Discovery of charge order in a cuprate Mott insulator.

Copper oxide superconductors universally exhibit multiple forms of electronically ordered phases that break the native translational symmetry of the CuO2 planes. In underdoped cuprates with correlated metallic ground states, charge/spin stripes and incommensurate charge density waves (CDWs) have been experimentally observed over the years, while early theoretical studies also predicted the emergence of a Coulomb-frustrated 'charge crystal' phase in the very lightly doped, insulating limit of CuO2 planes. Here, we search for signatures of CDW order in very lightly hole-doped cuprates from the 123 family RBa2Cu3O7 - δ (RBCO; R: Y or rare earth), by using resonant X-ray scattering, electron transport, and muon spin rotation measurements to resolve the electronic and magnetic ground states fully. Specifically, Pr is used to substitute Y at the R-site to systematically suppress the superconductivity and access the extremely low hole-doping regime of the cuprate phase diagram without changing the oxygen stoichiometry. X-ray scattering data taken on Pr-doped YBCO thin films reveal an in-plane CDW order that follows the same linear evolution of wave vector versus hole concentration as oxygen-underdoped YBCO but extends all the way to the insulating and magnetically ordered Mott limit. Combined with the recent observation of charge crystal phase on an insulating surface of Bi2Sr2CaCu2O8 + z, our results in RBCO suggest that this electronic symmetry breaking is universally present in very lightly doped CuO2 planes. These findings bridge the gap between the Mott insulating state and the underdoped metallic state and underscore the prominent role that Coulomb-frustrated electronic phase separation plays among all cuprates.

Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films.

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

Emergent Magnetism with Continuous Control in the Ultrahigh-Conductivity Layered Oxide PdCoO2.

The current challenge to realizing continuously tunable magnetism lies in our inability to systematically change properties, such as valence, spin, and orbital degrees of freedom, as well as crystallographic geometry. Here, we demonstrate that ferromagnetism can be externally turned on with the application of low-energy helium implantation and can be subsequently erased and returned to the pristine state via annealing. This high level of continuous control is made possible by targeting magnetic metastability in the ultrahigh-conductivity, nonmagnetic layered oxide PdCoO2 where local lattice distortions generated by helium implantation induce the emergence of a net moment on the surrounding transition metal octahedral sites. These highly localized moments communicate through the itinerant metal states, which trigger the onset of percolated long-range ferromagnetism. The ability to continuously tune competing interactions enables tailoring precise magnetic and magnetotransport responses in an ultrahigh-conductivity film and will be critical to applications across spintronics.

Proximity-Induced Odd-Frequency Superconductivity in a Topological Insulator.

At an interface between a topological insulator (TI) and a conventional superconductor (SC), superconductivity has been predicted to change dramatically and exhibit novel correlations. In particular, the induced superconductivity by an s-wave SC in a TI can develop an order parameter with a p-wave component. Here we present experimental evidence for an unexpected proximity-induced novel superconducting state in a thin layer of the prototypical TI, Bi_{2}Se_{3} proximity coupled to Nb. From depth-resolved magnetic field measurements below the superconducting transition temperature of Nb, we observe a local enhancement of the magnetic field in Bi_{2}Se_{3} that exceeds the externally applied field, thus supporting the existence of an intrinsic paramagnetic Meissner effect arising from an odd-frequency superconducting state. Our experimental results are complemented by theoretical calculations supporting the appearance of such a component at the interface which extends into the TI. This state is topologically distinct from the conventional Bardeen-Cooper-Schrieffer state it originates from. To the best of our knowledge, these findings present a first observation of bulk odd-frequency superconductivity in a TI. We thus reaffirm the potential of the TI-SC interface as a versatile platform to produce novel superconducting states.

Interface-induced superconductivity in magnetic topological insulators.

The interface between two different materials can show unexpected quantum phenomena. In this study, we used molecular beam epitaxy to synthesize heterostructures formed by stacking together two magnetic materials, a ferromagnetic topological insulator (TI) and an antiferromagnetic iron chalcogenide (FeTe). We observed emergent interface-induced superconductivity in these heterostructures and demonstrated the co-occurrence of superconductivity, ferromagnetism, and topological band structure in the magnetic TI layer-the three essential ingredients of chiral topological superconductivity (TSC). The unusual coexistence of ferromagnetism and superconductivity is accompanied by a high upper critical magnetic field that exceeds the Pauli paramagnetic limit for conventional superconductors at low temperatures. These magnetic TI/FeTe heterostructures with robust superconductivity and atomically sharp interfaces provide an ideal wafer-scale platform for the exploration of chiral TSC and Majorana physics.

Spatially homogeneous ferromagnetism below the enhanced Curie temperature in EuO(1-x) thin films.

