We combine single-crystal neutron diffraction studies and Monte Carlo simulations to determine the spin structures and finite-temperature phase diagram of the spin-5/2 triangular-lattice antiferromagnet NaBaMn(PO) in magnetic field. With the application of a magnetic field in two different directions, namely along the -axis and in the -plane of the trigonal symmetry, we track the evolution of the spin structure through changes of the magnetic propagation vector. We account for these results with a minimal Heisenberg Hamiltonian that includes easy-axis anisotropy and weak, frustrated interlayer couplings in addition to intralayer exchange. Guided by representation analysis, we refine symmetry-allowed modes to the measured intensities and obtain the spin structures for all field-induced phases, which we compare quantitatively with simulated configurations. Taken together, our measurements and simulations show that frustrated interlayer exchange – rather than purely 2D physics – organizes the unexpectedly rich field-induced phases of NaBaMn(PO).

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