Exotic Magnetic Field-Induced Spin-Superstructures in a Mixed Honeycomb-Triangular Lattice System

Abstract

The temperature-magnetic field phase diagram of the mixed honeycomb-triangular lattice system K2Mn3(VO4)2CO3 is investigated by means of magnetization, heat-capacity, and neutron-scattering measurements. The results indicate that triangular and honeycomb magnetic layers undergo sequential magnetic orderings and act as nearly independent magnetic sublattices. The honeycomb sublattice orders at about 85 K in a Neél-type antiferromagnetic structure, while the triangular sublattice displays two consecutive ordered states at much lower temperatures, 3 and 2.2 K. The ground state of the triangular sublattice consists of a planar "Y" magnetic structure that emerges from an intermediate collinear "up-up-down" state. Applied magnetic fields parallel or perpendicular to the c axis induce exotic ordered phases characterized by various spin-stacking sequences of triangular layers that yield bilayer, three-layer, or four-layer magnetic superstructures. The observed superstructures cannot be explained in the framework of quasiclassical theory based only on nearest-neighbor interlayer coupling and point towards the presence of effective second-nearest-neighbor interactions mediated by fluctuations of the magnetic moments in the honeycomb sublattice.