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Understanding the interplay between individual magnetic impurities and superconductivity is crucial for bottom-up construction of novel phases of matter. For decades, the description by Yu, Shiba and Rusinov (YSR) of single spins in a superconductor and its extension to include quantum effects has proven highly successful: the pair-breaking potential of the spin generates sub-gap electron- and hole excitations that are energetically equidistant from zero. By tuning the energy of the sub-gap states through zero, the impurity screening by the superconductor makes the ground state gain or lose an electron, signalling a parity breaking quantum phase transition. Here we show that in multi-orbital impurities, correlations between the in-gap states can conversely lead to a quantum phase transition where more than one electron simultaneously leave the impurity without significant effect of the screening by the superconductor, while the parity may remain unchanged. This finding implies that the YSR treatment is not always valid, and that intra-atomic interactions, particularly Hund's coupling that favours high spin configurations, are an essential ingredient for understanding the sub-gap states. The interaction-driven quantum phase transition should be taken into account for impurity-based band-structure engineering, and may provide a fruitful basis in the search for novel physics., Comment: Main text and supplementary

We study the optical rectification in a metallic tunnel junction. We consider a planar junction in a Kretschmann configuration and measure the photon-assisted tunneling under infrared illumination at $\lambda= 1.5\, \mu \mathrm{m}$. To address the microscopic mechanism at the origin of the optical rectification, we compare the photon assisted current and the current-voltage characteristics of the junction measured on a voltage range much greater than $V_0=\frac{hc}{e\lambda}=0.825 \, \mathrm{V}$. The experimental results do not agree with the Tucker theory based on the exchange of energy quanta between electrons and photons and describing the dc current induced by photon-assisted processes in terms of a linear combination of the shifted characteristics $I(V)$ and $I(V\pm V_0)$. We show instead that the illumination power mainly goes into heating and that the rectification results mainly from the non-linearity of the tunnel junction at optical frequency.

In conventional Bardeen-Cooper-Scrieffer (BCS) superconductors, Cooper pairs of electrons of opposite spin (i.e. singlet structure) form the ground state. Equal spin triplet pairs (ESTPs), as in superfluid $^3$He, are of great interest for superconducting spintronics and topological superconductivity, yet remain elusive. Recently, odd-parity ESTPs were predicted to arise in (few-)monolayer superconducting NbSe$_2$, from the non-colinearity between the out-of-plane Ising spin-orbit field (due to the lack of inversion symmetry in monolayer NbSe$_2$) and an applied in-plane magnetic field. These ESTPs couple to the singlet order parameter at finite field. Using van der Waals tunnel junctions, we perform spectroscopy of superconducting NbSe$_2$ flakes, of 2--25 monolayer thickness, measuring the quasiparticle density of states (DOS) as a function of applied in-plane magnetic field up to 33T. In flakes $\lesssim$ 15 monolayers thick the DOS has a single superconducting gap. In these thin samples, the magnetic field acts primarily on the spin (vs orbital) degree of freedom of the electrons, and superconductivity is further protected by the Ising field. The superconducting energy gap, extracted from our tunnelling spectra, decreases as a function of the applied magnetic field. However, in bilayer NbSe$_2$, close to the critical field (up to 30T, much larger than the Pauli limit), superconductivity appears to be more robust than expected from Ising protection alone. Our data can be explained by the above-mentioned ESTPs.

In the spin energy excitation mode of normal metals and superconductors, spin up and down electrons (or quasiparticles) carry different heat currents. This mode occurs only when spin up and down energy distribution functions are non-identical, most simply when the two spins have different effective temperatures, and can be excited by spin-polarised current injection into the system. While evidence for spin-dependent heat transport has been observed in a normal metal, these measurements averaged over the distribution function of the electrons. By performing spectroscopy of quasiparticle populations in a mescoscopic superconductor, we reveal distribution functions which are strongly out-of-equilibrium, i.e. non-Fermi-Dirac. In addition, unlike in normal metals, the spin energy mode in superconductors is associated with a charge imbalance (different numbers of hole- and electron-like quasiparticles) at the superconducting gap edge, in finite Zeeman magnetic fields. Our spectroscopic technique allows us to observe this charge imbalance and thus unambiguously identify the spin energy mode. Our results agree well with theory and contribute to laying the foundation for spin caloritronics with superconductors.

