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Strong quantum zero-point motion (ZPM) of light nuclei and other particles is a crucial aspect of many state-of-the-art quantum materials. However, it has only recently begun to be explored from an ab initio perspective, through several competing approximations. Here we develop a unified description of muon and light nucleus ZPM and establish the regimes of anharmonicity and positional quantum entanglement where different approximation schemes apply. Via density functional theory and path-integral molecular dynamics simulations we demonstrate that in solid nitrogen, α–N2, muon ZPM is both strongly anharmonic and many-body in character, with the muon forming an extended electric-dipole polaron around a central, quantum-entangled [N2–μ–N2]+ complex. By combining this quantitative description of quantum muon ZPM with precision muon quadrupolar level-crossing resonance experiments, we independently determine the static 14N nuclear quadrupolar coupling constant of pristine α–N2 to be –5.36(2) MHz, a significant improvement in accuracy over the previously-accepted value of –5.39(5) MHz, and a validation of our unified description of light-particle ZPM. Quantum entanglement and uncertainty in the positions of light nuclei and implanted particles can crucially impact our understanding of advanced materials. This paper develops a unified theoretical description of these effects and applies it to muon spectroscopy measurements of a material constant to significantly improve their accuracy. [ABSTRACT FROM AUTHOR]

The synthesis, crystal structure, and electrical, optical, and magnetic properties of k-BETS2[Fe(super III)(C2O4)CI2] where BETS is bis(ethylenedithio)tetraselenafulvalene, are reported. It is an organic-inorganic hybrid that displays the coexistence of two-dimensional (2D) pi electrons, 1D antiferromagnetism, and possible canted antiferromagnetism involving pi and d spins.

The crystal structure and electronic properties of Ca2.5Sr0.5GaMn2O8 has been studied by neutron diffraction and muSR spectroscopy. The results show that short-range 2D magnetic order begins to develop within the perovskite-bilayers of MnO6 octahedra.

The charge transfer salts (BEDT-TTF)4AFe(C2O4)3.C6H5CN (BEDT-TTF = bis(ethylenedithio)tetrathiafulvalene) act as semiconductors when A is K or NH4, but as superconductors when A is H2O. In the semiconductor salts, the dimers of (BEDT-TTF)(sub 2)(super 2+) isolated by discrete (BEDT-TTF)0 form the BEDT-TTF layers. High spin 3d5 Fe(III) exists in both types of salts. The C6H5CN molecules in the hexagonal cavities stabilize the lattice structures of the salts.

The molecular cluster system [Fe19(metheidi)10(OH)14O6(H2O)12]NO3•24H2O, abbreviated as Fe19, contains nineteen Fe(III) ions arranged in a disc-like structure with the total spin S = 35/2. For the first order, it behaves magnetically as a single molecule magnet with a 16 K anisotropy barrier. The high spin value enhances weak intermolecular interactions for both dipolar and superexchange mechanisms and an eventual transition to antiferromagnetic order occurs at 1.2 K. We used neutron diffraction to determine both the mode of ordering and the easy spin axis. The observed ordering was not consistent with a purely dipolar driven order, indicating a significant contribution from intermolecular superexchange. The easy axis is close to the molecular Fe1--Fe10 axis. Inelastic neutron scattering was used to follow the magnetic order parameter and to measure the magnetic excitations. Direct transitions to at least three excited states were found in the 2 to 3 meV region. Measurements below 0.2 meV revealed two low energy excited states, which were assigned to S = 39/2 and S = 31/2 spin states with respective excitation gaps of 1.5 and 3 K. Exchange interactions operating over distances of order 10 Å were determined to be on the order of 5 mK and were eight-times stronger than the dipolar coupling. [ABSTRACT FROM AUTHOR]

The achiral organic radical dinitrophenyl nitronyl nitroxide crystallizes in two enantiomorphs, both being chiral tetragonal space groups that are mirror images of each other. Muon-spin rotation experiments have been performed to study the magnetic properties of these crystals and demonstrate that long-range magnetic order is established below a temperature of 1.10(1) K. Two oscillatory components are detected in the muon data, which show two different temperature dependences. [ABSTRACT FROM AUTHOR]

High-resolution X-ray and neutron diffraction measurements, magnetometry and muon-spin rotation spectroscopy are used for probing the response of the superconducting state and crystal structure of LiFeAs to chemical substituents on both the Li and the Fe sites. The superconductivity is very sensitive to composition, where Li-deficient materials have shown a very rapid suppression of the superconducting state.

In incommensurate structure of [Bi.sub.2][Mn.sub.4/3][Ni.sub.2/3][O.sub.6] is produced by the competition between ferroelectric Bi lone pair-driven A site displacement, chemical order of Mn and Ni on the B site, and both charge and orbital order at these transition metals. The interplay between the frustrated polar Bi displacements and the frustrated spin order at the B site has produced magnetodielectric coupling between the incommensurately modulated lattice and the spin-glass-like ground state with different relationship between the magnetocapacitance and the applied field.

