G.J. MacDougall

Magnetic properties of the geometrically frustrated S= 1 2 antiferromagnets, La2 LiMoO6 and Ba2 YMoO 6, with the B-site ordered double perovskite structure: Evidence for a collective spin-singlet ground state

Two B-site ordered double perovskites, La2LiMoO6 and Ba2YMoO6, based on the S = 1/2 ion, Mo5+, have been investigated in the context of geometric magnetic frustration. Powder neutron diffraction, heat capacity, susceptibility, muon spin relaxation(_SR), and 89Y NMR- including MAS NMR- data have been collected. La2LiMoO6 deviates strongly from simple Curie-Weiss paramagnetic behavior below 150K and zero-field cooled/ field cooled (ZFC/FC)irreversibility occurs below 20K with a weak, broad susceptibility maximum near 5K in the ZFC data. A Curie-Weiss fit shows a reduced mu_eff=1.42\mu_B, (spin only = 1.73 muB) and a Weiss temperature, \theta_c, which depends strongly on the temperature range of the fit. Powder neutron diffraction, heat capacity and 7Li NMR show no evidence for long range magnetic order to 2K. On the other hand oscillations develop below 20K in muSR indicating at least short range magnetic correlations. Susceptibility data for Ba2YMoO6 also deviate strongly from the C-W law below 150K with a similarly reduced mu_eff = 1.72\mu_B and \theta_c = - 219(1)K. Heat capacity, neutron powder diffraction and muSR data show no evidence for long range order to 2K but a very broad maximum appears in the heat capacity. The 89Y NMR paramagnetic Knight shift shows a remarkable local spin susceptibility behavior below about 70K with two components from roughly equal sample volumes, one indicating a singlet state and the other a strongly fluctuating paramagnetic state. Further evidence for a singlet state comes from the behavior of the relaxation rate, 1/T1. These results are discussed and compared with those from other isostructural S = 1/2 materials and those based on S = 3/2 and S = 1.

New magnetic phase diagram of (Sr,Ca)2RuO4

High-T(c) cuprates, iron pnictides, organic BEDT and TMTSF, alkali-doped C(60), and heavy-fermion systems have superconducting states adjacent to competing states exhibiting static antiferromagnetic or spin density wave order. This feature has promoted pictures for their superconducting pairing mediated by spin fluctuations. Sr(2)RuO(4) is another unconventional superconductor which almost certainly has a p-wave pairing. The absence of known signatures of static magnetism in the Sr-rich side of the (Ca, Sr) substitution space, however, has led to a prevailing view that the superconducting state in Sr(2)RuO(4) emerges from a surrounding Fermi-liquid metallic state. Using muon spin relaxation and magnetic susceptibility measurements, we demonstrate here that (Sr,Ca)(2)RuO(4) has a ground state with static magnetic order over nearly the entire range of (Ca, Sr) substitution, with spin-glass behaviour in Sr(1.5)Ca(0.5)RuO(4) and Ca(1.5)Sr(0.5)RuO(4). The resulting new magnetic phase diagram establishes the proximity of superconductivity in Sr(2)RuO(4) to competing static magnetic order.

Itinerant spin excitations near the hidden order transition in URu2Si2

By means of neutron scattering we show that the high temperature precursor to the hidden order state of the heavy fermion superconductor URu(2)Si(2) exhibits heavily damped incommensurate paramagnons whose strong energy dispersion is very similar to that of the long-lived longitudinal f spin excitations that appear below T(0). This suggests that there is a strongly hybridized character to the itinerant excitations observed previously above the hidden order transition. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets; hence the hidden order phase probably originates from a Fermi surface instability. We identify wavevectors that span nested regions of a f-d hybridized band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase.

2D Kagomé ordering in the 3D frustrated spinel Li2Mn2O4

Muon spin relaxation (μSR) experiments on the geometrically frustrated spinel oxide, Li2Mn2O4, show the development of spin correlations over a range of lengthscales with decreasing temperature. Increased relaxation below ~150 K is consistent with the onset of spin correlations. Below 50 K, spin order, on a lengthscale which is long range for the μSR probe, appears abruptly in temperature, consistent with prior neutron diffraction results. The oscillations in the zero field asymmetry are analysed using a three frequency model. By locating the muon site, this is shown to be consistent with the unexpected 2D structure on the Kagome planes proposed originally from neutron data. Longitudinal field data demonstrate that some spin dynamics persist even at 2 K. Thus, a very complex magnetic ground state, featuring the coexistence of long lengthscale 2D ordering and significant spin dynamics, is proposed. This is unusual considering the 3D topology of the Mn3+ spins in this material.

Impurity-induced singlet breaking in SrCu2(BO3)2

We have performed muon spin relaxation

Study of the ground state properties of LiHo(x)Y(1-x)F4 using muon spin relaxation.

(\ensuremath{\mu}\mathrm{SR})

Study of the Ground State Properties ofLiHoxY1−xF4Using Muon Spin Relaxation

studies on single crystals of

Study of the ground state properties of

\mathrm{Sr}{\mathrm{Cu}}_{2}{(\mathrm{B}{\mathrm{O}}_{3})}_{2}

LiHo_xY_{1-x}F_4

, a quasi-two-dimensional spin system with a spin-singlet ground state. We find evidence for two different muon sites which we associate with muons located adjacent to the two inequivalent O sites. One site, presumably located in the Cu-O-Cu superexchange path, exhibits a large increase in the frequency shift with decreasing temperature which is unaffected by the onset of the singlet ground state, indicating that the muon has perturbed the Cu-Cu interaction and created two quasifree spins. We have also performed

using

\ensuremath{\mu}\mathrm{SR}