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We present an experimental investigation of the magnetic ground state in Ba$_4$NbIr$_3$O$_{12}$, a fractional valent trimer iridate. X-ray absorption and photoemission spectroscopy show that the Ir valence lies between 3+ and 4+ while Nb is pentavalent. Combined dc/ac magnetization, specific heat, and muon spin rotation/relaxation ($\mu$SR) measurements reveal no magnetic phase transition down to 0.05~K. Despite a significant Weiss temperature ($\Theta_{\mathrm{W}} \sim -15$ to $-25$~K) indicating antiferromagnetic correlations, a quantum spin-liquid (QSL) phase emerges and persists down to 0.1~K. This state likely arises from geometric frustration in the edge-sharing equilateral triangle Ir network. Our $\mu$SR analysis reveals a two-component depolarization, arising from the coexistence of rapidly (90\%) and slowly (10\%) fluctuating Ir moments. Powder x-ray diffraction and Ir-L$_3$edge x-ray absorption fine structure spectroscopy identify ~8-10\% Nb/Ir site-exchange, reducing frustration within part of the Ir network, and likely leading to the faster muon spin relaxation, while the structurally ordered Ir ions remain highly geometrically frustrated, giving rise to the rapidly spin-fluctuating QSL ground state. At low temperatures, the magnetic specific heat varies as $\gamma T + \alpha T^2$, indicating gapless spinon excitations, and possible Dirac QSL features with linear spinon dispersion, respectively., Comment: 27 pages, 15 figures

Spin-orbit coupling (SOC) offers a large variety of novel and extraordinary magnetic and electronic properties in otherwise `ordinary pool' of heavy ion oxides. Here we present a detailed study on an apparently isolated hexagonal 2$H$ spin-chain $d^4$ iridate Sr$_3$LiIrO$_6$ (SLIO) with geometric frustration. Our structural studies clearly reveal perfect Li-Ir chemical order in this compound. Our combined experimental and {\it ab-initio} electronic structure investigations establish a magnetic ground state with finite Ir$^{5+}$ magnetic moments in this compound, contrary to the anticipated nonmagnetic $J$=0 state. Furthermore, the dc magnetic susceptibility ($\chi$), heat capacity ($C_p$) and spin-polarized density functional theory (DFT) studies unravel that despite having noticeable antiferromagnetic correlation among the Ir$^{5+}$ local moments, this SLIO system evades any kind of magnetic ordering down to at least 2 K due to geometrical frustration, arising from the comparable interchain Ir-O-O-Ir superexchange interaction strengths, hence promoting SLIO as a potential quantum spin liquid candidate., Comment: 13 pages, 5 figures. arXiv admin note: text overlap with arXiv:2107.04431

Spin-orbit coupling (SOC) often gives rise to interesting electronic and magnetic phases in an otherwise ordinary pool of paramagnetic heavy metal oxides. In presence of strong SOC, assumed to be working in $j$-$j$ coupling regime, 5$d^4$ iridates are generally speculated to possess a nonmagnetic $J_{eff}$~=~0 singlet ground state, which invariably gets masked due to different solid-state effects (e.g. hopping). Here, we try to probe the trueness of the atomic SOC-based proposal in an apparently 1-dimensional system, Sr$_3$NaIrO$_6$, possessing a 2$H$ hexagonal structure with well separated Ir$^{5+}$ (5$d^4$) ions. But all the detailed experimental as well as theoretical characterizations reveal that the ground state of Sr$_3$NaIrO$_6$ is not nonmagnetic, rather accommodating a significantly high effective magnetic moment on Ir$^{5+}$ ion. However our combined dc susceptibility ($\chi$), ${}^{23}$Na nuclear magnetic resonance (NMR), muon-spin-relaxation/rotation ($\mu$SR) and heat capacity ($C_p$) measurements clearly refute any sign of spin-freezing or ordered magnetism among the Ir$^{5+}$ moments due to geometrical exchange frustration, while in-depth zero-field (ZF) and longitudinal field (LF) $\mu$SR investigations strongly point towards inhomogeneous quantum spin-orbital liquid (QSOL)-like ground state. In addition, the linear temperature dependence of both the NMR spin-lattice relaxation rate and the magnetic heat capacity at low temperatures suggest low-lying gapless spin excitations in the QSOL phase of this material. Finally, we conclude that the effective SOC realised in $d^4$ iridates are unlikely to offer a ground state which will be consistent with a purely atomic $j$-$j$ coupling description., Comment: 13 pages, 12 figures

