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Magnetic transitions in the spin S=5/2 frustrated magnet BiMn2PO6 and strong lattice softening in BiMn2PO6 and BiZn2PO6 below 200 K

The crystallographic, magnetic and thermal properties of BiMn2PO6 and BiZn2PO6 were investigated by x-ray diffraction, magnetic susceptibility χ, heat capacity Cp, and 31P NMR measurements as well as by density-functional band-theory calculations. Both compounds show a strong monotonic lattice softening on cooling, where the Debye temperature decreases by a factor of two from Θ_D=650K at T=300K to Θ_D=300K at T=2K. The χ(T) data for BiMn2PO6 above 150K follow a Curie-Weiss law with a Curie constant consistent with a S=5/2 with g=2 and an antiferromagnetic (AFM) Weiss temperature θ_CW= -78K. The χdata indicate long-range AFM ordering below TN=30K, confirmed by a sharp lambda-type peak in Cp(T) at 28.8K. The band-theory calculations indicate that BiMn2PO6 is an AFM compound with dominant interactions J1/kB= 6.7K and J3/kB= 5.6K along the legs and rungs of a two-leg spin-ladder, respectively. In addition to the long-range AFM ordering at TN=30K, a second transition at 10 K is observed from the χand NMR measurements but is not evident in the Cp data. The Cp data at low T suggest a significant contribution from AFM spin waves moving in three dimensions and the absence of a spin-wave gap. A detailed analysis of the NMR spectra indicates commensurate magnetic order between 10K and 30K and a possible incommensurate modulation and/or spin canting below 10K. The commensurate order is consistent with microscopic simulations that yield a collinear Neel-type AFM spin arrangement both within and between the ladders, despite the presence of multiple weak interactions frustrating this magnetic structure. Frustration for AFM ordering and 1D spatial anisotropy of the 3D spin interactions are manifested in the frustration ratio f=|θCW|/TN=2.6, indicating a suppression of TN from 68K in the absence of these effects to 30K in BiMn2PO6.