Scientific Highlights

We report microscopic studies by muon spin rotation/relaxation as a function of pressure of the Ca₃Ir₄Sn₁₃ and Sr₃Ir₄Sn₁₃ cubic compounds, which are members of the (Ca_1−xSr_x)₃Ir₄Sn₁₃ system displaying superconductivity and a structural phase transition associated with the formation of a charge density wave (CDW). We find a strong enhancement of the superfluid density and a dramatic increase of the pairing strength above a pressure of ≈1.6 GPa, giving direct evidence of the presence of a quantum critical point separating a superconducting phase coexisting with CDW from a pure superconducting phase. The superconducting order parameter in both phases has the same s-wave symmetry. In spite of the conventional phonon-mediated BCS character of the weakly correlated (Ca_1−xSr_x)₃Ir₄Sn₁₃ system, the dependence of the effective superfluid density on the critical temperature puts this compound in the 'Uemura' plot close to unconventional superconductors. This system exemplifies that conventional BCS superconductors in the presence of competing orders or multiband structure can also display characteristics of unconventional superconductors.

The superconducting gap structure in iron-based high-temperature superconductors (Fe-HTSs) is non-universal. In contrast to other unconventional superconductors, in the Fe-HTSs both d-wave and extended s-wave pairing symmetries are close in energy. Probing the proximity between these very different superconducting states and identifying experi- mental parameters that can tune them is of central interest. Here we report high-pressure muon spin rotation experiments on the temperature-dependent magnetic penetration depth in the optimally doped nodeless s-wave Fe-HTS Ba_0.65Rb_0.35Fe₂As₂. Upon pressure, a strong decrease of the penetration depth in the zero-temperature limit is observed, while the superconducting transition temperature remains nearly constant. More importantly, the low- temperature behaviour of the inverse-squared magnetic penetration depth, which is a direct measure of the superfluid density, changes qualitatively from an exponential saturation at zero pressure to a linear-in-temperature behaviour at higher pressures, indicating that hydrostatic pressure promotes the appearance of nodes in the superconducting gap.

In 1933, Meissner and Ochsenfeld reported the expulsion of magnetic flux - the diamagnetic Meissner effect - from the interior of superconducting lead. This discovery was crucial in formulating the Bardeen-Cooper-Schrieffer (BCS) theory of superconductivity. In exotic superconducting systems BCS theory does not strictly apply. A classical example is a superconductor-magnet hybrid system where magnetic ordering breaks time-reversal symmetry of the superconducting condensate and results in the stabilization of an odd-frequency superconducting state. It has been predicted that under appropriate conditions, odd-frequency superconduc- tivity should manifest in the Meissner state as fluctuations in the sign of the magnetic susceptibility, meaning that the superconductivity can either repel (diamagnetic) or attract (paramagnetic) external magnetic flux. Here, we report local probe measurements of faint magnetic fields in a Au/Ho/Nb trilayer system using low-energy muons, where antiferromagnetic Ho (4.5 nm) breaks time-reversal symmetry of the proximity-induced pair correlations in Au. From depth-resolved measurements below the superconducting transition of Nb, we observe a local enhancement of the magnetic field in Au that exceeds the externally applied field, thus proving the existence of an intrinsic paramagnetic Meissner effect arising from an odd-frequency superconducting state.

Superconducting spintronics has emerged in the past decade as a promising new field that seeks to open a new dimension for nanoelectronics by utilizing the internal spin structure of the superconducting Cooper pair as a new degree of freedom. Its basic building blocks are spin-triplet Cooper pairs with equally aligned spins, which are promoted by proximity of a conventional superconductor to a ferromagnetic material with inhomogeneous macroscopic magnetization. Using low-energy muon spin-rotation experiments we find an unanticipated effect, in contradiction with the existing theoretical models of superconductivity and ferromagnetism: the appearance of a magnetization in a thin layer of a non-magnetic metal (gold), separated from a ferromagnetic double layer by a 50-nm-thick superconducting layer of Nb. The effect can be controlled either by temperature or by using a magnetic field to control the state of the remote ferromagnetic elements, and may act as a basic building block for a new generation of quantum interference devices based on the spin of a Cooper pair.

