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Christian R. Ast

Publications and source records attributed to Christian R. Ast.

At least 19 recordsLinked to original sources

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

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$μ$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

Josephson tunneling through a Yu-Shiba-Rusinov state: Interplay of $π$-shifts in Josephson current and local superconducting order parameter

An impurity hosting a magnetic moment coupled to a conventional $s$-wave superconductor gives rise to so-called Yu-Shiba-Rusinov (YSR) states with energies inside the superconducting gap. Depending on the coupling between the impurity and the superconductor, the system can have two distinct quantum ground states separated by a quantum phase transition (QPT). We investigate the interplay of two effects observed at the QPT. First, the tunneling supercurrent through the impurity reverses its sign at the QPT, denoted as a $π$-shift in the current-phase relation. Secondly, the local superconducting order parameter at the impurity site is suppressed and becomes negative at the QPT, generally termed a $π$-shift in the local superconducting order parameter. We find that both these effects are governed by the presence of the YSR state, however, they do not significantly depend or influence each other. In particular, we establish that the $π$-shift in the superconducting order parameter does not induce a $π$-shift in the tunneling Josephson current, nor can the Josephson current and its spatial behavior be used to directly probe the impurity-induced changes in the local superconducting order parameter, which occur on a length scale substantially shorter than the superconducting coherence length.

cond-mat.supr-con

Temperature dependent energy gap for Yu-Shiba-Rusinov states at the quantum phase transition

Motivated by recent experiments, which allow for fine tuning of the effective magnetic interaction between the impurity and the superconductor, we investigate the regime around the quantum phase transition where the system's ground state changes from a weakly coupled free spin to a screened spin regime. At this transition we find that the Yu-Shiba-Rusinov (YSR) states remain at finite energies at low temperatures, thereby generating a gap in the spectrum, which is inconsistent with predictions of the original YSR theory. We investigate various gap-generating scenarios and determine that the local suppression of the order parameter, only captured by self-consistent calculations, generates the gap.

cond-mat.supr-con

Theory of Electron Spin Resonance in Scanning Tunneling Microscopy

Electron spin resonance (ESR) spectroscopy in scanning tunneling microscopy (STM) has enabled probing the electronic structure of single magnetic atoms and molecules on surfaces with unprecedented energy resolution, as well as demonstrating coherent manipulation of single spins. Despite this remarkable success, the field could still be greatly advanced by a more quantitative understanding of the ESR-STM physical mechanisms. Here, we present a theory of ESR-STM which quantitatively models not only the ESR signal itself, but also the full background tunneling current, from which the ESR signal is derived. Our theory is based on a combination of Green's function techniques to describe the electron tunneling and a quantum master equation for the dynamics of the spin system along with microwave radiation interacting with both the tunneling current and the spin system. We show that this theory is able to quantitatively reproduce the experimental results for a spin-1/2 system (TiH molecules on MgO) across many orders of magnitude in tunneling current, providing access to the relaxation and decoherence rates that govern the spin dynamics due to intrinsic mechanisms and to the applied bias voltage. More importantly, our work establishes that: (i) sizable ESR signals, which are a measure of microwave-induced changes in the junction magnetoresistance, require surprisingly high tip spin polarizations, (ii) the coupling of the magnetization dynamics to the microwave field gives rise to the asymmetric ESR spectra often observed in this spectroscopy. Additionally, our theory provides very specific predictions for the dependence of the relaxation and decoherence times on the bias voltage and the tip-sample distance. Finally, with the help of electromagnetic simulations, we find that the transitions in our ESR-STM experiments can be driven by the ac magnetic field at the junction.

cond-mat.mes-hall

Roadmap on Nanoscale Magnetic Resonance Imaging

The field of nanoscale magnetic resonance imaging (NanoMRI) was started 30 years ago. It was motivated by the desire to image single molecules and molecular assemblies, such as proteins and virus particles, with near-atomic spatial resolution and on a length scale of 100 nm. Over the years, the NanoMRI field has also expanded to include the goal of useful high-resolution nuclear magnetic resonance (NMR) spectroscopy of molecules under ambient conditions, including samples up to the micron-scale. The realization of these goals requires the development of spin detection techniques that are many orders of magnitude more sensitive than conventional NMR and MRI, capable of detecting and controlling nanoscale ensembles of spins. Over the years, a number of different technical approaches to NanoMRI have emerged, each possessing a distinct set of capabilities for basic and applied areas of science. The goal of this roadmap article is to report the current state of the art in NanoMRI technologies, outline the areas where they are poised to have impact, identify the challenges that lie ahead, and propose methods to meet these challenges. This roadmap also shows how developments in NanoMRI techniques can lead to breakthroughs in emerging quantum science and technology applications.