The synthesis, and structural and magnetic characterization of three [Cu.sup.2+]-containing coordination polymers, [Cu(H[F.sub.2])[(pyrazine).sub.2]]Sb[F.sub.6], [[Cu.sub.2]F(HF)(H[F.sub.2])[(pyrazine).sub.4]][(Sb[F.sub.6]).sub.2], and [CuAg([H.sub.3][F.sub.4])[(pyrazine).sub.5]][(Sb[F.sub.6]).sub.2] are presented. The polymers are found to crystallize in either tetragonal or orthorhombic space groups, have structures consisting of 2D square layers of [[M[(pyz).sub.2]].sup.n+] that are linked in the third dimension by either H[F.sub.2.sup.-] or [H.sub.3][F.sub.4.sup.-] and the variations observed in magnetic behaviors are driven by differences in the H***F hydrogen-bonding motifs.

X-ray powder diffraction and magnetic susceptibility measurements have shown that Ag[(pyz).sub.2]([S.sub.2][O.sub.8]) has 2-dimensional square nets of [Ag.sup.2+] ions resulting from the corner-sharing of axially elongated Ag[N.sub.4][O.sub.2] octahedral and have displayed characteristic 2D antiferromagnetism. [[mu].sup.+]SR measurements have shown that Ag[(pyz)([S.sub.2][O.sub.8]) has undergone 3D magnetic ordering below 7.8(3) K.

The quasi-one-dimensional molecule-based Heisenberg antiferromagnet Cu(NO3)2(pyz)3 has an intrachain coupling J = 13.7(1) K (UGRAPHIC DISPLAY="INLINE" ID="UGT1" SRC="UGT1"/) and exhibits a state of long-range magnetic order below TN = 0.105(1) K. The ratio of interchain to intrachain coupling is estimated to be ☋J′/J☋ = 3.3 × 10−3, demonstrating a high degree of isolation for the Cu chains. [ABSTRACT FROM AUTHOR]

The title compounds are bimetallic MOFs containing [Cu(pyz)2]2+ square lattices linked by MF6n− octahedra. In each, only the Cu2+ spins exhibit long-range magnetic order below 3.5 K (M = V4+) and 2.6 K (M = Ga3+). The V4+ spins remain disordered down to 0.5 K. [ABSTRACT FROM AUTHOR]

The spin dynamics of Cr8Mn, a nine-membered antiferromagnetic (AF) molecular nanomagnet, are investigated. Cr8Mn is a rare example of a large odd-membered AF ring, and has an odd-number of 3d-electrons present. Odd-membered AF rings are unusual and of interest due to the presence of competing exchange interactions that result in frustrated-spin ground states. The chemical synthesis and structures of two Cr8Mn variants that differ only in their crystal packing are reported. Evidence of spin frustration is investigated by inelastic neutron scattering (INS) and muon spin relaxation spectroscopy (μSR). From INS studies we accurately determine an appropriate microscopic spin Hamiltonian and we show that μSR is sensitive to the ground-spin-state crossing from S=1/2 to S=3/2 in Cr8Mn. The estimated width of the muon asymmetry resonance is consistent with the presence of an avoided crossing. The investigation of the internal spin structure of the ground state, through the analysis of spin-pair correlations and scalar-spin chirality, shows a non-collinear spin structure that fluctuates between non-planar states of opposite chiralities. [ABSTRACT FROM AUTHOR]

Melanins are pigmentary macromolecules found throughout the biosphere that, in the 1970s, were discovered to conduct electricity and display bistable switching. Since then, it has been widely believed that melanins are naturally occurring amorphous organic semiconductors. Here, we report electrical conductivity, muon spin relaxation, and electron paramagnetic resonance measurements of melanin as the environmental humidity is varied. We show that hydration of melanin shifts the comproportionation equilibrium so as to dope electrons and protons into the system. This equilibrium defines the relative proportions of hydroxyquinone, semiquinone, and quinone species in the macromolecule. As such, the mechanism explains why melanin at neutral pH only conducts when "wet" and suggests that both carriers play a role in the conductivity. Understanding that melanin is an electronic-ionic hybrid conductor rather than an amorphous organic semiconductor opens exciting possibilities for bioelectronic applications such as ion-toelectron transduction given its biocompatibility. [ABSTRACT FROM AUTHOR]

Muon-spin rotation and relaxation (μSR) experiments have been performed on a variety of novel organic and molecular magnetic systems. In these experiments, implanted muons are used to study the magnitude, distribution and dynamics of the local field at the muon site. Calculations of the spatial dependence of the dipole-field inside the unit cell are used to interpret the data and determine the muon site in certain cases. We describe and review muon experiments on nitronyl nitroxide organic ferromagnets and antiferromagnets. We discuss a muon study of the spin crossover phenomenon which has been studied in Fe(PM-PEA)2(NCS)2, and which shows Gaussian and root-exponential muon relaxation in the high-spin and low-spin phases, respectively. The effects of high temperature annealing on TDAE-C60 have also been studied with μSR. Experiments on a disc-shaped molecular complex containing Fe19 (with spin 31/2) reveal the effects of fluctuations of magnetization and allow an estimate of the fluctuation rate. These experiments demonstrate the wide range of problems which can be tackled using the μSR technique. [Copyright &y& Elsevier]