Materials with interacting magnetic degrees of freedom display a rich variety of magnetic behaviour that can lead to novel collective equilibrium and out-of-equilibrium phenomena. In equilibrium, thermodynamic phases appear with the associated phase transitions providing a characteristic signature of the underlying collective behaviour. Here we create a thermally active artificial kagome spin ice that is made up of a large array of dipolar interacting nanomagnets and undergoes phase transitions predicted by microscopic theory. We use low energy muon spectroscopy to probe the dynamic behaviour of the interacting nanomagnets and observe peaks in the muon relaxation rate that can be identified with the critical temperatures of the predicted phase transitions. This provides experimental evidence that a frustrated magnetic metamaterial can be engineered to admit thermodynamic phases.

The recent discovery of pressure (p) induced superconductivity in the binary helimagnet CrAs has raised questions on how superconductivity emerges from the magnetic state and on the mechanism of the superconducting pairing. In the present work the suppression of magnetism and the occurrence of superconductivity in CrAs were studied by means of muon spin rotation. The magnetism remains bulk up to p ≅ 3.5kbar while its volume fraction gradually decreases with increasing pressure until it vanishes at p ≅ 7kbar. At 3.5 kbar superconductivity abruptly appears with its maximum T_c ≅ 1.2K which decreases upon increasing the pressure. In the intermediate pressure region (3.5 ≤ p ≤ 7kbar) the superconducting and the magnetic volume fractions are spatially phase separated and compete for phase volume. Our results indicate that the less conductive magnetic phase provides additional carriers (doping) to the superconducting parts of the CrAs sample thus leading to an increase of the transition temperature (T_c) and of the superfluid density (ρ_s). A scaling of ρ_s with T_c^3.2 as well as the phase separation between magnetism and superconductivity point to a conventional mechanism of the Cooper-pairing in CrAs.

We report the low-temperature magnetic properties of Ce₂Sn₂O₇, a rare-earth pyrochlore. Our suscep- tibility and magnetization measurements show that due to the thermal isolation of a Kramers doublet ground state, Ce₂Sn₂O₇ has Ising-like magnetic moments of ∼1.18 μ_B. The magnetic moments are confined to the local trigonal axes, as in a spin ice, but the exchange interactions are antiferromagnetic. Below 1 K, the system enters a regime with antiferromagnetic correlations. In contrast to predictions for classical -Ising spins on the pyrochlore lattice, there is no sign of long-range ordering down to 0.02 K. Our results suggest that Ce₂Sn₂O₇ features an antiferromagnetic liquid ground state with strong quantum fluctuations.

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Only three elements are ferromagnetic at room temperature: the transition metals iron, cobalt and nickel. The Stoner criterion explains why iron is ferromagnetic but manganese, for example, is not, even though both elements have an unfilled 3d shell and are adjacent in the periodic table: according to this criterion, the product of the density of states and the exchange integral must be greater than unity for spontaneous spin ordering to emerge. Here we demonstrate that it is possible to alter the electronic states of non-ferromagnetic materials, such as diamagnetic copper and paramagnetic manganese, to overcome the Stoner criterion and make them ferromagnetic at room temperature. This effect is achieved via interfaces between metallic thin films and C₆₀ molecular layers. The emergent ferromagnetic state exists over several layers of the metal before being quenched at large sample thicknesses by the material’s bulk properties. Although the induced magnetization is easily measurable by magnetometry, low-energy muon spin spectroscopy provides insight into its distribution by studying the depolarization process of low-energy muons implanted in the sample. This technique indicates localized spin-ordered states at, and close to, the metal–molecule interface. Density functional theory simulations suggest a mechanism based on magnetic hardening of the metal atoms, owing to electron transfer. This mechanism might allow for the exploitation of molecular coupling to design magnetic metamaterials using abundant, non-toxic components such as organic semiconductors. Charge transfer at molecular interfaces may thus be used to control spin polarization or magnetization, with consequences for the design of devices for electronic, power or computing applications.