cond-mat.mes-hall

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

Microwave Excitation of Atomic Scale Superconducting Bound States

Magnetic impurities on superconductors lead to bound states within the superconducting gap, so called Yu-Shiba-Rusinov (YSR) states. They are parity protected, which enhances their lifetime, but makes it more difficult to excite them. Here, we realize the excitation of YSR states by microwaves facilitated by the tunnel coupling to another superconducting electrode in a scanning tunneling microscope (STM). We identify the excitation process through a family of anomalous microwave-assisted tunneling peaks originating from a second-order resonant Andreev process, in which the microwave excites the YSR state triggering a tunneling event transferring a total of two charges. We vary the amplitude and the frequency of the microwave to identify the energy threshold and the evolution of this excitation process. Our work sets an experimental basis and proof-of-principle for the manipulation of YSR states using microwaves with an outlook towards YSR qubits.

cond-mat.supr-con

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

Electric Control of Spin Transitions at the Atomic Scale

Electric control of spins has been a longstanding goal in the field of solid state physics due to the potential for increased efficiency in information processing. This efficiency can be optimized by transferring spintronics to the atomic scale. We present electric control of spin resonance transitions in single molecules by employing electron spin resonance scanning tunneling microscopy (ESR-STM). We find strong bias voltage dependent shifts in the ESR signal of about ten times its linewidth, which is due to the electric field induced displacement of the spin system in the tunnel junction. This opens up new avenues for ultrafast control of coupled spin systems, even towards atomic scale quantum computing, and expands on understanding and optimizing spin electric coupling in bulk materials.

cond-mat.mes-hall

Combining Electron Spin Resonance Spectroscopy with Scanning Tunneling Microscopy at High Magnetic Fields

Magnetic media remain a key in information storage and processing. The continuous increase of storage densities and the desire for quantum memories and computers pushes the limits of magnetic characterisation techniques. Ultimately, a tool which is capable of coherently manipulating and detecting individual quantum spins is needed. The scanning tunnelling microscope (STM) is the only technique which unites the prerequisites of high spatial and energy resolution, low temperature and high magnetic fields to achieve this goal. Limitations in the available frequency range for electron spin resonance STM (ESR-STM) mean that many instruments operate in the thermal noise regime. We resolve challenges in signal delivery to extend the operational frequency range of ESR-STM by more than a factor of two and up to 100GHz, making the Zeeman energy the dominant energy scale at achievable cryogenic temperatures of a few hundred millikelvin. We present a general method for augmenting existing instruments into ESR-STMs to investigate spin dynamics in the high-field limit. We demonstrate the performance of the instrument by analysing inelastic tunnelling in a junction driven by a microwave signal and provide proof of principle measurements for ESR-STM.

cond-mat.mes-hall

Extracting the Transport Channel Transmissions in Scanning Tunneling Microscopy using the Superconducting Excess Current

Transport through quantum coherent conductors, like atomic junctions, is described by the distribution of conduction channels. Information about the number of channels and their transmission can be extracted from various sources, such as multiple Andreev reflections, dynamical Coulomb blockade, or shot noise. We complement this set of methods by introducing the superconducting excess current as a new tool to continuously extract the transport channel transmissions of an atomic scale junction in a scanning tunneling microscope. In conjunction with ab initio simulations, we employ this technique in atomic aluminum junctions to determine the influence of the structure adjacent to the contact atoms on the transport properties.

cond-mat.supr-con

Band Engineering of Dirac Semimetals using Charge Density Waves

New developments in the field of topological matter are often driven by materials discovery, including novel topological insulators, Dirac semimetals and Weyl semimetals. In the last few years, large efforts have been performed to classify all known inorganic materials with respect to their topology. Unfortunately, a large number of topological materials suffer from non-ideal band structures. For example, topological bands are frequently convoluted with trivial ones, and band structure features of interest can appear far below the Fermi level. This leaves just a handful of materials that are intensively studied. Finding strategies to design new topological materials is a solution. Here we introduce a new mechanism that is based on charge density waves and non-symmorphic symmetry to design an idealized Dirac semimetal. We then show experimentally that the antiferromagnetic compound GdSb$_{0.46}$Te$_{1.48}$ is a nearly ideal Dirac semimetal based on the proposed mechanism, meaning that most interfering bands at the Fermi level are suppressed. Its highly unusual transport behavior points to a thus far unknown regime, in which Dirac carriers with Fermi energy very close to the node seem to gradually localize in the presence of lattice and magnetic disorder.

