Studies of a Large Odd‐Numbered Odd‐Electron Metal Ring: Inelastic Neutron Scattering and Muon Spin Relaxation Spectroscopy of Cr8Mn

The spin dynamics of Cr₈Mn, a nine‐membered antiferromagnetic (AF) molecular nanomagnet, are investigated. Cr₈Mn is a rare example of a large odd‐membered AF ring, and has an odd‐number of 3d‐electrons present. Odd‐membered AF rings are unusual and of interest due to the presence of competing exchange interactions that result in frustrated‐spin ground states. The chemical synthesis and structures of two Cr₈Mn variants that differ only in their crystal packing are reported. Evidence of spin frustration is investigated by inelastic neutron scattering (INS) and muon spin relaxation spectroscopy (μSR). From INS studies we accurately determine an appropriate microscopic spin Hamiltonian and we show that μSR is sensitive to the ground‐spin‐state crossing from S=1/2 to S=3/2 in Cr₈Mn. The estimated width of the muon asymmetry resonance is consistent with the presence of an avoided crossing. The investigation of the internal spin structure of the ground state, through the analysis of spin‐pair correlations and scalar‐spin chirality, shows a non‐collinear spin structure that fluctuates between non‐planar states of opposite chiralities.     

Characterization of the crystal and magnetic structures of the mixed-anion coordination polymer Cu(HCO2)(NO3)(pyz) {pyz = Pyrazine} by X-ray diffraction, ac magnetic susceptibility, dc magnetization, muon-spin relaxation, and spin dimer analysis

The mixed-anion coordination polymer Cu(HCO2)(NO3)(pyz) was synthesized, its crystal structure was determined by X-ray diffraction, and its magnetic structure was characterized by ac susceptibility, dc magnetization, muon-spin relaxation, and spin dimer analysis. The crystal structure consists of five-coordinate Cu2+ ions that are connected through syn-anti bridging mu-HCO2- and mu-pyz ligands to form a highly corrugated two-dimensional layered network. Bulk magnetic measurements show a broad maximum in chi(T) at 6.6 K. The HCO2- and pyz ligands mediate ferromagnetic and antiferromagnetic spin exchange interactions between adjacent Cu2+ ions with the spin exchange parameters J/kB = 8.17 and -5.4 K, respectively (H = -JSigmaSi x Sj). The muon-spin relaxation data show a transition to a long-range magnetic ordering below TN = 3.66(3) K. For T < TN, the M(H) and chi'ac measurements provide evidence for a field-induced spin-flop transition at 15.2 kOe. That Cu(HCO2)(NO3)(pyz) undergoes a long-range magnetic ordering is an unexpected result because the one-dimensional Cu(NO3)2(pyz) and three-dimensional Cu(HCO2)2(pyz) compounds display linear chain antiferromagnetism with no long-range magnetic ordering down to 2 K.     

Muon-fluorine entangled states in molecular magnets

The information accessible from a muon-spin relaxation experiment can be limited due to a lack of knowledge of the precise muon stopping site. We demonstrate here the possibility of localizing a spin polarized muon in a known stopping state in a molecular material containing fluorine. The muon-spin precession that results from the entangled nature of the muon spin and surrounding nuclear spins is sensitive to the nature of the stopping site. We use this property to identify three classes of sites that occur in molecular magnets and describe the extent to which the muon distorts its surroundings.     

Persistence to high temperatures of interlayer coherence in an organic superconductor

The interlayer magnetoresistance rho(zz) of the organic metal kappa-(BEDT-TTF)(2)Cu(NCS)(2) is studied in fields of up to 45 T and at temperatures T from 0.5 to 30 K. The peak in rho(zz) seen in in-plane fields, a definitive signature of interlayer coherence, remains to Ts exceeding the Anderson criterion for incoherent transport by a factor approximately 30. Angle-dependent magnetoresistance oscillations are modeled using an approach based on field-induced quasiparticle paths on a 3D Fermi surface, to yield the T dependence of the scattering rate tau(-1). The results suggest that tau(-1) does not vary strongly over the Fermi surface, and that it has a T(2) dependence due to electron-electron scattering.     

Coexistence of magnetic fluctuations and superconductivity in the pnictide high temperature superconductor SmFeAsO1-xFx measured by muon spin rotation

Muon spin rotation experiments were performed on the pnictide high temperature superconductor SmFeAsO1-xFx with x=0.18 and 0.3. We observed an unusual enhancement of slow spin fluctuations in the vicinity of the superconducting transition which suggests that the spin fluctuations contribute to the formation of an unconventional superconducting state. An estimate of the in-plane penetration depth lambda ab(0)=190(5) nm was obtained, which confirms that the pnictide superconductors obey an Uemura-style relationship between Tc and lambda ab(0);(-2).