Single atom manipulation within doped correlated electron systems would be highly beneficial to disentangle the influence of dopants, structural defects and crystallographic characteristics on their local electronic states. Unfortunately, their high diffusion barrier prevents conventional manipulation techniques. Here, we demonstrate the possibility to reversibly manipulate select sites in the optimally doped high temperature superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+x}$ using the local electric field of the tip. We show that upon shifting individual Bi atoms at the surface, the spectral gap associated with superconductivity is seen to reversibly change by as much as 15 meV (~5% of the total gap size). Our toy model that captures all observed characteristics suggests the field induces lateral movement of point-like objects that create a local pairing potential in the CuO2 plane., Comment: Published in Science, this is the originally submitted manuscript prior to changes during the review process

Detailed understanding of the role of single dopant atoms in host materials has been crucial for the continuing miniaturization in the semiconductor industry as local charging and trapping of electrons can completely change the behaviour of a device. Similarly, as dopants can turn a Mott insulator into a high temperature superconductor, their electronic behaviour at the atomic scale is of much interest. Due to limited time resolution of conventional scanning tunnelling microscopes, most atomic scale studies in these systems focussed on the time averaged effect of dopants on the electronic structure. Here, by using atomic scale shot-noise measurements in the doped Mott insulator Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+x}$, we visualize sub-nanometer sized objects where remarkable dynamics leads to an enhancement of the tunnelling current noise by at least an order of magnitude. From the position, current and energy dependence we argue that these defects are oxygen dopant atoms that were unaccounted for in previous scanning probe studies, whose local environment leads to charge dynamics that strongly affect the tunnelling mechanism. The unconventional behaviour of these dopants opens up the possibility to dynamically control doping at the atomic scale, enabling the direct visualization of the effect of local charging on e.g. high T$_{\text{c}}$ superconductivity., Comment: 12 pages, 4 figures, Supplementary Information included as ancillary file

The characteristic frequencies of a system provide important information on the phenomena that govern its physical properties. In this framework, there has recently been renewed interest in cryogenic microwave characterization for condensed matter systems since it allows to probe energy scales of the order of a few $\mu$eV. However, broadband measurements of the absolute value of a sample response in this frequency range are extremely sensitive to its environment and require a careful calibration. In this paper, we present an \textit{in situ} calibration method for cryogenic broadband microwave reflectometry experiments that is both simple to implement and through which the effect of the sample electromagnetic environment can be minimized. The calibration references are here provided by the sample itself, at three reference temperatures where its impedance is assumed or measured, and not by external standards as is usual. We compare the frequency-dependent complex impedance (0.1--2 GHz) of an a-Nb$_{15}$Si$_{85}$ superconducting thin film obtained through this Sample-Based Calibration (SBC) and through an Open-Short-Load Standard Calibration (SC) when working at very low temperature (0.02--4 K) and show that the SBC allows us to obtain the absolute response of the sample. This method brings the calibration planes as close as possible to the sample, so that the environment electrodynamic response does not affect the measurement, provided it is temperature independent. This results in a heightened sensitivity, for a given experimental set--up.

The excitations in conventional superconductors, Bogoliubov quasiparticles, are spin-1/2 fermions but their charge is energy-dependent and, in fact, zero at the gap edge. Therefore, in superconductors (unlike normal metals) the spin and charge degrees of freedom may be separated. In this article, we review spin injection into conventional superconductors and focus on recent experiments on mesoscopic superconductors. We show how quasiparticle spin transport and out-of-equilibrium spin dependent superconductivity can be triggered using the Zeeman splitting of the quasiparticle density of states in thin-film superconductors with small spin-mixing scattering. Finally, we address the spin dynamics and the feedback of quasiparticle spin imbalances on the strength of the superconducting energy gap., Comment: 18 pages, 5 figures

Spin/magnetisation relaxation and coherence times, respectively T_1 and T_2, initially defined in the context of nuclear magnetic resonance (NMR), are general concepts applicable to a wide range of systems, including quantum bits [1-4]. At first glance, these ideas might seem to be irrelevant to conventional Bardeen-Cooper-Schrieffer (BCS) superconductors, as the BCS superconducting ground state is a condensate of Cooper pairs of electrons with opposite spins (in a singlet state) [5]. It has recently been demonstrated, however, that a non-equilibrium magnetisation can appear in the quasiparticle (i.e. excitation) population of a conventional superconductor, with relaxation times on the order of several nanoseconds [6-10]. This raises the question of the spin coherence time of quasiparticles in superconductors and whether this can be measured through resonance experiments analogous to NMR and electron spin resonance (ESR). We have performed such measurements in aluminium and find a quasiparticle spin coherence time of 95+/-20ps., Comment: 12 pages, 3 figures + Supp. Info

