arXiv subjects

Klaus Kern

Publications and source records attributed to Klaus Kern.

At least 19 recordsLinked to original sources

arXiv2026

Continuous Tuning of the Charge-Phase Uncertainty in a Josephson Junction

Quantum mechanics constrains conjugate observables from being simultaneously measurable with arbitrary precision. In a Josephson junction, these are the transferred electric charge and the quantum-mechanical phase difference between the superconducting domains. Which of them fluctuates determines the supercurrent: a dissipative trickle of single Cooper pairs in one limit, a coherent dissipationless flow in the other. Bridging both regimes in one device remained elusive because the Josephson and charging energies are fixed at fabrication. Here, we use the tunable tunnel junction of a scanning tunneling microscope at millikelvin temperature to vary their ratio continuously over many orders of magnitude. In this way, we monitor the smooth transition between incoherent and coherent Cooper pair flow in a single junction, revealing the quantum-to-classical transition in a controlled way.

cond-mat.supr-con↗

arXiv2026

DeepConf: Machine Learning Conformer Reconstruction of Biomolecules from Scanning Tunneling Microscopy Images

Improving the detailed understanding of the underlying properties and functions of biomolecules has recently attracted growing interest, enabled by the possibility of real-space imaging of single, intact macromolecules using Scanning Tunneling Microscopy (STM) in combination with electrospray ion beam deposition and soft landing. This combination provides key insights into biomolecular behavior, but it also imposes stringent requirements on rapid and reliable data analysis. A major limiting factor for applying machine learning to STM images is often the scarcity of training data, caused by the long acquisition times required for both experimental imaging and high-accuracy simulations. Here, we propose a framework for the rapid generation of three-dimensional structures of glycans, peptides, and glycopeptides and their corresponding STM-like image simulations, based on state-of-the-art, machine-learning-accelerated Density Functional Theory (DFT). We generate datasets for the polypeptide bradykinin and for a representative glycan molecule, and we train a conformer estimation model to predict a molecule's three-dimensional structure from an STM image. On synthetic data, our approach achieves high accuracy, with median atomic deviations below $2\,\AA{}$ for peptides and below $4\,\AA{}$ for glycans. Application to experimental data predominantly yields a precise, reliable, and visually convincing determination of the local positions of molecular subunits. The application to experimental data represents an important milestone towards a fully automated structural search pipeline for complex, biologically relevant systems imaged with STM.

cond-mat.mes-hall↗

arXiv2026

Enhancing the Energy Resolution in Scanning Tunneling Microscopy: from dynamical Coulomb blockade to cavity quantum electrodynamics

Scanning tunneling microscopy and spectroscopy have become indispensable tools for probing condensed matter at atomic length scales, yet achieving ultimate energy resolution remains a persistent challenge. At mK temperatures, the dynamical Coulomb blockade regime fundamentally limits spectroscopic precision through energy exchange between tunneling electrons and the electromagnetic environment. Here, we demonstrate that combining local electromagnetic shielding with low-pass filtering directly at the cryogenic scan head improves the energy resolution by nearly an order of magnitude, reaching benchmark values as low as 3.7$\mu$eV at 10mK. We attribute this enhancement to efficient suppression of high-frequency radiation and capacitive shunting of the tunnel junction. Remarkably, this improved sensitivity reveals that the Josephson current couples to electromagnetic cavity modes of the centimeter-scale scan head, establishing a direct connection between atomic-scale tunneling processes and macroscopic cavity quantum electrodynamics. These advances open pathways for exploring ultra-low-energy phenomena with unprecedented precision.

cond-mat.supr-con↗

arXiv2025

Nanoscale magnetometry of a synthetic three-dimensional spin texture

Multilayered synthetic antiferromagnets (SAFs) are artificial three-dimensional (3D) architectures engineered to create novel, complex, and stable spin textures. Non-invasive and quantitative nanoscale magnetic imaging of the two-dimensional stray field profile at the sample surface is essential for understanding the fundamental properties of the spin-structure and being able to tailor them to achieve new functionalities. However, the deterministic detection of spin textures and their quantitative characterization at the nanoscale remain challenging. Here, we use nitrogen-vacancy scanning probe microscopy (NV-SPM) under ambient conditions to perform the first quantitative vector-field magnetometry measurements in the multilayered SAF [(Co/Pt)$_5$/Co/Ru]$_3$/(Co/Pt)$_6$. We investigate nanoscale static and dynamic properties of antiferromagnetic domains with boundaries hosting ``one-dimensional'' ferromagnetic stripes with ~ 100 nm of width and periodic modulation of the magnetization. By employing NV-SPM measurements in different imaging modes and involving NV-probes with various crystallographic orientations, we demonstrated distinct fingerprints emerging from GHz-range spin noise and constant stray fields on the order of several mT. This provides quantitative insights into the structure of domains and domain walls, as well as, into magnetic noise associated with thermal spin-waves. Our work opens up new opportunities for quantitative vector-field magnetometry of modern magnetic materials with tailored 3D spin textures and stray field profiles, and potentially novel spin-wave dispersions--in a quantitative and non-invasive manner, with exceptional magnetic sensitivity and nanometer scale spatial resolution.