In the generic phase diagram of heavy fermion systems, tuning an external parameter such as hydrostatic or chemical pressure modifies the superconducting transition temperature. The superconducting phase forms a dome in the temperature-tuning parameter phase diagram, which is associated with a maximum of the superconducting pairing interaction. Proximity to antiferromagnetism suggests a relation between the disappearance of antiferromagnetic order and superconductivity. We combine muon spin rotation, neutron scattering, and x-ray absorption spectroscopy techniques to gain access to the magnetic and electronic structure of CeCo(In_1−xCd_x)₅ at different time scales. Different magnetic structures are obtained that indicate a magnetic order of itinerant character, coexisting with bulk superconductivity. The suppression of the antiferromagnetic order appears to be driven by a modification of the bandwidth/carrier concentration, implying that the electronic structure and consequently the interplay of superconductivity and magnetism is strongly affected by hydrostatic and chemical pressure.

The superconducting properties of LaFeAsO_1−xF_x under conditions of optimal electron doping are investigated upon the application of external pressure up to ∼23 kbar. Measurements of muon-spin spectroscopy and dc magnetometry evidence a clear mutual independence between the critical temperature T_c and the low-temperature saturation value for the ratio n_s/m^* (superfluid density over effective band mass of Cooper pairs). Remarkably, a dramatic increase of ∼30% is reported for n_s/m^* at the maximum pressure value while T_c is substantially unaffected in the whole accessed experimental window. We argue and demonstrate that the explanation for the observed results must take the effect of nonmagnetic impurities on multiband superconductivity into account. In particular, the unique possibility to modify the ratio between intraband and interband scattering rates by acting on structural parameters while keeping the amount of chemical disorder constant is a striking result of our proposed model.

Materials with broad absorption bands are highly desirable for electromagnetic filtering and processing applications, especially if the absorption can be externally controlled. Here, a new class of broadband-absorption materials is introduced. Namely, layered metamagnets exhibit an electromagnetic excitation continuum in the magnetic-field-induced mixed ferro- and antiferromagnetic phase. Employing a series of complementary experimental techniques involving neutron scattering, muon spin relaxation, specific heat, ac and dc magnetization measurements, and electron magnetic resonance, a detailed magnetic phase diagram of Cu₃Bi(SeO₃)₂O₂Br is determined and it is found that the excitations in the mixed phase extend over at least ten decades of frequency. The results, which reveal a new dynamical aspect of the mixed phase in metamagnets, open up a novel approach to controllable microwave filtering.

Inhomogeneity in the ground state is an intriguing, emergent phenomenon in magnetism. Recently, it has been observed in the magnetostructural channel of the geometrically frustrated α-NaMnO₂, for the first time in the absence of active charge degrees of freedom. Here we report an in-depth numerical and local-probe experimental study of the isostructural sister compound CuMnO₂ that emphasizes and provides an explanation for the crucial differences between the two systems. The experimentally verified, much more homogeneous, ground state of the stoichiometric CuMnO₂ is attributed to the reduced magnetoelastic competition between the counteracting magnetic-exchange and elastic-energy contributions. The comparison of the two systems additionally highlights the role of disorder and allows the understanding of the puzzling phenomenon of phase separation in uniform antiferromagnets.

Diamagnetic oxides can, under certain conditions, become ferromagnetic at room temperature and therefore are promising candidates for future material in spintronic devices. Contrary to early predictions, doping ZnO with uniformly distributed magnetic ions is not essential to obtain ferromagnetic samples. Instead, the nanostructure seems to play the key role, as room temperature ferromagnetism was also found in nanograined, undoped ZnO. However, the origin of room temperature ferromagnetism in primarily non–magnetic oxides like ZnO is still unexplained and a controversial subject within the scientific community. Using low energy muon spin relaxation in combination with SQUID and TEM techniques, we demonstrate that the magnetic volume fraction is strongly related to the sample volume fraction occupied by grain boundaries. With molecular dynamics and density functional theory we find ferromagnetic coupled electron states in ZnO grain boundaries. Our results provide evidence and a microscopic model for room temperature ferromagnetism in oxides.