We have measured the lifetime of spin imbalances in the quasiparticle population of a superconductor ($\tau_s$) in the frequency domain. A time-dependent spin imbalance is created by injecting spin-polarised electrons at finite excitation frequencies into a thin-film mesoscopic superconductor (Al) in an in-plane magnetic field (in the Pauli limit). The time-averaged value of the spin imbalance signal as a function of excitation frequency, $f_{RF}$ shows a cut-off at $f_{RF} \approx 1/(2\pi\tau_s)$. The spin imbalance lifetime is relatively constant in the accessible ranges of temperatures, with perhaps a slight increase with increasing magnetic field. Taking into account sample thickness effects, $\tau_s$ is consistent with previous measurements and of the order of the electron-electron scattering time $\tau_{ee}$. Our data are qualitatively well-described by a theoretical model taking into account all quasiparticle tunnelling processes from a normal metal into a superconductor., Comment: Includes Supplementary Information

We study the spin and charge accumulation in junctions between a superconductor and a ferromagnet or a normal metal in the presence of a Zeeman magnetic field, when the junction is taken out of equilibrium by applying a voltage bias. We write down the most general form for the spin and charge current in such junctions, taking into account all spin-resolved possible tunneling processes. We make use of these forms to calculate the spin accumulation in NS junctions subjected to a DC bias, and to an AC bias, sinusoidal or rectangular. We observe that in the limit of negligeable changes on the superconducting gap, the NS dynamical conductance is insensitive to spin imbalance. Therefore to probe the spin accumulation in the superconductor, one needs to separate the injection and detection point, i. e. the electrical spin detection must be non-local. We address also the effect of the spin accumulation induced in the normal leads by driving a spin current and its effects on the detection of the spin accumulation in the superconductor. Finally, we investigate the out-of-equilibrium spin susceptibility of the SC, and we show that it deviates drastically from it's equilibrium value.

Reflection measurements give access to the complex impedance of a material on a wide frequency range. This is of interest to study the dynamical properties of various materials, for instance disordered superconductors. However reflection measurements made at cryogenic temperature suffer from the difficulty to reliably subtract the circuit contribution. Here we report on the design and first tests of a setup able to precisely calibrate in situ the sample reflection, at 4.2 K and up to 2 GHz, by switching and measuring, during the same cool down, the sample and three calibration standards., Comment: (6 pages, 6 figures)

What happens to spin-polarised electrons when they enter a superconductor? Superconductors at equilibrium and at finite temperature contain both paired particles (of opposite spin) in the condensate phase as well as unpaired, spin-randomised quasiparticles. Injecting spin-polarised electrons into a superconductor thus creates both spin and charge imbalances [1, 2, 3, 4, 5, 6, 7] (respectively Q* and S*, cf. Ref. [4]). These must relax when the injection stops, but not necessarily over the same time (or length) scale as spin relaxation requires spin-dependent interactions while charge relaxation does not. These different relaxation times can be probed by creating a dynamic equilibrium between continuous injection and relaxation, which leads to constant-in-time spin and charge imbalances. These scale with their respective relaxation times and with the injection current. While charge imbalances in superconductors have been studied in great detail both theoretically [8] and experimentally [9], spin imbalances have not received much experimental attention [6, 10] despite intriguing theoretical predictions of spin-charge separation effects [11, 12]. These could occur e.g. if the spin relaxation time is longer than the charge relaxation time, i.e. Q* relaxes faster than S*. Fundamentally, spin-charge decoupling in superconductors is possible because quasiparticles can have any charge between e and -e, and also because the condensate acts as a particle reservoir [13, 11, 12]. Here we present evidence for an almost-chargeless spin imbalance in a mesoscopic superconductor.

An extended Josephson junction consists of two superconducting electrodes that are separated by an insulator and it is therefore also a microwave cavity. The superconducting phase difference across the junction determines the supercurrent as well as its spatial distribution. Both, an external magnetic field and a resonant cavity intrafield produce a spatial modification of the superconducting phase along the junction. The interplay between these two effects leads to interference in the critical current of the junction and allows us to continuously tune the coupling strength between the first cavity mode and the Josephson phase from 1 to -0.5. This enables static and dynamic control over the junction in the ultra-strong coupling regime., Comment: 4 pages, 3 figures

An extended Josephson junction intrinsically couples the superconducting current to the microwave cavity in the insulating barrier. We demonstrate that this coupling produces sidebands in the microwave cavity resonances of the junction. By measuring the switching current distribution, we show that microwave radiation at sidebands brings the Josephson phase out of equilibrium. In particular, the effective phase temperature is reduced or enhanced through anti-Stokes and Stokes scattering, respectively. Phase cooling and heating both increase with microwave power., Comment: 4 pages, 4 figures

