative change of the amplitude excitation signal, thus acting as an apparent dissipation or drive. The experimental data is explained well by tunneling current-induced fluctuations of the electric potential on the sensor electrodes.

cond-mat.mes-hall↗

arXiv2022

Evidence for temporary and local transition of sp2 graphite-type to sp3 diamond-type bonding induced by the tip of an atomic force microscope

Artificial diamond is created by exposing graphite to pressures on the order of 10\,GPa and temperatures of about 2000\,K. Here, we provide evidence that the pressure exerted by the tip of an atomic force microscope onto graphene over the carbon buffer layer of silicon carbide can lead to a temporary transition of graphite to diamond on the atomic scale. We perform atomic force microscopy with CO terminated tips and copper oxide (CuOx) tips to image graphene and to induce the structural transition. For a local transition, DFT predicts that a repulsive barrier of $\approx13$\,nN, followed by a force reduction by $\approx4$\,nN is overcome when inducing the graphite-diamond transition. Experimental evidence for this transition is provided by the observation of third harmonics in the cantilever oscillation for relative flexible CO terminated tips and a kink in the force versus distance curve for rigid CuOx tips. The experimental observation of the third harmonic with a magnitude of about 200\,fm fits to a force with an amplitude of $\pm 3$\,nN. The large repulsive overall force of $\approx 10$\,nN is only compatible with the experiment if one assumes that the repulsive force acting on the tip when inducing the transition is compensated by an increased van-der-Waals attraction of the tip due to form fitting of tip and sample by local indentation. The transition changes flat sp$^2$ bonds to corrugated sp$^3$ bonds, resulting in a different height of the two basis atoms in the elementary cell of graphene. Both tip types show a strong asysmmetry between the two basis atoms of the lattice when using large repulsive tip forces that induce the transition. Experimental data of tunneling current, frequency shift and dissipation are consistent with the proposed transition. The experiment also shows that atomic force microscopy allows to perform high pressure physics on the atomic scale.

cond-mat.mtrl-sci↗

arXiv2022

Designer magnetic topological graphene nanoribbons

The interplay of magnetism and topology lies at the heart of condensed matter physics, which offers great opportunities to design intrinsic magnetic topological materials hosting a variety of exotic topological quantum states including the quantum anomalous Hall effect (QAHE), axion insulator state, and Majorana bound states. Extending this concept to one-dimension (1D) systems offers additional rich quantum spin physics with great promise for molecular-scale spintronics. Despite recent progress in the discovery of symmetry-protected topological quantum phases in 1D graphene nanoribbons (GNRs), the rational design and realization of magnetic topological GNRs (MT-GNRs) represents a grand challenge, as one must tackle multiple dimensions of complexity including time-reversal symmetry (TRS), spatial symmetry (width, edge, end geometry) and many-electron correlations. Here, we devised a new route involving the real- and reciprocal-space descriptions by unifying the chemists and physicists perspectives, for the design of such MT-GNRs with non-trivial electronic topology and robust magnetic terminal. Classic Clar's rule offers a conceptually qualitative real-space picture to predict the transition from closed-shell to open-shell with terminal magnetism, and band gap reopening with possible non-trivial electronic topology in a series of wave-like GNRs, which are further verified by first principle calculations of band-structure topology in a momentum-space. With the advance of on-surface synthesis and careful design of molecular precursors, we have fabricated these MT-GNRs with observation of topological edge bands, whose terminal pi-magnetism can be directly captured using a single-nickelocene spin sensor. Moreover, the transition from strong anti-ferromagnetic to weak coupling (paramagnetism-like) between terminal spins can be controlled by tuning the length of MT-GNRs.

cond-mat.mes-hall↗

arXiv2021

Dynamic friction unraveled using an atomically defined model system

The pervasive phenomenon of friction has been studied at the nanoscale by controlled manipulation of single atoms and molecules, which permitted a precise determination of the static friction force necessary to initiate motion. However, much less is known about the atomistic dynamics during manipulation. Here we reveal the complete manipulation process of a carbon monoxide molecule on a copper surface at low temperatures using a combination of atomic force microscopy, vibrational spectroscopy for different isotope molecules and density functional theory. We measured the energy dissipation associated with manipulation and relate its origin to hysteresis involving an intermediate state, which enables an atomistic interpretation of dynamic friction. Our results show how friction forces can be controlled and optimized, facilitating new fundamental insights for tribology.

