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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 laye red 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.
We report the results of muon-spin relaxation measurements on the low-dimensional antiferromagnet Rb4Cu(MoO4)3. No long-range magnetic order is observed down to 50 mK implying a ratio T_N/J<0.005 (where J is the principal exchange strength along the spin chains) and an effective ratio of interchain to intrachain exchange of |J_perp/J|<2 x 10^-3, making the material an excellent realization of a one-dimensional quantum Heisenberg antiferromagnet. We probe the persistent spin excitations at low temperatures and find that ballistic spin transport dominates the excitations detected below 0.3 K.
A muon-spin relaxation (muSR) investigation is presented for the molecular superconductor kappa-(BEDT-TTF)2Cu[N(CN)2Br]. Evidence is found for low-temperature phase-separation, with only a fraction of the sample showing a superconducting signal, even for slow cooling. Rapid cooling reduces the superconducting fraction still further. For the superconducting phase, the in-plane penetration depth is measured to be lambda_{parallel} = 0.47(1) mu m and evidence is seen for a vortex decoupling transition in applied fields above 40 mT. The magnetic fluctuations in the normal state produce Korringa behavior of the muon spin relaxation rate below 100 K, a precipitous drop in relaxation rate is seen at higher temperatures and an enhanced local spin susceptibility occurs just above T_c.
We address the cause of the unusual muon spin relaxation (muSR) results on molecular nanomagnets (MNMs). Through measurements on protonated and deuterated samples of the MNMs Cr7Mn (S=1) and Cr8 (S=0), we show that the muon spin for $S eq 0$ MNMs is relaxed via dynamic fluctuations of the electronic spins. A freezing out of dynamic processes occurs on cooling and at low temperatures the muon spins are relaxed by the electronic spins which themselves are dephased by incoherent nuclear field fluctuations.We observe a transition to a state of static magnetic order of the MNM electronic spins in Cr7Mn below 2 K.
We report heat capacity measurements of the pnictide materials SmFeAsO$_{1-x}$F$_x$, NdFeAsO, LaFeAsO$_{1-x}$F$_x$ and LiFeAs. For SmFeAsO$_{1-x}$F$_x$, with x close to 0.1, we use 3 He measurements to demonstrate a transfer of entropy from the peak at TN to a previously unidentified ~2 K feature which grows with increasing doping. Our results on the Sm samples are compared with a similarly doped La sample to elucidate the crystal field levels of the Sm3+ ion at 0, 23, and 56 meV which lead to a Schottky-like anomaly, and also show that there is a significant increase in the Sommerfeld coefficient $gamma$ when La is replaced by Sm or Nd. The lattice contribution to the heat capacity of the superconducting oxypnictides is found to vary negligibly with chemical substitution. We also present a heat capacity measurement of LiFeAs showing the feature at Tc, which is significantly rounded and much smaller than the BCS value.
Transverse-field muon-spin rotation measurements performed on two samples of LiFeAs demonstrate that the superfluid stiffness of the superconducting condensate in relation to its superconducting transition temperature is enhanced compared to other pn ictide superconductors. Evidence is seen for a field-induced magnetic state in a sample with a significantly suppressed superconducting transition temperature. The results in this system highlight the role of direct Fe-Fe interactions in frustrating pairing mediated by antiferromagnetic fluctuations and suggest that, in common with other pnictide superconductors, the system is close to a magnetic instability.
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