We show experimentally and theoretically that there is a coupling via the Aharonov-Bohm phase between the order parameter of a ferromagnet and a singlet, s-wave, Josephson supercurrent. We have investigated the possibility of measuring the dispersion of such spin waves by varying the magnetic field applied in the plane of the junction and demonstrated the electromagnetic nature of the coupling by the observation of magnetic resonance side-bands to microwave induced Shapiro steps., Comment: 6 pages, 5 figures

We use microwave excitation to elucidate the dynamics of long superconductor / normal metal / superconductor Josephson junctions. By varying the excitation frequency in the range 10 MHz - 40 GHz, we observe that the critical and retrapping currents, deduced from the dc voltage vs. dc current characteristics of the junction, are set by two different time scales. The critical current increases when the ac frequency is larger than the inverse diffusion time in the normal metal, whereas the retrapping current is strongly modified when the excitation frequency is above the electron-phonon rate in the normal metal. Therefore the critical and retrapping currents are associated with elastic and inelastic scattering, respectively.

Via a direct coupling between the magnetic order parameter and the singlet Josephson supercurrent, we detect spin-wave resonances, and their dispersion, in ferromagnetic Josephson junctions in which the usual insulating or metallic barrier is replaced with a weak ferromagnet. The coupling arises within the Fraunhofer interferential description of the Josephson effect, because the magnetic layer acts as a time dependent phase plate. A spin-wave resonance at a frequency ws implies a dissipation that is reflected as a depression in the current-voltage curve of the Josephson junction when hbar ws = 2eV. We have thereby performed a resonance experiment on only 10^7 Ni atoms., Comment: 4 pages, 4 figures

We have investigated the classical phase dynamics of underdamped ferromagnetic Josephson junctions by measuring the switching probability in both the stationary and nonstationary regimes down to 350 mK. We found the escape temperature to be the bath temperature, with no evidence of additional spin noise. In the nonstationary regime, we have performed a pump-probe experiment on the Josephson phase by increasing the frequency of the junction current bias. We show that an incomplete energy relaxation leads to dynamical phase bifurcation. Bifurcation manifests itself as premature switching, resulting in a bimodal switching distribution. We directly measure the phase relaxation time by following the evolution of the bimodal switching distribution when varying the bias frequency. Numerical simulations account for the experimental values of the phase relaxation time., Comment: 4 pages, 3 figures

Hybrid Superconductor/Ferromagnet structures have been investigated recently to address the interplay between ferromagnetism and superconductivity. They also open up new routes for the investigation of out of equilibrium superconductivity. Here, we show how it is possible for out of equilibrium excitations produced in a superconducting thin film (S) to be localized in a ferromagnetic trap (F). Specifically, a ferromagnetic nano-volume in good contact with S represents a potential well for the quasiparticles (QPs) at the gap edge. As the superconducting proximity effect is highly suppressed in F, QPs get efficiently trapped and they share their energy with the free electrons in the trap. The electronic temperature Te in the trap can be increased by up to 60% from the bath temperature at 320 mK as measured by tunneling spectroscopy using a second junction.

We investigate the magnetic response of a superconducting Nb ring containing a ferromagnetic PdNi Josephson junction and a tunnel junction in parallel. A doubling of the switching frequency is observed within certain intervals of the external magnetic field. Assuming sinusoidal current-phase relations of both junctions our model of a dc-SQUID embedded within a superconducting ring explains this feature by a sequence of current reversals in the ferromagnetic section of the junction in these field intervals. The switching anomalies are induced by the coupling between the magnetic fluxes in the two superconducting loops., Comment: 5 pages, 4 figures

We report on a direct test of pairing fluctuations in the pseudogap regime of underdoped superconducting cuprates using a Josephson junction. In this experiment, the coupling between a rigid superconducting pair field and pairing fluctuations produces a strong specific signature in the current-voltage characteristics. Our results show that fluctuations survive only close to Tc (T-Tc<15K) and therefore cannot be responsible for the opening of the pseudogap at high temperature.

