Muons and magnets

Abstract:

We present the results of muon spin relaxation (μ+SR) studies on low dimensional molecular magnet systems. μ+SR measurements have been carried out on the Cu-based chain compounds CuX2(pyz) (where X = Br, Cl, NCS and pyz = pyrazine) as a function of temperature and applied longitudinal magnetic field. Oscillations in the time dependence of the muon polarization, characteristic of magnetic order at two distinct muon sites, are detected in both CuBr2(pyz) (below TN = 3.6(1) K) and CuCl2(pyz) (below TN = 3.2(2) K). No evidence of magnetic order is observed in Cu(NCS)2(pyz) down to 0.35 K. The results are discussed in terms of the estimated Cu-X-Cu and Cu-(pyz)-Cu exchange constants. The theory of μSR in high spin molecule (HSM) systems, which are effectively zero-dimensional magnets, is discussed and results are presented on [Ni 12(chp)12(O2CMe)12(H 2O)6(THF)6] (S = 12), [Mn9O 7(OAc)11(thme)(py)3(H2O) 2] (S = 17/2) and [Fe14(bta)6(O) 6(OMe)18 Cl6] (S ≥ 23). Measurements made in applied longitudinal magnetic fields on HSM materials at dilution refrigerator temperatures strongly suggest that dynamic local magnetic field fluctuations are responsible for the relaxation of the muon spin ensemble. Trends in temperature and field dependent behaviour in these systems, as probed by the muon, are discussed.

Abstract:

The temperature dependence of the crystal structure and electronic properties of brownmillerite-like Ca(2.5)Sr(0.5)GaMn(2)O(8) has been studied by neutron powder diffraction and muSR spectroscopy. The results show that short-range 2D magnetic order begins to develop within the perovskite-like bilayers of MnO(6) octahedra approximately 50 K above the 3D Néel temperature of approximately 150 K. The bilayers show a structural response to the onset of magnetism throughout this temperature range whereas the GaO(4) layers that separate the bilayers only respond below the 3D ordering temperature. XANES spectroscopy shows that the sample contains Mn(3+) and Mn(4+) cations in a 1:1 ratio, and the behavior in the region of the Néel transition is interpreted as a local charge ordering. Electron diffraction and high-resolution electron microscopy have been used to show that the local microstructure is more complex than the average structure revealed by neutron diffraction, and that microdomains exist in which the GaO(4) tetrahedra show different orientations. It is argued that the bonding requirements of diamagnetic gallium control the electronic behavior within the perovskite-like bilayers.

Abstract:

The temperature dependence of the crystal structure and electronic properties of brownmillerite-like Ca2.5Sr0.5GaMn 2O8 has been studied by neutron powder diffraction and μSR spectroscopy. The results show that short-range 2D magnetic order begins to develop within the perovskite-like bilayers of MnO6 octahedra approximately 50 K above the 3D Néel temperature of ∼150 K. The bilayers show a structural response to the onset of magnetism throughout this temperature range whereas the GaO4 layers that separate the bilayers only respond below the 3D ordering temperature. XANES spectroscopy shows that the sample contains Mn3+ and Mn4+ cations in a 1:1 ratio, and the behavior in the region of the Néel transition is interpreted as a local charge ordering. Electron diffraction and high-resolution electron microscopy have been used to show that the local microstructure is more complex than the average structure revealed by neutron diffraction, and that microdomains exist in which the GaO4 tetrahedra show different orientations. It is argued that the bonding requirements of diamagnetic gallium control the electronic behavior within the perovskite-like bilayers.