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We employ synchrotron-based near-field infrared spectroscopy to reveal the vibrational properties of bulk, few-sheet, and single-sheet members of the MPS3 (M=Mn, Fe, Ni) family of materials and compare our findings with complementary lattice dynamics calculations. MnPS3 and the Fe analog are similar in terms of their symmetry crossovers, from C2/m to P3¯1m, as the monolayer is approached. These states differ as to the presence of a C3 rotation around the metal center. On the other hand, NiPS3 does not show a symmetry crossover, and the lack of a Bu symmetry mode near 450 cm-1 suggests that C3 rotational symmetry is already present, even in the bulk material. We discuss these findings in terms of local symmetry and temperature effects as well as the curious relationship between these symmetry transformations and those that take place under pressure.

The electronic structure of the chiral helimagnet Cr1/3NbS2 has been studied with core level and angle-resolved photoemission spectroscopy (ARPES). Intercalated Cr atoms are found to be effective in donating electrons to the NbS2 layers but also cause significant modifications of the electronic structure of the host NbS2 material. In particular, the data provide evidence that a description of the electronic structure of Cr1/3NbS2 on the basis of a simple rigid band picture is untenable. The data also reveal substantial inconsistencies with the predictions of standard density functional theory. The relevance of these results to the attainment of a correct description of the electronic structure of chiral helimagnets, magnetic thin films/multilayers, and transition metal dichalcogenides intercalated with 3d magnetic elements is discussed.