Reproducible high-Tc Josephson junctions have been made in a rather simple two-step process using ion irradiation. A microbridge (1 to 5 ?m wide) is firstly designed by ion irradiating a c-axis-oriented YBa2Cu3O7-? film through a gold mask such as the non-protected part becomes insulating. A lower Tc part is then defined within the bridge by irradiating with a much lower fluence through a narrow slit (20 nm) opened in a standard electronic photoresist. These planar junctions, whose settings can be finely tuned, exhibit reproducible and nearly ideal Josephson characteristics. This process can be used to produce complex Josephson circuits., Comment: 4 pages, 5 figures, to be published in Applied Physics Letters

The ground state of highly damped PdNi based 0-pi ferromagnetic Josephson junctions shows a spontaneous half quantum vortex, sustained by a supercurrent of undetermined sign. This supercurrent flows in the electrode of a Josephson junction used as a detector and produces a phi(0)/4 shift in its magnetic diffraction pattern. We have measured the statistics of the positive or negative sign shift occurring at the superconducting transition of such a junction. The randomness of the shift sign, the reproducibility of its magnitude and the possibility of achieving exact flux compensation upon field cooling: all these features show that 0-pi junctions behave as classical spins, just as magnetic nanoparticles with uniaxial anisotropy., Comment: 4 pages, 4 figures

We report a simple method for the fabrication of Niobium superconducting (SC) tips for scanning tunnelling microscopy which allow atomic resolution. The tips, formed in-situ by the mechanical breaking of a niobium wire, reveal a clear SC gap of 1.5 meV and a critical temperature Tc=9.2+-0.3 K as deduced from Superconductor Insulator Normal metal (NIS) and Superconductor Insulator Superconductor (SIS) spectra. These match the values of bulk Nb samples. We systematically find an enhanced value of the critical magnetic field in which superconductivity in the tip is destroyed (around 1 T for some tips) up to five times larger than the critical field of bulk Nb (0.21 T). Such enhancement is attributed to a size effect at the tip apex, Comment: to appear in Physica C

An experimental device was designed to measure the effect of the injection of spin-polarized carriers on the superconductive gap and density-of-states (DOS). Quasiparticles were injected from a ferromagnet ($Ni_{0.8}Fe_{0.2}$) through a tunnel junction into a conventional superconductor (Nb), while charge neutrality was maintained by a supercurrent. The DOS of the superconductor was measured through a second tunnel junction with a normal paramagnetic metal. No significant decrease of the superconductive gap was observed while a noticeable heating of the quasiparticles of the superconductor was measured. A similar experiment performed with current injected from a paramagnet (Al or Ag) showed no heating of quasiparticles. These observations are consistent with spin-charge separation of Bogoliubov quasi-particles and spin-bottleneck due to the enhanced recombination time of pure spin-excitations., Comment: minor replacements

We present magnetization measurements of mesoscopic superconducting niobium loops containing a ferromagnetic (PdNi) pi-junction. The loops are prepared on top of the active area of a micro Hall-sensor based on high mobility GaAs/AlGaAs heterostructures. We observe asymmetric switching of the loop between different magnetization states when reversing the sweep direction of the magnetic field. This provides evidence for a spontaneous current induced by the intrinsic phase shift of the pi-junction. In addition, the presence of the spontaneous current near zero applied field is directly revealed by an increase of the magnetic moment with decreasing temperature, which results in half integer flux quantization in the loop at low temperatures., Comment: 4 pages, 4 figures

We investigate Josephson coupling through a ferromagnetic thin film using Superconductor-Insulator-Ferromagnet-Superconductor planar junctions. Damped oscillations of the critical current are observed as a function of the ferromagnetic layer thickness. We show that they result from the exchange energy gained or lost by a quasiparticle Andreev-reflected at the ferromagnet-superconductor interface. The critical current cancels out at the transition from positive ("0") to negative ("$\pi$") coupling, in agreement with theoretical calculations., Comment: 4 pages, 4 figures

Planar tunneling spectroscopy reveals damped oscillations of the superconducting order parameter induced into a ferromagnetic thin film by the proximity effect. The oscillations are due to the finite momentum transfer provided to Cooper pairs by the splitting of the spin up and down bands in the ferromagnet. As a consequence, for negative values of the superconducting order parameter the tunneling spectra are capsized ("$\pi$-state"). The oscillations' damping and period are set by the same length scale, which depends on the spin polarization., Comment: 4 pages, 3 figures, submitted to PRL

We have made in-situ [103] and [110]YBCO/Pb junctions, which display an hysteretic behaviour with both a well-defined Quasi-Particule branch and a Josephson current. A zero energy conductance peak is observed in the tunneling conductance which is a signature of Andreev Bound States (ABS) at a surface of a d-wave superconductor. The observed splitting of this peak at low temperature may confirm the existence of a surface state which breaks time-reversal symmetry. However, up to now, we have not seen any evidence of a coupling between Josephson current and the zero-energy ABS, predicted by Y. Tanaka and S. Kashiwaya (PRB 56 p.892)., Comment: 5 pages with 2 eps figures, uses jltp.sty, to be published in Journal of Low Temperature Physics (Proceedings of the MOS'99 Conference)