Long-range magnetic ordering in Li2MnGeO4 and precursor short-range spin correlations
Long-range magnetic ordering and short-range spin correlations in layered noncentrosymmetric orthogermanate Li2MnGeO4 were studied by means of polarized and unpolarized neutron scattering. The combined Rietveld refinement of synchrotron and neutron powder diffraction data at room temperature within the Pmn21 space group allowed us to specify the details of the crystal structure. According to the additional Bragg peaks in low-temperature neutron diffraction patterns a long-range antiferromagnetic ordering with the propagation vector k=(1/21/21/2) has been found below TN≈8K. Symmetry analysis revealed the model of the ground state spin structure within the Cac (no. 9.41) magnetic space group. It is represented by the noncollinear ordering of manganese atoms with a refined magnetic moment of 4.9μB/Mn2+ at 1.7 K, which corresponds to the saturated value for the high-spin configuration S=5/2. Diffuse magnetic scattering was detected on the neutron diffraction patterns at temperatures just above TN. Its temperature evolution was investigated in detail by polarized neutron scattering with the following XYZ-polarization analysis. Reverse Monte Carlo simulation of diffuse scattering data showed the development of short-range ordering in Li2MnGeO4, which is symmetry consistent on a small scale with the long-range magnetic state below TN. The reconstructed radial spin-pair correlation function S(0)S(r) displayed the predominant role of antiferromagnetic correlations. It was found that spin correlations are significant only for the nearest magnetic neighbors and almost disappear at r≈12Å at 10 K. Temperature dependence of the diffuse scattering implies short-range ordering long before the magnetic phase transition. Besides, the spin arrangement was found to be similar in both cases above and below TN. As a result, an exhaustive picture of the gradual formation of magnetic ordering in Li2MnGeO4 is presented.