Low-energy Muon Spin Relaxation Research Articles

Proximate Quantum Spin Liquid on Designer Lattice.

Complementary to bulk synthesis, here we propose a designer lattice with extremely high magnetic frustration and demonstrate the possible realization of a quantum spin liquid state from both experiments and theoretical calculations. In an ultrathin (111) CoCr2O4 slice composed of three triangular and one kagome cation planes, the absence of a spin ordering or freezing transition is demonstrated down to 0.03 K, in the presence of strong antiferromagnetic correlations in the energy scale of 30 K between Co and Cr sublattices, leading to the frustration factor of ∼1000. Persisting spin fluctuations are observed at low temperatures via low-energy muon spin relaxation. Our calculations further demonstrate the emergence of highly degenerate magnetic ground states at the 0 K limit, due to the competition among multiply altered exchange interactions. These results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.

A Journey in Lanthanide Coordination Chemistry: From Evaporable Dimers to Magnetic Materials and Luminescent Devices.

ConspectusLanthanide ions are prime ingredients for the design of compounds, materials, and devices with unique magnetic and optical properties. Accordingly, coordination chemistry is one of the best tools for building molecular edifices from these ions because it allows careful control of the ions' environment and of the dimensionality of the final compound.In this Account, we review our results on lanthanide-based dimers. We show how a pure fundamental study on lanthanide coordination chemistry allows the investigation of a full continuum of results from the compound to materials and then to devices. The conversion of molecules into materials is a tricky task because it requires strong molecular robustness toward the surface deposition processes as well as the preservation and detectability of the molecular properties in the material. Additionally, the passage of a material toward a device implies a material with a given function, for example, a tailored response to an external stimulus.To do so, we targeted neutral and isolated molecules whose transfer on surfaces by chemi- or physisorption is much easier than that of charged molecules or extended coordination networks. Then, we focused on molecules with very strong evaporability to avoid wet chemistry deposition processes that are more likely to damage the molecules and/or distort their geometries.We thus designed lanthanide dimers based on fluorinated β-diketonates and pyridine-N-oxide ligands. As expected, they show remarkable evaporability but also strong luminescence and interesting magnetic behavior because they behave as single-molecule magnets (SMMs). Ligand substitutions and stoichiometric modifications allow the optimization of the geometric organization of the dimers in the crystal packing as well as their evaporability, SMM behavior, luminescent properties, or their ability to be anchored on surfaces. Most of all, this family of molecules shows a strong ability to form thick films on various substrates. This allows converting these molecules to magnetic materials and luminescent devices.Magnetic materials can be designed by creating thick films of the dimers deposited on gold. These films have been designed and investigated with the most advanced techniques of on-surface imaging (atomic force microscopy, AFM), on-surface physicochemical characterization (X-ray photoelectron spectroscopy (XPS), time of flight-secondary ion mass spectroscopy (Tof-SIMS)), and on-surface magnetic investigation (low-energy muon spin relaxation (LE-μSR)). Contrary to what was previously observed on other SMM films, no depth dependence of the SMM behavior was observed. This means that the dimers do not suffer from the vacuum or substrate interface and behave similarly, whatever their localization. This exceptional magnetic robustness is a key ingredient in the creation of materials for molecular magnetic data storage.Luminescent devices can be obtained by layering molecular films of the dimers with a copper-rich solid-state electrolyte between ITO/Pt electrodes. The electromigration of Cu2+ ions into films of Eu3+, Tb3+, and Dy3+ dimers quenches their luminescence. This luminescence tuning by electromigration is reversible, and this setup can be considered to be a proof of concept of full solid-state luminescent device where reversible coding can be tailored by an electric field. It is envisioned for optical data storage purposes. In the future, it could also benefit from the SMM properties of the molecules to pave the way toward multifunctional molecular data storage devices.

Intertwined magnetic, structural, and electronic transitions in V2O3

We present a coordinated study of the paramagnetic-to-antiferromagnetic, rhombohedral-to-monoclinic, and metal-to-insulator transitions in thin-film specimens of the classic Mott insulator V$_2$O$_3$ using low-energy muon spin relaxation, x-ray diffraction, and nanoscale-resolved near-field infrared spectroscopic techniques. The measurements provide a detailed characterization of the thermal evolution of the magnetic, structural, and electronic phase transitions occurring in a wide temperature range, including quantitative measurements of the high- and low-temperature phase fractions for each transition. The results reveal a stable coexistence of the high- and low-temperature phases over a broad temperature range throughout the transition. Careful comparison of temperature dependence of the different measurements, calibrated by the resistance of the sample, demonstrates that the electronic, magnetic, and structural degrees of freedom remain tightly coupled to each other during the transition process. We also find evidence for antiferromagnetic fluctuations in the vicinity of the phase transition, highlighting the important role of the magnetic degree of freedom in the metal-insulator transition.