cond-mat.mes-hall↗

arXiv2020

Edge Channels of Broken-Symmetry Quantum Hall States in Graphene probed by Atomic Force Microscopy

The quantum Hall (QH) effect, a topologically non-trivial quantum phase, expanded and brought into focus the concept of topological order in physics. The topologically protected quantum Hall edge states are of crucial importance to the QH effect but have been measured with limited success. The QH edge states in graphene take on an even richer role as graphene is distinguished by its four-fold degenerate zero energy Landau level (zLL), where the symmetry is broken by electron interactions on top of lattice-scale potentials but has eluded spatial measurements. In this report, we map the quantum Hall broken-symmetry edge states comprising the graphene zLL at integer filling factors of $ν=0,\pm 1$ across the quantum Hall edge boundary using atomic force microscopy (AFM). Measurements of the chemical potential resolve the energies of the four-fold degenerate zLL as a function of magnetic field and show the interplay of the moiré superlattice potential of the graphene/boron nitride system and spin/valley symmetry-breaking effects in large magnetic fields.

cond-mat.mes-hall↗

arXiv2020

Experimental demonstration of pitfalls and remedies for precise force deconvolution in frequency-modulation atomic force microscopy

Frequency-modulation atomic force microscopy provides an outstanding precision of the measurement of chemical bonding forces. However, as the cantilever oscillates with an amplitude A that is usually on the order of atomic dimensions or even larger, blurring occurs. To extract a force versus distance curve from an experimental frequency versus distance spectrum, a deconvolution algorithm to recover the force from the experimental frequency shift is required. It has been recently shown that this deconvolution can be an ill-posed inversion problem causing false force-distance curves. Whether an inversion problem is well- or ill-posed is determined by two factors: the shape of the force-distance curve and the oscillation amplitude used for the measurement. A proper choice of the oscillation amplitude as proposed by the in ection point test of Sader et al. [Nat. Nanotechnol. 13, 1088 (2018)] should avoid ill-posedness. Here, we experimentally validate their in ection point test by means of two experimental data sets: force-distance spectra over a single carbon monoxide molecule as well as a Fe trimer on Cu(111) measured with a set of deliberately chosen amplitudes. Furthermore, we comment on typical pitfalls which are caused by the discrete nature of experimental data and provide MATLAB code which can be used by everyone to perform this test with their own data.

cond-mat.mtrl-sci↗

arXiv2019

Characterization of Hydrogen Plasma Defined Graphene Edges

We investigate the quality of hydrogen plasma defined graphene edges by Raman spectroscopy, atomic resolution AFM and low temperature electronic transport measurements. The exposure of graphite samples to a remote hydrogen plasma leads to the formation of hexagonal shaped etch pits, reflecting the anisotropy of the etch. Atomic resolution AFM reveals that the sides of these hexagons are oriented along the zigzag direction of the graphite crystal lattice and the absence of the D-peak in the Raman spectrum indicates that the edges are high quality zigzag edges. In a second step of the experiment, we investigate hexagon edges created in single layer graphene on hexagonal boron nitride and find a substantial D-peak intensity. Polarization dependent Raman measurements reveal that hydrogen plasma defined edges consist of a mixture of zigzag and armchair segments. Furthermore, electronic transport measurements were performed on hydrogen plasma defined graphene nanoribbons which indicate a high quality of the bulk but a relatively low edge quality, in agreement with the Raman data. These findings are supported by tight-binding transport simulations. Hence, further optimization of the hydrogen plasma etching technique is required to obtain pure crystalline graphene edges.

cond-mat.mes-hall↗

arXiv2018

Lateral manipulation with combined atomic force and scanning tunneling microscopy using CO-terminated tips