Spin-orbit coupling (SOC) plays a crucial role in magnetic and electronic properties of 5$d$ iridates. In this paper we have experimentally investigated the structural and physical properties of a series of Ir-based double perovskite compounds Pr$_{2-x}$Sr$_x$MgIrO$_6$ ($x$ = 0, 0.5, 1; hereafter abbreviated as PMIO, PSMIO1505, and PSMIO). Interestingly, these compounds have recently been proposed to undergo a transition from the spin-orbit-coupled Mott insulating phase at $x$ = 0 to the elusive half-metallic antiferromagnetic (HMAFM) state with Sr doping at $x$ = 1. However, our detailed magnetic and electrical measurements refute any kind of HMAFM possibility in either of the doped samples. In addition, we establish that within these Pr$_{2-x}$Sr$_x$MgIrO$_6$ double perovskites, changes in Ir-oxidation states (4+ for PMIO to 5+ for PSMIO via mixed 4+/5+ for PSMIO1505) lead to markedly different magnetic behaviors. While SOC on Ir is at the root of the observed insulating behaviors for all three samples, the correlated magnetic properties of these three compounds develop entirely due to the contribution from local Ir moments. Additionally, the magnetic Pr$^{3+}$ (4$f^2$) ions, instead of showing any kind of ordering, only contribute to the total paramagnetic moment. It is seen that the PrSrMgIrO$_6$ sample does not order down to 2 K despite antiferromagnetic interactions. But, the $d^5$ iridate Pr$_2$MgIrO$_6$ shows a sharp antiferromagnetic (AFM) transition at around 14 K, and in the mixed valent Pr$_{1.5}$Sr$_{0.5}$MgIrO$_6$ sample the AFM transition is shifted to a much lower temperature ($\sim$ 6 K) due to weakening of the AFM exchange., Comment: 3 tables, and 8 figures

While it was speculated that 5$d^4$ systems would possess non-magnetic $J$~=~0 ground state due to strong Spin-Orbit Coupling (SOC), all such systems have invariably shown presence of magnetic moments so far. A puzzling case is that of Ba$_2$YIrO$_6$, which in spite of having a perfectly cubic structure with largely separated Ir$^{5+}$ ($d^4$) ions, has consistently shown presence of weak magnetic moments. Moreover, we clearly show from Muon Spin Relaxation ($\mu$SR) measurements that a change in the magnetic environment of the implanted muons in Ba$_2$YIrO$_6$ occurs as temperature is lowered below 10~K. This observation becomes counterintuitive, as the estimated value of SOC obtained by fitting the RIXS spectrum of Ba$_2$YIrO$_6$ with an atomic $j-j$ model is found to be as high as 0.39~eV, meaning that the system within this model is neither expected to possess moments nor exhibit temperature dependent magnetic response. Therefore we argue that the atomic $j-j$ coupling description is not sufficient to explain the ground state of such systems, where despite having strong SOC, presence of hopping triggers delocalisation of holes, resulting in spontaneous generation of magnetic moments. Our theoretical calculations further indicate that these moments favour formation of spin-orbital singlets in the case of Ba$_2$YIrO$_6$, which is manifested in $\mu$SR experiments measured down to 60~mK., Comment: 20 Pages, 7 Figures

We have studied the temperature induced $0 -\pi $ thermodynamic transition in Nb/PdNi/Nb Superconductor/Ferromagnetic/Superconductor (SFS) heterostructures by microwave measurements of the superfluid density. We have observed a shift in the transition temperature with the ageing of the heterostructures, suggesting that structural and/or chemical changes took place. Motivated by the electrodynamics findings, we have extensively studied the local structural properties of the samples by means of X-ray Absorption Spectroscopy (XAS) technique, and the compositional profile by Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS). We found that the samples have indeed changed their properties, in particular for what concerns the interfaces and the composition of the ferromagnetic alloy layer. The structural and compositional data are consistent with the shift of the $0-\pi$ transition toward the behaviour of heterostructures with different F layers. An important emerging indication to the physics of SFS is the weak relevance of the ideality of the interfaces: even in aged samples, with less-than-ideal interfaces, the temperature-induced $0-\pi$ transition is still detectable albeit at a different critical F thickness., Comment: 11 pages, 9 figures, accepted for publication on Phys. Rev. B, http://journals.aps.org/prb/

