arXiv subjects

Katharina J. Franke

Publications and source records attributed to Katharina J. Franke.

At least 19 recordsLinked to original sources

arXiv2026

Modified Low-Temperature Scanning Tunneling Microscope for Ultrafast Pump-Probe Spectroscopy

Combining scanning tunneling microscopy (STM) with terahertz pulses (THz-STM) enables ultrafast dynamics of phonons, spins, and charge carriers to be probed with atomic-scale spatial and sub-picosecond temporal resolution. However, coupling THz radiation into a low-temperature STM junction presents some technical challenges as it requires optical access for laser illumination while maintaining junction stability. Instead of designing a completely new STM head with customized optical access and optics within the ultra-high vacuum chamber, we modified a Besocke "Beetle" style STM with minimal changes of the cryogenic radiation shields. Despite the given geometrical conditions, we achieved efficient coupling of THz and optical pulses to the STM junction while maintaining temperatures below 6 K. We designed the optical setup on a separate laser table, starting with femtosecond laser pulses that are used to generate THz pulses in a LiNbO$_3$ crystal. We show the obtained THz pulse shapes and determine the effective time resolution using cross-correlation measurements. We further demonstrate the stable performance of the modified STM by measuring THz-induced tunneling currents from monolayer molybdenum disulfide (MoS$_2$) grown on Au(111). The resulting current maps resolve atomic-scale contrast revealing a point defect. The measurements confirm efficient THz coupling and stable low-temperature STM operation with atomic resolution.

cond-mat.mes-hall↗

arXiv2026

Probing crystal-field modulations with magnetic adatoms on the incipient charge-density-wave superconductor $2H$-NbS$_2$

The interplay between multiple quantum phases in layered materials may lead to incipient quantum behavior, where the material's ground state is close to a phase transition and sensitive to local disorder. The transition metal dichalcogenide material $2H$-NbS$_2$ exhibits incipient charge-density-wave behavior along with a well-developed superconducting state, creating a scenario where the local lattice instabilities play a crucial role. Here we present how an individual magnetic atom on $2H$-NbS$_2$ can be applied as a local sensor to reveal hidden crystal-field modulations. By manipulating the adatom across the surface with the tip of a scanning tunneling microscope, we measure variations in the Yu-Shiba-Rusinov (YSR) excitation spectra and map the local environment around an intrinsic point defect. We find that while the superconducting state is spatially uniform, the YSR excitation energy strongly depends on the position of the atom. We determine that the main contribution to this effect originates from variations in the local crystal-field environment. These results establish a new approach to investigate crystal-field modulations at the atomic scale and reveal how defects and lattice instabilities shape the atomic landscape of an incipient charge-density-wave material.

cond-mat.mes-hall↗

arXiv2025

Influence of atomic-scale defects on coherent phonon excitations by THz near fields in an STM

Coherent phonons describe the collective, ultrafast motion of atoms and play a central role in light-induced structural dynamics. Here, we employ terahertz scanning tunneling microscopy (THz-STM) to excite and detect coherent phonons in semiconducting 2H-$MoTe_{2}$ and resolve how their excitation is influenced by atomic-scale defects. In a THz pump-probe scheme, we observe long-lived oscillatory signals that we assign to out-of-plane breathing and in-plane shear modes, which are both forbidden in the bulk. Remarkably, the relative excitation strength of these modes varies near defects, indicating that local band bending modulates the coupling to the THz field. This defect-tunable coupling offers new opportunities to control material properties via selective excitation of vibrational modes at the nanoscale.

cond-mat.mes-hall↗

arXiv2025

From Shapiro steps to photon-assisted tunneling in microwave-driven atomic-scale Josephson junctions with a single (magnetic) adatom

