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We report the feasibility of using magnetoentropic mapping for the rapididentification of magnetic cycloid and skyrmion phases in uniaxial systems,based on the GaV4S8 and GaV4Se8 model skyrmion hosts with easy-axis andeasy-plane anisotropies respectively. We show that these measurements can beinterpreted with the help of a simple numerical model for the spin Hamiltonianto yield unambiguous assignments for both single phase regions and phaseboundaries. In the two lacunar spinel chemistries, we obtain excellentagreement between the measured magnetoentropic features and a minimal spinHamiltonian built on Heisenberg exchange, single-ion anisotropy, andanisotropic Dzyaloshinskii-Moriya interactions. In particular, we identifycharacteristic high-entropy behavior in the cycloid phase that serves as aprecursor to the formation of skyrmions at elevated temperatures and is areadily-measurable signature of this phase transition. Our results demonstratethat rapid magnetoentropic mapping guided by numerical modeling is an effectivemeans of understanding the complex magnetic phase diagrams innate to skyrmionhosts. One notable exception is the observation of an anomalous,low-temperature high-entropy state in the easy-plane system GaV$_4$Se$_8$,which is not captured in the numerical model. Possible origins of this stateare discussed.

Magnetoentropic mapping and computational modeling of cycloids and skyrmions in the lacunar spinels GaV$_4$S$_8$ and GaV$_4$Se$_8$