The superconducting and structural properties of S/F/S (Superconductor/Ferromagnet/Superconductor) heterostructures have been studied by means of microwave measurements (1-20 GHz) and x-ray absorption fine structure (XAFS) spectroscopy. Nb/PdNi/Nb trilayers have been studied as a function of F layer thicness. With respect to pure Nb, XAFS analysis shows that the heterostructures exhibit larger structural disorder in the S layers. Microwave measurements show evidence for a progressively weaker vortex pinning with increasing F thickness. However, no clear correlation is found with the local disorder in Nb: the weakest pinning is not in the most disordered trilayer. Therefore the structural disorder in the superconducting material cannot explain on its own the changes in vortex pinning. We argue that the F layer acts on the superconducting state itself. We propose possible explanations for the observed behavior., Comment: Submitted to J. Supercond. and Novel Magnetism

We combine wideband (1-20 GHz) Corbino disk and dielectric resonator (8.2 GHz) techniques to study the microwave properties in Nb/PdNi/Nb trilayers, grown by UHV dc magnetron sputtering, composed by Nb layers of nominal thickness $d_S$=15 nm, and a ferromagnetic PdNi layer of thickness $d_F$= 1, 2, 8 and 9 nm. We focus on the vortex state. Magnetic fields up to $H_{c2}$ were applied. The microwave resistivity at fixed $H/H_{c2}$ increases with $d_F$, eventually exceeding the Bardeen Stephen flux flow value., Comment: 6 pages. Submitted to Journal of Superconductivity and Novel Magnetism

Several doped 6H hexagonal ruthenates, having the general formula Ba3MRu2O9, have been studied over a significant period of time in order to understand the unusual magnetism of ruthenium metal. However, among them, the M=Fe compound appears different since it is observed that unlike others, the 3d Fe ions and 4d Ru ions can easily exchange their crystallographic positions and as a result many possible magnetic interactions become realizable. The present study involving several experimental methods on this compound establish that the magnetic structure of Ba3FeRu2O9 is indeed very different from all other 6H ruthenates. Local structural study reveals that the possible Fe/Ru-site disorder further extends to create local chemical inhomogeneity, affecting the high temperature magnetism of this material. There is a gradual decrease of 57Fe M\"ossbauer spectral intensity with decreasing temperature (below 100 K), which reveals that there is a large spread in the magnetic ordering temperatures, corresponding to many spatially inhomogeneous regions. However, finally at about 25 K, the whole compound is found to take up a global glass-like magnetic ordering., Comment: 24 page, 7 figures

We performed near-edge x-ray absorption spectroscopy (XANES) at V K edge in the antiferromagnetic insulating (AFI) phase of a 2.8% Cr-doped V_2O_3 single crystal. Linear dichroism of several percent is measured in the hexagonal plane and found to be in good agreement with ab-initio calculations based on multiple scattering theory. This experiment definitively proves the structural origin of the signal and therefore solves a controversy raised by previous interpretations of the same dichroism as non-reciprocal. It also calls for a further investigation of the role of the magnetoelectric annealing procedure in cooling to the AFI phase., Comment: 4 pages 3 figures. To be published in Phys. Rev. B (2005)

The structure of La$_{1-x}$Ca$_{x}$MnO$_{3}$ solid solutions (x=0, 0.25, 0.50, 0.67, 1) under high pressure (up to 40-45 GPa) has been investigated by synchrotron X-ray powder diffraction (XRD) in order to characterize their volume \emph{vs.} pressure (P-V) equation of state. All the members of the solid solution, except the extreme compounds: LaMnO$_3$ and CaMnO$_{3}$, present low pressure orthorhombic P$nma$ phase evolving toward an high pressure tetragonal (I$4/mcm$) symmetry. The details of this transition are related to the Ca doping: on increasing the Ca content, the critical pressure of the transition decreases, but the energetic cost of the transition increases. This study depicts a peculiar evolution of structural distortions as a function of pressure and concentration., Comment: 12 pages, 8 eps figures