Ultra-small Josephson junctions are strongly influenced by noise and damping due to energy dissipation into the environment, which are expected to suppress phase coherence. Here, we investigate the coherence properties of atomic-scale Josephson junctions in a scanning tunneling microscope under microwave excitation. Plain Pb-Pb junctions exhibit hysteretic Shapiro steps as signature of a coherent resonant state. With increasing AC amplitude, phase coherence is reduced due to an increase of thermal fluctuations. In the presence of magnetic adatoms the Josephson coupling energy is reduced and quasi-particle tunneling is enhanced. With AC driving we observe a rapid suppression of coherence that we ascribe to photon-assisted quasi-particle tunneling through Yu-Shiba-Rusinov states. Our results highlight the presence of phase coherence and shed light on the origin of the transition to incoherent transport, thereby revealing the importance of controlling dissipation in nanoscale superconducting devices.

cond-mat.mes-hall↗

arXiv2025

Direct signatures of $d$-level hybridization and dimerization in magnetic adatom chains on a superconductor

Magnetic adatom chains on superconductors provide a platform to explore correlated spin states and emergent quantum phases. Using low-temperature scanning tunneling spectroscopy, we study the distance-dependent interaction between Fe atoms on 2H-NbSe$_2$. While single atoms exhibit four Yu-Shiba-Rusinov states and partially occupied $d$ levels consistent with a $S=2$ spin state, the spin is quenched when two Fe atoms reside in nearest neighbor lattice sites, where the $d$ levels of the atoms hybridize. The non-magnetic dimer configuration is stable in that dimerization persists in chains with weak interactions among the dimers. Thus, the spin-state quenching has important implications also for Fe chains. While even-numbered chains are stable and non-magnetic, odd-numbered chains host a single magnetic atom at one of the chain's ends, with its position being switchable by voltage pulses. Our findings emphasize the role of interatomic coupling in shaping quantum ground states and suggest that engineering alternating hopping amplitudes analogous to the Su-Schrieffer-Heeger model may offer a pathway to realizing topological systems.

cond-mat.mes-hall↗

arXiv2025

Signatures of Kondo-lattice behavior in the two-dimensional ferromagnet Fe$_3$GeTe$_2$

Fe$_2$GeTe$_3$ is a paradigmatic van der Waals magnet with the full microscopic picture of magnetic interactions still under debate. Here, we use scanning tunneling microscopy and spectroscopy at 1.1 K to map out the low-energy physics on the surface. In agreement with previous works, we observe a spatially varying Fano lineshape that has been ascribed to a Kondo resonance. In addition, we identify a small gap of $\approx$ 5 meV width on top of the larger-energy Fano resonance. We suggest that this gap is the signature of a coherent Kondo lattice that has been proposed to originate from hybridization of a strongly dispersing and a flat band both derived from $d$ electrons of the Fe atoms in the lattice. Adding magnetic adatoms on the surface hardly influences the magnetic signatures of the substrate, indicating the robustness of the intralayer Kondo correlations against magnetic adsorbates.

cond-mat.mes-hall↗

arXiv2025

Odd-parity ground state in dilute Yu-Shiba-Rusinov dimers and chains

Magnetic adatoms on superconductors induce Yu-Shiba-Rusinov (YSR) states, which are key to the design of low-dimensional correlated systems and topological superconductivity. Competing magnetic interactions and superconducting pairing lead to a rich phase diagram. Using a scanning tunneling microscope (STM), we position Fe atoms on 2H-NbSe$_2$ to build a dimer with an odd-parity ground state, i.e., a partially screened YSR channel with the hybridized states spanning the Fermi level. This ground state makes the dimer a promising precursor for a topological YSR chain. By adding one atom at a time, we track the formation of YSR bands. The lowest-energy band crosses the Fermi level and we find strong site-dependent spectral variations especially at the chain's terminations. We attribute these features to quantum spin effects and ferromagnetic coupling influenced by the local chemical environment, rather than topological superconductivity or Majorana modes.

