Abstract
Author(s): Neal, SN; Kim, HS; O'Neal, KR; Haglund, AV; Smith, KA; Mandrus, DG; Bechtel, HA; Carr, GL; Haule, K; Vanderbilt, D; Musfeldt, JL | Abstract: 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.
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