We have used low-energy implanted muons as a volume sensitive probe of the magnetic properties of EuO(1-x) thin films. We find that static and homogeneous magnetic order persists up to the elevated T(C) in the doped samples, and the muon signal displays the double dome feature also observed in the sample magnetization. Our results appear incompatible with either the magnetic phase separation or bound magnetic polaron descriptions previously suggested to explain the elevated T(C), but are compatible with an RKKY-like interaction mediating magnetic interactions above 69 K.

Metal-insulator transition in composition-tuned nickel oxide films.

Thin films of the solid solution Nd1-xLaxNiO3are grown in order to study the expected 0 K phase transitions at a specific composition. We experimentally map out the structural, electronic and magnetic properties as a function ofxand a discontinuous, possibly first order, insulator-metal transition is observed at low temperature whenx= 0.2. Raman spectroscopy and scanning transmission electron microscopy show that this is not associated with a correspondingly discontinuous global structural change. On the other hand, results from density functional theory (DFT) and combined DFT and dynamical mean field theory calculations produce a 0 K first order transition at around this composition. We further estimate the temperature-dependence of the transition from thermodynamic considerations and find that a discontinuous insulator-metal transition can be reproduced theoretically and implies a narrow insulator-metal phase coexistence withx. Finally, muon spin rotation (µSR) measurements suggest that there are non-static magnetic moments in the system that may be understood in the context of the first order nature of the 0 K transition and its associated phase coexistence regime.

Efficient magnetic switching in a correlated spin glass.

The interplay between spin-orbit interaction and magnetic order is one of the most active research fields in condensed matter physics and drives the search for materials with novel, and tunable, magnetic and spin properties. Here we report on a variety of unique and unexpected observations in thin multiferroic Ge1-xMnxTe films. The ferrimagnetic order parameter in this ferroelectric semiconductor is found to switch direction under magnetostochastic resonance with current pulses many orders of magnitude lower as for typical spin-orbit torque systems. Upon a switching event, the magnetic order spreads coherently and collectively over macroscopic distances through a correlated spin-glass state. Utilizing these observations, we apply a novel methodology to controllably harness this stochastic magnetization dynamics.

Measurement of the transition frequency from 2S1/2, F = 0 to 2P1/2, F = 1 states in Muonium.

Muons are puzzling physicists since their discovery when they were first thought to be the meson predicted by Yukawa to mediate the strong force. The recent result at Fermilab on the muon g-2 anomaly puts the muonic sector once more under the spotlight and calls for further measurements with this particle. Here, we present the results of the measurement of the 2S1/2, F = 0 → 2P1/2, F = 1 transition in Muonium. The measured value of 580.6(6.8) MHz is in agreement with the theoretical calculations. A value of the Lamb shift of 1045.5(6.8) MHz is extracted, compatible with previous experiments. We also determine the 2S hyperfine splitting in Muonium to be 559.6(7.2) MHz. The measured transition being isolated from the other hyperfine levels holds the promise to provide an improved determination of the Muonium Lamb shift at a level where bound state QED recoil corrections not accessible in hydrogen could be tested. This result would be sensitive to new physics in the muonic sector, e.g., to new bosons which might provide an explanation of the g-2 muon anomaly and allow to test Lorentz and CPT violation. We also present the observation of Muonium in the n = 3 excited state opening up the possibility of additional precise microwave measurements.

Phase transition in the cuprates from a magnetic-field-free stiffness meter viewpoint.

A method to measure the superconducting (SC) stiffness tensor [Formula: see text], without subjecting the sample to external magnetic field, is applied to La1.875Sr0.125CuO4. The method is based on the London equation [Formula: see text], where J is the current density and A is the vector potential which is applied in the SC state. Using rotor free A and measuring J via the magnetic moment of superconducting rings, [Formula: see text] at T → Tc is extracted. The technique is sensitive to very small stiffnesses (penetration depths on the order of a few millimeters). The method is applied to two different rings: one with the current running only in the CuO2 planes, and another where the current must cross planes. We find different transition temperatures for the two rings, namely, there is a temperature range with two-dimensional stiffness. Additional low energy muon spin rotation measurements on the same sample determine the stiffness anisotropy at T < Tc.

Isotope effects on the spin dynamics of single-molecule magnets probed using muon spin spectroscopy.

Muon spin relaxation (µSR) experiments on a single-molecule magnet enriched in different Dy isotopes detect unambiguously the slowing down of the zero field spin dynamics for the non-magnetic isotope. This occurs in the low temperature regime dominated by quantum tunnelling, in agreement with previous ac susceptibility investigations. In contrast to the latter, however, µSR is sensitive to all fluctuation modes affecting the lifetime of the spin levels.

Collective magnetism in an artificial 2D XY spin system.