cond-mat.mes-hall↗

arXiv2024

Charge-density-wave control by adatom manipulation and its effect on magnetic nanostructures

Charge-density waves (CDWs) are correlated states of matter, where the electronic density is modulated periodically as a consequence of electronic and phononic interactions. Often, CDW phases coexist with other correlated states, such as superconductivity, spin-density waves or Mott insulators. Controlling CDW phases may therefore enable the manipulation of the energy landscape of these interacting states. 2H-NbSe$_2$ is a prime example of a transition metal dichalcogenide (TMDC) hosting CDW order and superconductivity. The CDW is of incommensurate nature resulting in different CDW-to-lattice alignments at the atomic scale. Here, we use the tip of a scanning tunneling microscope (STM) to position adatoms on the surface and induce reversible switching of the CDW domains. We show that the domain structure critically affects other local interactions, namely the hybridization of Yu-Shiba-Rusinov (YSR) states, which arise from exchange interactions of magnetic Fe atoms with the superconductor. Our results suggest that CDW manipulation could also be used to introduce domain walls in coupled spin chains on superconductors, potentially also affecting topological superconductivity.

cond-mat.mes-hall↗

arXiv2024

Quantifying the quantum nature of high spin YSR excitations in transverse magnetic field

Excitations of individual and coupled spins on superconductors provide a platform to study quantum spin impurity models as well as a pathway toward realizing topological quantum computing. Here, we characterize, using ultra-low temperature scanning tunneling microscopy/spectroscopy, the Yu-Shiba-Rusinov (YSR) states of individual manganese phthalocyanine molecules with high spin character on the surface of an ultra-thin lead film in variable transverse magnetic field. We observe two types of YSR excitations, depending on the adsorption geometry of the molecule. Using a zero-bandwidth model, we detail the role of the magnetic anisotropy, spin-spin exchange, and Kondo exchange. We illustrate that one molecular type can be treated as an individual spin akin to an isolated spin on the metal center, whereas the other molecular type invokes a coupled spin system represented by a spin on the center and the ligand. Using the field-dependent evolution of the YSR excitations and comparisons to modeling, we describe the quantum phase of each of the molecules. These results provide an insight into the quantum nature of YSR excitations in magnetic field, and a platform to study spin impurity models on superconductors in magnetic field.

cond-mat.supr-con↗

arXiv2024

Wave-function engineering on superconducting substrates: Chiral Yu-Shiba-Rusinov molecules

Magnetic adatoms on superconductors give rise to Yu-Shiba-Rusinov (YSR) states that hold considerable interest for the design of topological superconductivity. Here, we show that YSR states are also an ideal platform to engineer structures with intricate wave-function symmetries. We assemble structures of iron atoms on the quasi-two-dimensional superconductor $2H$-NbSe$_2$. The Yu-Shiba-Rusinov wave functions of individual atoms extend over several nanometers enabling hybridization even at large adatom spacing. We show that the substrate can be exploited to deliberately break symmetries of the adatom structure in ways unachievable in the gas phase. We highlight this potential by designing chiral wave functions of triangular adatom structures confined within a plane. Our results significantly expand the range of interesting quantum states that can be engineered using arrays of magnetic adatoms on superconductors.

cond-mat.mes-hall↗

arXiv2024

An atomic-scale perspective on individual thiol-terminated molecules anchored to single S vacancies in MoS$_2$

Sulphur vacancies in MoS$_2$ on Au(111) have been shown to be negatively charged as reflected by a Kondo resonance. Here, we use scanning tunneling microscopy to show that these vacancies serve as anchoring sites for thiol-based molecules (CF$_3$-3P-SH) with two distinct reaction products, one of them showing a Kondo resonance. Based on comparisons with density-functional theory (DFT) calculations, including a random structure search and computation of energies and electronic properties at a hybrid exchange-correlation functional level, we conclude that both anchored molecules are charge neutral. One of them is an anchored intact CF$_3$-3P-SH molecule while the other one is the result of catalytically activated dehydrogenation to CF$_3$-3P-S with subsequent anchoring. Our investigations highlight a perspective of functionalizing defects with thiol-terminated molecules that can be equipped with additional functional groups, such as charge donor- or acceptor-moieties, switching units or magnetic centers.