cond-mat.mes-hall↗

arXiv2025

Probing up-conversion electroluminescence of decoupled porphyrin molecules in a plasmonic nanocavity

Molecular triplet states can produce significant phosphorescence and act as a relay state for luminescence, such as in up-conversion processes. While this property makes triplet emitters interesting for organic light-emitting diodes (OLEDs), the study of their luminescence at the single molecule level in high resolution scanning tunneling microscopy (STM) is challenging. We investigate individual Pd-octaethylporphyrin (PdOEP) molecules decoupled from Ag(100) and Ag(111) by an ultrathin NaCl layer and observe singlet and triplet emission lines at visible wavelengths, only about 100 nm apart from each other. This is in stark contrast to the metal or free-base phthalocyanines, for which typically the lowest triplet transitions lie in the far red or infrared where the sensitivity of charge coupled device (CCD) detectors decrease significantly. The singlet S1 state of PdOEP emits photons even when the photon energy is higher than the energy provided by a tunneling electron, in an energy up-conversion process. This mechanism requires a relay (or shelving) state in which energy is stored in the molecule for the interval between tunneling electrons. Analyzing the energy levels of different molecular states (S1, D0, and T1 states) and fitting the current dependencies of S1 under up-conversion electroluminescence (UCEL) condition for S1 and T1 emission, we verify the validity of a triplet-mediated up-conversion model.

cond-mat.mes-hall↗

arXiv2025

Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules

Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the electronic inhomogeneity in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper napthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.

physics.optics↗

arXiv2025

Single-molecule phosphorescence and intersystem crossing in a coupled exciton-plasmon system

Scanning the sharp metal tip of a scanning tunneling microscope (STM) over a molecule allows tuning the coupling between the tip plasmon and a molecular fluorescence emitter. This allows access to local variations of fluorescence field enhancement and wavelength shifts, which are central parameters for characterizing the plasmon-exciton coupling. Performing the same for phosphorescence with molecular scale resolution remains a significant challenge. In this study, we present the investigation of phosphorescence from isolated Pt-Phthalocyanine molecules by analyzing tip-enhanced emission spectra in both current-induced and laser-induced phosphorescence. The latter directly monitors singlet-to-triplet state intersystem crossing of a molecule below the tip. The study contributes to a detailed understanding of triplet excitation pathways and their potential control at sub-molecular length scales. Additionally, the coupling of organic phosphors to plasmonic structures is a promising route for improving light-emitting diodes.

cond-mat.mes-hall↗

arXiv2024

Visualizing hot carrier dynamics by nonlinear optical microscopy at the atomic length scale

Probing and manipulating the spatiotemporal dynamics of hot carriers in nanoscale metals is crucial to a plethora of applications ranging from nonlinear nanophotonics to single molecule photochemistry. The direct investigation of these highly non-equilibrium carriers requires the experimental capability of high energy resolution (~ meV) broadband femtosecond spectroscopy. When considering the ultimate limits of atomic scale structures, this capability has remained out of reach until date. Using a two color femtosecond pump-probe spectroscopy, we present here the real-time tracking of hot carrier dynamics in a well-defined plasmonic picocavity, formed in the tunnel junction of a scanning tunneling microscope (STM). The excitation of hot carriers in the picocavity enables ultrafast all optical control over the broadband (~ eV) anti Stokes electronic resonance Raman scattering (ERRS) and the four-wave mixing (FWM) signals generated at the atomic length scale. By mapping the ERRS and FWM signals from a single graphene nanoribbon (GNR), we demonstrate that both signals are more efficiently generated along the edges of the GNR: a manifestation of atomic-scale nonlinear optical microscopy. This demonstration paves the way to the development of novel ultrafast nonlinear picophotonic platforms, affording unique opportunities in a variety of contexts, from the direct investigation of non equilibrium light matter interactions in complex quantum materials, to the development of robust strategies for hot carriers harvesting in single molecules and the next generation of active metasurfaces with deep-sub-wavelength meta-atoms.