Two-dimensional magnetic systems with continuous spin degrees of freedom exhibit a rich spectrum of thermal behaviour due to the strong competition between fluctuations and correlations. When such systems incorporate coupling via the anisotropic dipolar interaction, a discrete symmetry emerges, which can be spontaneously broken leading to a low-temperature ordered phase. However, the experimental realisation of such two-dimensional spin systems in crystalline materials is difficult since the dipolar coupling is usually much weaker than the exchange interaction. Here we realise two-dimensional magnetostatically coupled XY spin systems with nanoscale thermally active magnetic discs placed on square lattices. Using low-energy muon-spin relaxation and soft X-ray scattering, we observe correlated dynamics at the critical temperature and the emergence of static long-range order at low temperatures, which is compatible with theoretical predictions for dipolar-coupled XY spin systems. Furthermore, by modifying the sample design, we demonstrate the possibility to tune the collective magnetic behaviour in thermally active artificial spin systems with continuous degrees of freedom.

Robust Magnetic Properties of a Sublimable Single-Molecule Magnet.

The organization of single-molecule magnets (SMMs) on surfaces via thermal sublimation is a prerequisite for the development of future devices for spintronics exploiting the richness of properties offered by these magnetic molecules. However, a change in the SMM properties due to the interaction with specific surfaces is usually observed. Here we present a rare example of an SMM system that can be thermally sublimated on gold surfaces while maintaining its intact chemical structure and magnetic properties. Muon spin relaxation and ac susceptibility measurements are used to demonstrate that, unlike other SMMs, the magnetic properties of this system in thin films are very similar to those in the bulk, throughout the full volume of the film, including regions near the metal and vacuum interfaces. These results exhibit the robustness of chemical and magnetic properties of this complex and provide important clues for the development of nanostructures based on SMMs.

Iridates from the molecular side.

New exotic phenomena have recently been discovered in oxides of paramagnetic Ir(4+) ions, widely known as 'iridates'. Their remarkable properties originate from concerted effects of the crystal field, magnetic interactions and strong spin-orbit coupling, characteristic of 5d metal ions. Despite numerous experimental reports, the electronic structure of these materials is still challenging to elucidate, and not attainable in the isolated, but chemically inaccessible, [IrO6](8-) species (the simplest molecular analogue of the elementary {IrO6}(8-) fragment present in all iridates). Here, we introduce an alternative approach to circumvent this problem by substituting the oxide ions in [IrO6](8-) by isoelectronic fluorides to form the fluorido-iridate: [IrF6](2-). This molecular species has the same electronic ground state as the {IrO6}(8-) fragment, and thus emerges as an ideal model for iridates. These results may open perspectives for using fluorido-iridates as building-blocks for electronic and magnetic quantum materials synthesized by soft chemistry routes.

Interfacial dominated ferromagnetism in nanograined ZnO: a µSR and DFT study.

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.

Polymer dynamics near the surface and in the bulk of poly(tetrafluoroethylene) probed by zero-field muon-spin-relaxation spectroscopy.

The results of many experiments on polymers such as polystyrene indicate that the polymer chains near a free surface exhibit enhanced dynamics when compared with the bulk. We have investigated whether this is the case for poly(tetrafluoroethylene) (PTFE) by using zero-field muon-spin-relaxation spectroscopy to characterize a local probe, the F-Mu(+)-F state, which forms when spin-polarized positive muons are implanted in PTFE. Low-energy muons (implantation energies from 2.0 to 23.0 keV) were used to study the F-Mu(+)-F state between ∼ 23 and 191 nm from the free surface of PTFE. Measurements were also made with surface muons (4.1 MeV) where the mean implantation depth is on the order of ∼ 0.6 mm. The relaxation rate of the F-Mu(+)-F state up to ∼ 150 K was found to be significantly higher for muons implanted at 2.0 keV than for higher implantation energies, which suggests that the polymer chains in a region on the order of a few tens of nanometers from the free surface are more mobile than those in the bulk.

Depth-dependent spin dynamics in thin films of TbPc2 nanomagnets explored by low-energy implanted muons.

We present measurements of the magnetic properties of thin film TbPc(2) single-molecule magnets evaporated on a gold substrate and compare them to those in bulk. Zero-field muon spin relaxation measurements were used to determine the molecular spin fluctuation rate of TbPc(2) as a function of temperature. At low temperature, we find that the fluctuations in films are much faster than in bulk and depend strongly on the distance between the molecules and the Au substrate. We measure a molecular spin correlation time that varies between 1.4 µs near the substrate and 6.6 µs far away from it. We attribute this behavior to differences in the packing of the magnetic cores, which change gradually on the scale of ~10-20 nm away from the TbPc(2)/Au interface.