Tuning the antiferromagnetic helical pitch length and nanoscale domain size in Fe3PO4 O3 by magnetic dilution

The insulating magnetic material Fe3PO4O3 features a noncentrosymmetric lattice composed of Fe3+ triangular units. Frustration, due to competing near-neighbor (J1) and next-nearest-neighbor (J2) antiferromagnetic interactions, was recently suggested to be the origin of an antiferromagnetic helical ground state with unusual needlelike nanoscale magnetic domains in Fe3PO4O3. Magnetic dilution is shown here to tune the ratio of these magnetic interactions, thus providing deeper insight into this unconventional antiferromagnet. Dilution of the Fe3+ lattice in Fe3PO4O3 was accomplished by substituting nonmagnetic Ga3+ to form the solid solution series Fe3-xGaxPO4O3 with x=0.012, 0.06, 0.25, 0.5, 1.0, 1.5. Magnetic susceptibility and neutron powder diffraction data from this series are presented. A continuous decrease of both the helical pitch length and the domain size is observed with increasing dilution up to at least x=0.25, while for x≥0.5, the compounds lack long-range magnetic order entirely. The decrease in the helical pitch length with increasing x can be qualitatively understood by reduction of the ratio of J2/J1 in the Heisenberg model, consistent with mean-field considerations. Intriguingly, the magnetic correlation length in the ab plane remains nearly equal to the pitch length for each value of x≤0.25, showing that the two quantities are intrinsically connected in this unusual antiferromagnet.