physics.optics↗

arXiv2024

Nanoscale Mapping of Magnetic Auto-oscillations with a single Spin Sensor

Magnetic auto-oscillations are damping-compensated magnetization precessions. They can be generated in spin Hall nano-oscillators (SHNO) among others. Current research on these devices is dedicated to create next generation energy-efficient hardware for communication technologies. However, the underlying physics governing the formation of auto-oscillation modes, their output power and line width in a single SHNO device have remained elusive so far. We image the sources of magnetic auto-oscillations in a metallic SHNO using a single spin quantum sensor. We directly measure the microwave field generated by an auto-oscillation spot at the nanoscale by driving the electron spin resonance transition of the sensor spin, enabling faster acquisition speed (100 ms/pixel). Instead of being defined by the points of the largest antidamping only, we experimentally demonstrate for the first time with quantitative magnetometry that the auto-oscillation spots are determined by the positions of the magnetic field minima. The latter act as local potential wells for confining spin-waves, thus supporting large amplitude auto-oscillations. By comparing the magnitude of the magnetic stray field at these spots, we decipher the different frequencies of the auto-oscillation modes. The insights gained regarding the interaction between auto-oscillation modes and spin-wave potential wells enable advanced engineering of real devices.

cond-mat.mes-hall↗

arXiv2024

Selective Excitation of Vibrations in a Single Molecule

The capability to excite, probe, and manipulate vibrational modes is essential for understanding and controlling chemical reactions at the molecular level. Recent advancements in tip-enhanced Raman spectroscopies have enabled the probing of vibrational fingerprints in a single molecule with Angstrom-scale spatial resolution. However, achieving controllable excitation of specific vibrational modes in individual molecules remains challenging. Here, we demonstrate the selective excitation and probing of vibrational modes in single deprotonated phthalocyanine molecules utilizing resonance Raman spectroscopy in a scanning tunneling microscope. Selective excitation is achieved by finely tuning the excitation wavelength of the laser to be resonant with the vibronic transitions between the molecular ground electronic state and the vibrational levels in the excited electronic state, resulting in the state-selective enhancement of the resonance Raman signal. Our approach sets the stage for steering chemical transformations in molecules on surfaces by selective excitation of molecular vibrations.

physics.optics↗

arXiv2024

Scanning Tunneling Microscopy for Molecules: Effects of Electron Propagation into Vacuum

Using scanning tunneling microscopy (STM), we experimentally and theoretically investigate isolated platinum phthalocyanine (PtPc) molecules adsorbed on atomically thin NaCl(100) vapor deposited on Au(111). We obtain good agreement between theory and constant-height STM topography. We examine why strong distortions of STM images occur as a function of distance between molecule and STM tip. The images of the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) exhibit, for increasing distance, significant radial expansion due to electron propagation in the vacuum. Additionally, the imaged angular dependence is substantially distorted. The LUMO image has substantial intensity along the molecular diagonals where PtPc has no atoms. In the electronic transport gap the image differs drastically from HOMO and LUMO, even at energies very close to these orbitals. As the tunneling becomes increasingly off-resonant, the eight angular lobes of the HOMO or of the degenerate LUMOs diminish and reveal four lobes with maxima along the molecular axes, where both, HOMO and LUMO have little or no weight. These images are strongly influenced by low-lying PtPc orbitals that have simple angular structures.

cond-mat.mes-hall↗

arXiv2023

Character of electronic states in the transport gap of molecules on surfaces

We report on scanning tunneling microscopy (STM) topographs of individual metal phthalocyanines (MPc) on a thin salt (NaCl) film on a gold substrate, at tunneling energies within the molecule's electronic transport gap. Theoretical models of increasing complexity are discussed. The calculations for MPcs adsorbed on a thin NaCl layer on Au(111) demonstrate that the STM pattern rotates with the molecule's orientations - in excellent agreement with the experimental data. Thus, even the STM topography obtained for energies in the transport gap represent the structure of a one atom thick molecule. It is shown that the electronic states inside the transport gap can be rather accurately approximated by linear combinations of bound molecular orbitals (MOs). The gap states include not only the frontier orbitals but also surprisingly large contributions from energetically much lower MOs. These results will be essential for understanding processes, such as exciton creation, which can be induced by electrons tunneling through the transport gap of a molecule.

cond-mat.mes-hall↗

arXiv2023

Anionic Character of the Conduction Band of Sodium Chloride

The alkali halides are ionic compounds. Each alkali atom donates an electron to a halogen atom, leading to ions with full shells. The valence band is mainly located on halogen atoms, while, in a traditional picture, the conduction band is mainly located on alkali atoms. Scanning tunnelling microscopy of NaCl at 4 K actually shows that the conduction band is located on Cl$^-$ because the strong Madelung potential reverses the order of the Na$^+$ 3s and Cl$^-$ 4s levels. We verify this reversal is true for both atomically thin and bulk NaCl, and discuss implications for II-VI and I-VII compounds.

cond-mat.mtrl-sci↗

arXiv2023

Tracking a Spin-Polarized Superconducting Bound State across a Quantum Phase Transition