Hydrogen in the Earth's deep interior has been thought to exist as a hydroxyl group in high-pressure minerals. We present Muon Spin Rotation experiments on SiO₂ stishovite, which is an archetypal high-pressure mineral. Positive muon (which can be considered as a light isotope of proton) implanted in stishovite was found to capture electron to form muonium (corresponding to neutral hydrogen). The hyperfine-coupling parameter and the relaxation rate of spin polarization of muonium in stishovite were measured to be very large, suggesting that muonium is squeezed in small and anisotropic interstitial voids without binding to silicon or oxygen. These results imply that hydrogen may also exist in the form of neutral atomic hydrogen in the deep mantle.

Superconductivity is a striking example of a quantum phenomenon in which electrons move coherently over macroscopic distances without scattering. The high-temperature superconducting oxides (cuprates) are the most studied class of superconductors, composed of two-dimensional CuO₂ planes separated by other layers that control the electron concentration in the planes. A key unresolved issue in cuprates is the relationship between superconductivity and magnetism. Here we report a sharp phase boundary of static three-dimensional magnetic order in the electron-doped superconductor La_2-xCe_xCuO_4-δ, where small changes in doping or depth from the surface switch the material from superconducting to magnetic. Using low-energy spin-polarized muons, we find that static magnetism disappears close to where superconductivity begins and well below the doping level at which dramatic changes in the transport properties are reported. These results indicate a higher degree of symmetry between the electron and hole-doped cuprates than previously thought.

We have studied the magnetic and superconducting properties of Ba(Fe_0.95Co_0.05)₂As₂ as a function of temperature and external magnetic field using neutron scattering and muon spin rotation. Below the superconducting transition temperature the magnetic and superconducting order parameters coexist and compete. A magnetic field can significantly enhance the magnetic scattering in the superconducting state, roughly doubling the Bragg intensity at 13.5T. We perform a microscopic modeling of the data by use of a five-band Hamiltonian relevant to iron pnictides. In the superconducting state, vortices can slow down and freeze spin fluctuations locally. When such regions couple they result in a long-range ordered antiferromagnetic phase producing the enhanced magnetic elastic scattering in agreement with experiments.

Although muon spin relaxation is commonly used to probe local magnetic order, spin freezing, and spin dynamics, we identify an experimental situation in which the measured response is dominated by an effect resulting from the muon-induced local distortion rather than the intrinsic behavior of the host compound. We demonstrate this effect in some quantum spin ice candidate materials Pr₂B₂O₇ (B = Sn, Zr, Hf), where we detect a static distribution of magnetic moments that appears to grow on cooling. Using density functional theory we show how this effect can be explained via a hyperfine enhancement arising from a splitting of the non-Kramers doublet ground states on Pr ions close to the muon, which itself causes a highly anisotropic distortion field. We provide a quantitative relationship between this effect and the measured temperature dependence of the muon relaxation and discuss the relevance of these observations to muon experiments in other magnetic materials.

Superconducting [(Li_1-xFe_x)OH](Fe_1-yLi_y)Se (x≈0.2, y≈0.08) was synthesized by hydrothermal methods and characterized by single-crystal and powder X-ray diffrac- tion. The structure contains alternating layers of anti-PbO type (Fe_1-yLi_y)Se and (Li_1-xFe_x)OH. Electrical resistivity and magnetic susceptibility measurements reveal superconductivity at 43K. An anomaly in the diamagnetic shielding indicates ferromagnetic ordering near 10K while superconductivity is retained. The ferromagnetism is from the iron atoms in the (Li_1-xFe_x)OH layer. Isothermal magnetization measurements confirm the superposition of ferromagnetic and superconduct- ing hysteresis. The internal ferromagnetic field is larger than the lower, but smaller than the upper critical field of the superconductor. The formation of a spontaneous vortex phase where both orders coexist is supported by ⁵⁷Fe-Mössbauer spectra, ⁷Li-NMR spectra, and μSR experiments.