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Register a new userAnother dimension: investigations of molecular magnetism using muon-spin relaxation
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We review examples of muon-spin relaxation measurements on molecule-based magnetic coordination polymers, classified by their magnetic dimensionality. These include the one-dimensional s=1/2 spin chain Cu(pyz)(NO3)2 and the two-dimensional s=1/2 layered material [Cu(HF2)(pyz)2]BF4. We also describe some of the more exotic ground states that may become accessible in the future given the ability to tune the interaction strengths of our materials through crystal engineering.
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We present the results of muon-spin spectroscopy ($mu^{+}$SR) measurements on the molecular spin ladder system (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$, [Hpip=(C$_{5}$H$_{12}$N)]. Using transverse field $mu^{+}$SR we are able to identify characteristic behaviour in each of the regions of the phase diagram of the $x=0$ strong-rung spin ladder system (Hpip)$_{2}$CuBr$_4$. Comparison of our results to those of the dimer-based molecular magnet Cu(pyz)(gly)(ClO$_{4}$) shows several common features. We locate the crossovers in partially disordered (Hpip)$_{2}$CuBr$_{4(1-x)}$Cl$_{4x}$ ($x=0.05$), where a region of behaviour intermediate between quantum disordered and Luttinger liquid-like is identified. Our interpretation of the results incorporates an analysis of the probable muon stopping states in (Hpip)$_{2}$CuBr$_4$ based on density functional calculations and suggests how the muon plus its local distortion can lead to a local probe unit with good sensitivity to the magnetic state. Using longitudinal field $mu^{+}$SR we compare the dynamic response of the $x=1$ strong-rung material (Hpip)$_{2}$CuCl$_{4}$ to that of the strong-leg material (C$_{7}$H$_{10}$N)$_{2}$CuBr$_{4}$ (known as DIMPY) and demonstrate that our results are in agreement with predictions based on interacting fermionic quasiparticle excitations in these materials.
The magnetic and quadrupolar ordered states of polycrystalline YbRu2Ge2 have been investigated using zero-field muon spin relaxation ({mu}SR) and neutron diffraction measurements. Specific heat measurements show three successive phase transitions, with decreasing temperature from a paramagnetic to a quadrupolar state at T0 ~ 10 K, from the quadrupolar to a magnetic state at T1 ~ 6.5 K and a possible change in the magnetic ground state at T2 ~ 5.5 K. Clear evidence for the magnetic transition below 7 K (spectrum at 8 K reveals paramagnetic state) and a likely change in the magnetic structure near 5.8 K is observed in the zero-field {mu}SR measurements. The {mu}SR data, however, do not reveal any signature of magnetic order in the temperature range 8 - 45 K. This result is further supported by neutron diffraction measurements, where clear magnetic Bragg peaks have been observed below 8 K, but not above it. Below 8 K, the magnetic Bragg peaks can be characterized by an incommensurate antiferromagnetic ordering with the propagation vector q = [0.352, 0, 0] and the magnetic moment 2.9(3) {mu}B of Yb along the b-axis. These results are discussed in terms of quadrupolar ordered and magnetically ordered states.
Nd2Hf2O7, belonging to the family of geometrically frustrated cubic rare earth pyrochlore oxides, was recently identified to order antiferromagnetically below T_N = 0.55 K with an all-in/all-out arrangement of Nd3+ moments, however with a much reduced ordered state moment. Herein we investigate the spin dynamics and crystal field states of Nd2Hf2O7 using muon spin relaxation (muSR) and inelastic neutron scattering (INS) measurements. Our muSR study confirms the long range magnetic ordering and shows evidence for coexisting persistent dynamic spin fluctuations deep inside the ordered state down to 42 mK. The INS data show the crytal electric field (CEF) excitations due to the transitions both within the ground state multiplet and to the first excited state multiplet. The INS data are analyzed by a model based on CEF and crystal field states are determined. Strong Ising-type anisotropy is inferred from the ground state wavefunction. The CEF parameters indicate the CEF-split Kramers doublet ground state of Nd3+ to be consistent with the dipolar-octupolar character.
We present longitudinal field muon spin relaxation ($mu$SR) measurements in the unilluminated state of the photo-sensitive molecular magnetic Co-Fe Prussian blue analogues M$_{1-2x}$Co$_{1+x}$[Fe(CN)$_6$]$cdot z$ H$_2$O, where M=K and Rb with $x=0.4$ and $simeq 0.17$, respectively. These results are compared to those obtained in the $x=0.5$ stoichiometric limit, Co$_{1.5}$[Fe(CN)$_6$]$cdot 6$ H$_2$O, which is not photo-sensitive. We find evidence for correlation between the range of magnetic ordering and the value of $x$ in the unilluminated state which can be explained using a site percolation model.
We present the results of muon-spin relaxation (muSR) measurements on the hexagonal manganite HoMnO3. Features in the temperature-dependent relaxation rate, lambda, correlate with the magnetic transitions at 76 K, 38 K and 34 K. The highest temperature transition, associated with the ordering of Mn3+ moments has the largest effect on lambda. The application of a static electric field of E=10^4 Vm^-1 below T=50 K causes a small reduction in lambda which is suggestive of coupling between ferroelectric and magnetic domain walls in the ordered state of the material.
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