The magnetic exchange coupling between magnetic impurities and a superconductor induce so-called Yu-Shiba-Rusinov (YSR) states which undergo a quantum phase transition (QPT) upon increasing the exchange interaction beyond a critical value. While the evolution through the QPT is readily observable, in particular if the YSR state features an electron-hole asymmetry, the concomitant change in the ground state is more difficult to identify. We use ultralow temperature scanning tunneling microscopy to demonstrate how the change in the YSR ground state across the QPT can be directly observed for a spin-1/2 impurity in a magnetic field. We observe a change in the excitation spectrum from the doublet ground state in the free spin regime (two spectral features) to the singlet ground state in the screened spin regime (four spectral features). We also identify a transition regime, where the YSR excitation energy is smaller than the Zeeman energy. We thus provide a straightforward way for unambiguously identifying the ground state of a spin-1/2 YSR state.

cond-mat.supr-con↗

arXiv2023

Real-Time Tracking of Coherent Oscillations of Electrons in a Nanodevice by Photo-assisted Tunnelling

Coherent collective oscillations of electrons excited in metallic nanostructures (localized surface plasmons) can confine incident light to atomic scales and enable strong light-matter interactions, which depend nonlinearly on the local field. Direct sampling of such collective electron oscillations in real-time is crucial to performing petahertz scale optical modulation, control, and readout in a quantum nanodevice. Here, we demonstrate real-time tracking of collective electron oscillations in an Au bowtie nanoantenna, by recording photo-assisted tunnelling currents generated by such oscillations in this quantum nanodevice. The collective electron oscillations show a noninstantaneous response to the driving laser fields with a decay time of nearly 10 femtoseconds. The temporal evolution of nonlinear electron oscillations resulting from the coherent nonlinear optical response of the nanodevice were also traced in real-time. The contributions of linear and nonlinear electron oscillations in the generated tunnelling currents in the nanodevice were precisely determined. A coherent control of electron oscillations in the nanodevice is illustrated directly in the time domain. Functioning in ambient conditions, the excitation, coherent control, and read-out of coherent electron oscillations pave the way toward on-chip light-wave electronics in quantum nanodevices.

physics.optics↗

arXiv2022

Universal scaling of tunable Yu-Shiba-Rusinov states across the quantum phase transition

Quantum magnetic impurities give rise to a wealth of phenomena attracting tremendous research interest in recent years. On a normal metal, magnetic impurities generate the correlation-driven Kondo effect. On a superconductor, bound states emerge inside the superconducting gap called the Yu-Shiba-Rusinov (YSR) states. Theoretically, quantum impurity problems have been successfully tackled by numerical renormalization group (NRG) theory, where the Kondo and YSR physics are shown to be unified and the normalized YSR energy scales universally with the Kondo temperature divided by the superconducting gap. However, experimentally the Kondo temperature is usually extracted from phenomenological approaches, which gives rise to significant uncertainties and cannot account for magnetic fields properly. Using scanning tunneling microscopy at 10mK, we apply a magnetic field to several YSR impurities on a vanadium tip to reveal the Kondo effect and employ the microscopic single impurity Anderson model with NRG to fit the Kondo spectra in magnetic fields accurately and extract the corresponding Kondo temperature unambiguously. Some YSR states move across the quantum phase transition (QPT) due to the changes in atomic forces during tip approach, yielding a continuous universal scaling with quantitative precision for quantum spin-1/2 impurities.

cond-mat.supr-con↗

arXiv2022

Imaging and Controlling Coherent Phonon Wave Packets in Single Graphene Nanoribbons

The motion of atoms is at the heart of any chemical or structural transformation in molecules and materials. Upon activation of this motion by an external source, several (usually many) vibrational modes can be coherently coupled, thus facilitating the chemical or structural phase transformation. These coherent dynamics occur on the ultrafast time scale, as revealed, e.g., by nonlocal ultrafast vibrational spectroscopic measurements in bulk molecular ensembles and solids. Tracking and controlling vibrational coherences locally at the atomic and molecular scales is, however, much more challenging and in fact has remained elusive so far. Here, we demonstrate that the vibrational coherences induced by broadband laser pulses on a single graphene nanoribbon (GNR) can be probed by femtosecond coherent anti-Stokes Raman spectroscopy (CARS) when performed in a scanning tunnelling microscope (STM). In addition to determining dephasing (~ 440 fs) and population decay times (~1.8 ps) of the generated phonon wave packets, we are able to track and control the corresponding quantum coherences, which we show to evolve on time scales as short as ~ 70 fs. We demonstrate that a two-dimensional frequency correlation spectrum unequivocally reveals the quantum couplings between different phonon modes in the GNR.

physics.optics↗

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↗