cond-mat.mtrl-sci

Spin-dependent tunneling between individual superconducting bound states

Magnetic impurities on superconductors induce discrete bound levels inside the superconducting gap, known as Yu-Shiba-Rusinov (YSR) states. YSR levels are fully spin-polarized such that the tunneling between YSR states depends on their relative spin orientation. Here, we use scanning tunneling spectroscopy to resolve the spin dynamics in the tunneling process between two YSR states by experimentally extracting the angle between the spins. To this end, we exploit the ratio of thermally activated and direct spectral features in the measurement to directly extract the relative spin orientation between the two YSR states. We find freely rotating spins down to 7mK, indicating a purely paramagnetic nature of the impurities. Such a non-collinear spin alignment is essential not only for producing Majorana bound states but also as an outlook manipulating and moving the Majorana state onto the tip.

cond-mat.supr-con

Visualizing the multifractal wavefunctions of a disordered two-dimensional electron gas

The wavefunctions of a disordered two-dimensional electron gas at the quantum-critical Anderson transition are predicted to exhibit multifractal scaling in their real space amplitude. We experimentally investigate the appearance of these characteristics in the spatially resolved local density of states of a two-dimensional mixed surface alloy Bi_xPb_{1-x}/Ag(111), by combining high-resolution scanning tunneling microscopy with spin and angle-resolved inverse-photoemission experiments. Our detailed knowledge of the surface alloy electronic band structure, the exact lattice structure and the atomically resolved local density of states enables us to construct a realistic Anderson tight binding model of the mixed surface alloy, and to directly compare the measured local density of states characteristics with those from our model calculations. The statistical analyses of these two-dimensional local density of states maps reveal their log-normal distributions and multifractal scaling characteristics of the underlying wavefunctions with a finite anomalous scaling exponent. Finally, our experimental results confirm theoretical predictions of an exact scaling symmetry for Anderson quantum phase transitions in the Wigner-Dyson classes.

cond-mat.mes-hall

Interplay Between Yu-Shiba-Rusinov States and Multiple Andreev Reflections

Motivated by recent scanning tunneling microscopy experiments on single magnetic impurities on superconducting surfaces, we present here a comprehensive theoretical study of the interplay between Yu-Shiba-Rusinov bound states and (multiple) Andreev reflections. Our theory is based on a combination of an Anderson model with broken spin degeneracy and nonequilibrium Green's function techniques that allows us to describe the electronic transport through a magnetic impurity coupled to superconducting leads for arbitrary junction transparency. Using this combination we are able to elucidate the different tunneling processes that give a significant contribution to the subgap transport. In particular, we predict the occurrence of a large variety of Andreev reflections mediated by Yu-Shiba-Rusinov bound states that clearly differ from the standard Andreev processes in non-magnetic systems. Moreover, we provide concrete guidelines on how to experimentally identify the subgap features originating from these tunneling events. Overall, our work provides new insight into the role of the spin degree of freedom in Andreev transport physics.

cond-mat.supr-con

Microwave-assisted tunneling and interference effects in superconducting junctions under fast driving signals

As scanning tunneling microscopy is pushed towards fast local dynamics, a quantitative understanding of tunnel junctions under the influence of a fast AC driving signal is required, especially at the ultra-low temperatures relevant to spin dynamics and correlated electron states. We subject a superconductor-insulator-superconductor junction to a microwave signal from an antenna mounted \textit{in situ} and examine the DC response of the contact to this driving signal. Quasi-particle tunneling and the Josephson effect can be interpreted in the framework of Tien-Gordon theory. The situation is more complex when it comes to higher order effects such as multiple Andreev reflections. Microwave assisted tunneling unravel these complex processes, providing deeper insights into tunneling than are available in a pure DC measurement.

cond-mat.supr-con

Tunneling dynamics between superconducting bound states at the atomic limit

Despite plenty of room at the bottom, there is a limit to the miniaturization of every process. For charge transport this is realized by the coupling of single discrete energy levels at the atomic scale. Here, we demonstrate sequential tunneling between parity protected Yu-Shiba-Rusinov (YSR) states bound to magnetic impurities located on the superconducting tip and sample of a scanning tunneling microscope at 10 mK. We reduce the relaxation of the excited YSR state to the bare minimum and find an enhanced lifetime for single quasiparticle levels. Our work offers a way to characterize and to manipulate coupled superconducting bound states, such as Andreev levels, YSR states, or Majorana bound states.

cond-mat.supr-con