CO-terminated tips currently provide the best spatial resolution obtainable in atomic force microscopy. Due to their chemical inertness, they allow to probe interactions dominated by Pauli repulsion. The small size and inertness of the oxygen front atom yields unprecedented resolution of organic molecules, metal clusters and surfaces. We study the capability of CO-terminated tips to laterally manipulate single iron adatoms on the Cu(111) surface with combined atomic force and scanning tunneling microscopy at 7\,K. Furthermore, we find that even a slight asymmetry of the tip results in a distortion of the lateral force field. In addition, the influence of the tilt of the CO tip on the lateral force field is inverted compared to the use of a monoatomic metal tip which we can attribute to the inverted dipole moment of a CO tip with respect to a metal tip. Moreover, we demonstrate atom-by-atom assembly of iron clusters with CO tips while using the high-resolution capability of the CO tips in between to determine the arrangement of the individual iron atoms within the cluster. Additionally, we were able to laterally manipulate single copper and silicon adatoms without changing or losing the CO from the tip's apex.

cond-mat.mes-hall↗

arXiv2018

Analysis of STM images with pure and CO-functionalized tips: A first-principles and experimental study

We describe a first principles method to calculate scanning tunneling microscopy (STM) images, and compare the results to well-characterized experiments combining STM with atomic force microscopy (AFM). The theory is based on density functional theory (DFT) with a localized basis set, where the wave functions in the vacuum gap are computed by propagating the localized-basis wave functions into the gap using a real-space grid. Constant-height STM images are computed using Bardeen's approximation method, including averaging over the reciprocal space. We consider copper adatoms and single CO molecules adsorbed on Cu(111), scanned with a single-atom copper tip with and without CO functionalization. The calculated images agree with state-of-the-art experiments, where the atomic structure of the tip apex is determined by AFM. The comparison further allows for detailed interpretation of the STM images.

cond-mat.mes-hall↗

arXiv2017

Interatomic force laws that corrupt their own measurement

Atomically-resolved imaging and force measurements using the atomic force microscope (AFM) are performed most commonly in a frequency-modulation (FM) mode. This has led to spectacular results, including direct observation of the atomic structure of complex molecules and quantification of chemical and frictional forces at the atomic scale. We address here a critical question: Is recovery of force from the measured frequency shift experienced by the AFM cantilever ill-posed - that is, unreliable in the presence of (unavoidable) measurement uncertainty? Resolution of this issue underlies all force measurements using FM-AFM, but remains outstanding. It is shown that concavity of the force law's distance dependence controls ill-posed behavior, with a rapid concavity change corrupting force measurements by inducing spurious and unphysical effects - such rapid change is not uncommon. Practical conditions to eliminate ill-posed behavior are formulated which are verified experimentally. This study lays the foundations for robust atomically-resolved force spectroscopy and future work that will seek to regularize ill-posed force measurements.

cond-mat.mes-hall↗

arXiv2016

Attempts to test an alternative electrodynamic theory of superconductors by low-temperature scanning tunneling and atomic force microscopy

We perform an experiment to test between two theories of the electrodynamics of superconductors: the standard London theory and an alternative proposed by J. E. Hirsch [Phys. Rev. B 69, 214515 (2004)]. The two alternatives give different predictions with respect to the screening of an electric field by a superconductor, and we try to detect this effect using atomic force microscopy on a niobium sample. We also perform the reverse experiment, where we demonstrate a superconductive tip mounted on a qPlus force sensor. Due to limited accuracy, we are able neither to prove nor to disprove Hirsch's hypothesis. Within our accuracy of 0.17 N/m, the superconductive transition does not alter the atomic-scale interaction between tip and sample.

cond-mat.supr-con↗

arXiv2016

Amplitude dependence of image quality in atomically-resolved bimodal atomic microscopy

In bimodal FM-AFM, two flexural modes are excited simultaneously. The total vertical oscillation deflection range of the tip is the sum of the peak-to-peak amplitudes of both flexural modes (sum amplitude). We show atomically resolved images of KBr(100) in ambient conditions in bimodal AFM that display a strong correlation between image quality and sum amplitude. When the sum amplitude becomes larger than about 200 pm, the signal-to-noise ratio (SNR) is drastically decreased. We propose this is caused by the temporary presence of one or more water layers in the tip-sample gap. These water layers screen the short range interaction and must be displaced with each oscillation cycle. Further decreasing the sum amplitude, however, causes a decrease in SNR. Therefore, the highest SNR in ambient conditions is achieved when the sum amplitude is slightly less than the thickness of the primary hydration layer.

cond-mat.mes-hall↗