cond-mat.mtrl-sci↗

arXiv2023

Electronic and magnetic properties of single chalcogen vacancies in MoS$_2$/Au(111)

Two-dimensional (2D) transition-metal dichalcogenides (TMDC) are considered highly promising platforms for next-generation optoelectronic devices. Owing to its atomically thin structure, device performance is strongly impacted by a minute amount of defects. Although defects are usually considered to be disturbing, defect engineering has become an important strategy to control and design new properties of 2D materials. Here, we produce single S vacancies in a monolayer of MoS$_2$ on Au(111). Using a combination of scanning tunneling and atomic force microscopy, we show that these defects are negatively charged and give rise to a Kondo resonance, revealing the presence of an unpaired electron spin exchange coupled to the metal substrate. The strength of the exchange coupling depends on the density of states at the Fermi level, which is modulated by the moiré structure of the MoS$_2$ lattice and the Au(111) substrate. In the absence of direct hybridization of MoS$_2$ with the metal substrate, the S vacancy remains charge-neutral. Our results suggest that defect engineering may be used to induce and tune magnetic properties of otherwise non-magnetic materials.

cond-mat.mes-hall↗

arXiv2023

Yu-Shiba-Rusinov bands in a self-assembled kagome lattice of magnetic molecules

Kagome lattices constitute versatile platforms for studying paradigmatic correlated phases. While molecular self-assembly of kagome structures on metallic substrates is promising, it is challenging to realize pristine kagome properties because of hybridization with the bulk degrees of freedom and modified electron-electron interactions. We suggest that a superconducting substrate offers an ideal support for a magnetic kagome lattice. Exchange coupling induces kagome-derived bands at the interface, which are protected from the bulk by the superconducting energy gap. We realize a magnetic kagome lattice on a superconductor by depositing Fe-porphin-chloride molecules on Pb(111) and using temperature-activated de-chlorination and self-assembly. This allows us to control the formation of smaller kagome precursors and long-range ordered kagome islands. Using scanning tunneling microscopy and spectroscopy at 1.6 K, we identify Yu-Shiba-Rusinov states inside the superconducting energy gap and track their hybridization from the precursors to larger islands, where the kagome lattice induces extended YSR bands. These YSR-derived kagome bands are protected inside the superconducting energy gap, motivating further studies to resolve possible spin-liquid or Kondo-lattice-type behavior.

cond-mat.mes-hall↗

arXiv2023

Variations of vibronic states in densely-packed structures of molecules with intramolecular dipoles

Electrostatic potentials strongly affect molecular energy levels and charge states, providing the fascinating opportunity of molecular gating. Their influence on molecular vibrations remains less explored. Here, we investigate Ethyl-Diaminodicyanoquinone molecules on a monolayer of MoS$_2$ on Au(111) using scanning tunneling and atomic force microscopy and spectroscopy. These molecules exhibit a large dipole moment in gas phase, which we find to (partially) persist on the MoS$_2$ monolayer. The self-assembled structures consist of chains, where the dipoles of neighboring molecules are aligned anti-parallel. Thanks to the decoupling efficiency of the molecular states from the metal by the MoS$_2$ interlayer, we resolve vibronic states of the molecules, which vary in intensity depending on the molecular surrounding. We suggest that the vibrations are strongly damped by electrostatic interactions with the environment.