Evidence for the homogeneous ferromagnetic phase in (Ga,Mn)(Bi,As) epitaxial layers from muon spin relaxation spectroscopy

Ferromagnetic semiconductor thin layers of the quaternary (Ga,Mn)(Bi,As) and reference, ternary (Ga,Mn)As compounds, epitaxially grown under either compressive or tensile strain, have been characterized from a perspective of structural and magnetization homogeneity. The quality and composition of the layers have been confirmed by secondary-ion mass spectrometry (SIMS). A thorough evaluation of the magnetic properties as a function of temperature and applied magnetic field has been performed by means of SQUID magnetometry and low-energy muon spin relaxation (µSR) spectroscopy, which enables studying local (on the nanometer scale) magnetic properties of the layers. The results testify that the ferromagnetic order builds up almost homogeneously below the Curie temperature in the full volume fraction of both the (Ga,Mn)As and (Ga,Mn)(Bi,As) layers. Incorporation of a small amount of heavy Bi atoms into (Ga,Mn)As, which distinctly enhances the strength of spin-orbit coupling in the quaternary (Ga,Mn)(Bi,As) layers, does not deteriorate noticeably their magnetic properties.

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.

Distribution of glass transition temperatures Tg in polystyrene thin films as revealed by low-energy muon spin relaxation: A comparison with neutron reflectivity results.

In a previous paper [Phys. Rev. E 83, 021801 (2011)] we performed neutron reflectivity (NR) measurements on a five-layer polystyrene (PS) thin film consisting of alternatively stacked deuterated polystyrene (dPS) and hydrogenated polystyrene (hPS) layers (dPS/hPS/dPS/hPS/dPS, ∼100 nm thick) on a Si substrate to reveal the distribution of Tg along the depth direction. Information on the Tg distribution is very useful to understand the interesting but unusual properties of polymer thin films. However, one problem that we have to clarify is if there are effects of deuterium labeling on Tg or not. To tackle the problem we performed low-energy muon spin relaxation (μSR) measurements on the above-mentioned deuterium-labeled five-layer PS thin film as well as dPS and hPS single-layer thin films ∼100 nm thick as a function of muon implantation energy. It was found that the deuterium labeling had no significant effects on the Tg distribution, guaranteeing that we can safely discuss the unusual thin film properties based on the Tg distribution revealed by NR on the deuterium-labeled thin films. In addition, the μSR result suggested that the higher Tg near the Si substrate is due to the strong orientation of phenyl rings.

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.

Depth-dependent Spin Dynamics in TbMnO3 Thin Films Measured by Low Energy Muon Spin Relaxation

Abstract We report on low energy muon measurements performed on 100 nm and 28 nm thin epitaxial, highly strained and twin free TbMnO3 films grown on (110) YAlO3 substrates by pulsed laser deposition (λ = 248 nm, ν = 2 Hz, T S = 760°C). These investigations were done at the LEM beamline at the PSI, Switzerland which allowed for depthdependent analysis of the muon spin relaxation rate as a function of temperature. A clear decrease of the relaxation rates could be observed in regions near the substrate/thin film interface compared to measurements at the surface or in the middle of the films. This behavior could be attributed to a straininduced change of the Tb spin dynamics. Furthermore, it could be shown that the films are fully magnetic below a temperature of 40 – 50 K, which agrees well with susceptibility measurements performed on these films as well as with the bulk literature value of TN,Mn = 41 K.

Zero-field Spin Depolarization of Low-Energy Muons in Ferromagnetic Nickel and Silver Metal

We present zero-field muon-spin depolarization measurements in nickel and silver performed using low-energy muon-spin relaxation technique.Ni or Ag are usually used in this depth-resolved technique as a backing material to enable background subtraction when studying small crystals or materials with weak magnetism. The depolarization rate of the asymmetry in silver and that of the slow relaxing part of the asymmetry in nickel are small(≤ 0.05 μ s −1 ), and weakly temperature and energy-dependent.

Magnetic polarons in Eu-based films of magnetic semiconductors

Various films of magnetic semiconductors EuO, EuS, EuSe, and EuTe have been studied by low-energy muon spin relaxation $(\text{LE-}\ensuremath{\mu}\text{SR})$ as well as by magnetization measurement techniques. $\text{LE-}\ensuremath{\mu}\text{SR}$ allows measurements of the distribution of magnetic field on the subnanometer scale unaccessible to traditional macroscopic techniques. A bound state of an electron around a positive muon---a magnetic polaron---is formed in the paramagnetic phase of Eu-based films up to room temperature. The local environment around the muon in the magnetic polaron is shown to be ferromagnetic.

Interaction between the magnetic and superconducting order parameters in aLa1.94Sr0.06CuO4wire studied via muon spin rotation

We investigate the coupling between the magnetic and superconducting order parameters in an 8 m long meander line ("wire") made of a La1.94Sr0.06CuO4 film with a cross section of 0.5 x 100 um^2. The magnetic order parameter is determined using the Low-Energy muon spin relaxation technique. The superconducting order parameter is characterized by transport measurements and modified by high current density. We find that, when the superconducting order parameter is suppressed by the current, the magnetic transition temperature, Tm, increases. The extracted sign and magnitude of the Ginzburg-Landau coupling constant indicate that the two orders are repulsive, and that our system is located close to the border between first and second order phase transition.