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Register a new userProbing magnetic order and disorder in the one-dimensional molecular spin chains CuF2(pyz) and [Ln(hfac)3(boaDTDA)]n (Ln=Sm, La) using implanted muons
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We present the results of muon-spin relaxation ($mu^{+}$SR) measurements on antiferromagnetic and ferromagnetic spin chains. In antiferromagnetic CuF$_{2}$(pyz) we identify a transition to long range magnetic order taking place at $T_{mathrm{N}} = 0.6(1)$ K, allowing us to estimate a ratio with the intrachain exchange of $T_{mathrm{N}}/|J| approx 0.1$ and the ratio of interchain to intrachain exchange coupling as $|J/J| approx 0.05$. The ferromagnetic chain [Sm(hfac)$_{3}$(boaDTDA)]$_{n}$ undergoes an ordering transition at $T_{mathrm{c}}=2.8(1)$ K, seen via a broad freezing of dynamic fluctuations on the muon (microsecond) timescale and implying $T_{mathrm{c}}/|J| approx 0.6$. The ordered radical moment continues to fluctuate on this timescale down to 0.3 K, while the Sm moments remain disordered. In contrast, the radical spins in [La(hfac)$_{3}$(boaDTDA)]$_{n}$ remain magnetically disordered down to $T=0.1$ K suggesting $T_{mathrm{c}}/|J| < 0.17$.
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We present the results of muon-spin relaxation measurements of spin excitations in the one-dimensional quantum Heisenberg antiferromagnet Cu(pyz)(NO$_{3}$)$_{2}$. Using density-functional theory we propose muon sites and assess the degree of perturbation the muon probe causes on the system. We identify a site involving the muon forming a hydroxyl-type bond with an oxygen on the nitrate group that is sensitive to the characteristic spin dynamics of the system. Our measurements of the spin dynamics show that in the temperature range $T_{mathrm{N}}<T<J$ (between the ordering temperature $T_{mathrm{N}}$ and the exchange energy scale $J$) the field-dependent muon spin relaxation is characteristic of diffusive transport of spin excitations over a wide range of applied fields. We also identify a possible crossover at higher applied fields in the muon probes response to the fluctuation spectrum, to a regime where the muon detects early-time transport with a ballistic character. This behavior is contrasted with that found for $T>J$ and that in the related two-dimensional system Cu(pyz)$_2$(ClO$_4$)$_{2}$.
Neutron powder diffraction (NPD) study of textit{Ln}MnSbO (textit{Ln }$=$ La or Ce) reveals differences between the magnetic ground state of the two compounds due to the strong Ce-Mn coupling compared to La-Mn. The two compounds adopt the textit{P4/nmm} space group down to 2 K and whereas magnetization measurements do not show obvious anomaly at high temperatures, NPD reveals a C-type antiferromagnetic (AFM) order below $T_{mathrm{N}} = 255 $ K for LaMnSbO and 240 K for CeMnSbO. While the magnetic structure of LaMnSbO is preserved to base temperature, a sharp transition at $T_{mathrm{SR}} = 4.5 $K is observed in CeMnSbO due to a spin-reorientation (SR) transition of the Mn$^{mathrm{2+}}$ magnetic moments from pointing along the $c$-axis to the textit{ab}-plane. The SR transition in CeMnSbO is accompanied by a simultaneous long-range AFM ordering of the Ce moments which indicates that the Mn SR transition is driven by the Ce-Mn coupling. The ordered moments are found to be somewhat smaller than those expected for Mn$^{mathrm{2+}}$ ($S = 5/2$) in insulators, but large enough to suggest that these compounds belong to the class of local-moment antiferromagnets. The lower $T_{mathrm{Nthinspace }}$ found in these two compounds compared to the As-based counterparts ($T_{mathrm{N}} = 317$ for LaMnAsO, $T_{mathrm{N}} = 347$ K for CeMnAsO) indicates that the Mn-$Pn$ ($Pn=$ As or Sb) hybridization that mediates the superexchange Mn-$Pn$-Mn coupling is weaker for the Sb-based compounds.
The magnetic phase diagram has been mapped out via the measurements of electronic resistivity, magnetization and specific heat in the cobalt-based layered LnCo1-xFexAsO (Ln=La, Sm) compounds. The ferromagnetic (FM) transition at 63 K for LaCoAsO is rapidly suppressed upon Fe doping, and ultimately disappears around x=0.3 in the LaCo1-xFexAsO system. When La is replaced by magnetic rare earth element Sm, the 3d electrons first undergo a FM transition at Tc = 75 K, followed by an antiferromagnetic (AFM) transition at a lower temperature TN1 = 45 K. With partial Fe doping on the Co site, both FM (Tc) and AFM (TN1) transition temperatures are significantly suppressed, and finally approach zero kelvin at x = 0.3 and 0.2, respectively. Meanwhile, a third magnetic transition at TN2 = 5.6 K for SmCoAsO, associated with the AFM order of the Sm3+ 4f-oments, is uncovered and TN2 is found to be almost robust against the small Fe-doping. These results suggest that the 4f electrons of Sm3+ have an important effect on the magnetic behavior of 3d electrons in the 1111 type Co-based LnCo1-xFexAsO systems. In contrast, the magnetism of the f-electrons is relatively unaffected by the variation of the 3d electrons. The rich magnetic phase diagram in the Co-rich side of the LnCo1-xFexAsO system, therefore, is established.
We prepared the samples K$_{1-x}$Ln$_{x}$Fe$_2$As$_2$ (Ln=Sm, Nd and La) with ThCr$_2$Si$_2$-type structure. These samples were characterized by X-ray diffraction, resistivity, susceptibility and thermoelectric power (TEP). Substitution of Ln (Ln=La, Nd and Sm) for K in K$_{1-x}$Ln$_{x}$Fe$_2$As$_2$ system raises the superconducting transition temperature to 34-36 K. The TEP measurements indicate that the TEP of K$_{1-x}$Ln$_{x}$Fe$_2$As$_2$ is positive, being similar to the case of the Ba$_{1-x}$K$_{x}$Fe$_2$As$_2$ system with p-type carrier. In the K$_{1-x}$Ln$_{x}$Fe$_2$As$_2$ system, the superconducting $KFe_2As_2$ with $T_csim 3$ K is the parent compound, and no structural and spin-density wave instabilities exist in this system.
We investigate the effect of external pressure on magnetic order in undoped LnFeAsO (Ln = La, Ce, Pr, La) by using muon-spin relaxation measurements and ab-initio calculations. Both magnetic transition temperature $T_m$ and Fe magnetic moment decrease with external pressure. The effect is observed to be lanthanide dependent with the strongest response for Ln = La and the weakest for Ln = Sm. The trend is qualitatively in agreement with our DFT calculations. The same calculations allow us to assign a value of 0.68(2) $mu_B$ to the Fe moment, obtained from an accurate determination of the muon sites. Our data further show that the magnetic lanthanide order transitions do not follow the simple trend of Fe, possibly as a consequence of the different $f$-electron overlap.
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