cond-mat.mes-hall↗

arXiv2023

Tuning a two-impurity Kondo system by a moiré superstructure

Two-impurity Kondo models are paradigmatic for correlated spin-fermion systems. Working with Mn atoms on Au(111) covered by a monolayer of MoS$_2$, we tune the inter-adatom exchange via the adatom distance and the adatom-substrate exchange via the location relative to a moiré structure of the substrate. Differential-conductance measurements on isolated adatoms exhibit Kondo peaks with heights depending on the adatom location relative to the moiré structure. Mn dimers spaced by a few atomic lattice sites exhibit split Kondo resonances. In contrast, adatoms in closely spaced dimers couple antiferromagnetically, resulting in a molecular-singlet ground state. Exciting the singlet-triplet transition by tunneling electrons, we find that the singlet-triplet splitting is surprisingly sensitive to the moiré structure. We interpret our results theoretically by relating the variations in the singlet-triplet splitting to the heights of the Kondo peaks of single adatoms, finding evidence for coupling of the adatom spin to multiple conduction electron channels.

cond-mat.mes-hall↗

arXiv2022

Diode effects in current-biased Josephson junctions

Current-biased Josephson junctions exhibit hysteretic transitions between dissipative and superconducting states as characterized by switching and retrapping currents. Here, we develop a theory for diode-like effects in the switching and retrapping currents of weakly-damped Josephson junctions. We find that while the diode-like behavior of switching currents is rooted in asymmetric current-phase relations, nonreciprocal retrapping currents originate in asymmetric quasiparticle currents. These different origins also imply distinctly different symmetry requirements. We illustrate our results by a microscopic model for junctions involving a single magnetic atom. Our theory provides significant guidance in identifying the microscopic origin of nonreciprocities in Josephson junctions.

cond-mat.supr-con↗

arXiv2022

Diode effect in Josephson junctions with a single magnetic atom

Current flow in electronic devices can be asymmetric with bias direction, a phenomenon underlying the utility of diodes and known as non-reciprocal charge transport. The promise of dissipationless electronics has recently stimulated the quest for superconducting diodes, and non-reciprocal superconducting devices have been realized in various non-centrosymmetric systems. Probing the ultimate limits of miniaturization, we have created atomic-scale Pb--Pb Josephson junctions in a scanning tunneling microscope. Pristine junctions stabilized by a single Pb atom exhibit hysteretic behavior, confirming the high quality of the junctions, but no asymmetry between the bias directions. Non-reciprocal supercurrents emerge when inserting a single magnetic atom into the junction, with the preferred direction depending on the atomic species. Aided by theoretical modelling, we trace the non-reciprocity to quasiparticle currents flowing via Yu-Shiba-Rusinov (YSR) states inside the superconducting energy gap. Our results open new avenues for creating atomic-scale Josephson diodes and tuning their properties through single-atom manipulation.

cond-mat.supr-con↗

arXiv2022

Quantum spins and hybridization in artificially-constructed chains of magnetic adatoms on a superconductor

Magnetic adatom chains on surfaces constitute fascinating quantum spin systems. Superconducting substrates suppress interactions with bulk electronic excitations but couple the adatom spins to a chain of subgap Yu-Shiba-Rusinov (YSR) quasiparticles. Using a scanning tunneling microscope, we investigate such correlated spin-fermion systems by constructing Fe chains adatom by adatom on superconducting NbSe$_2$. The adatoms couple entirely via the substrate, retaining their quantum spin nature. In dimers, we observe that the deepest YSR state undergoes a quantum phase transition due to Ruderman-Kittel-Kasuya-Yosida interactions, a distinct signature of quantum spins. Chains exhibit coherent hybridization and band formation of the YSR excitations, indicating ferromagnetic coupling. Longer chains develop separate domains due to coexisting charge-density-wave order of NbSe$_2$. Despite the spin-orbit-coupled substrate, we find no signatures of Majoranas, possibly because quantum spins reduce the parameter range for topological superconductivity. We suggest that adatom chains are versatile systems for investigating correlated-electron physics and its interplay with topological superconductivity.

cond-mat.mes-hall↗