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Open Access Publications from the University of California

Near-field infrared spectroscopy of monolayer MnPS3

  • Author(s): Neal, SN;
  • Kim, HS;
  • Smith, KA;
  • Haglund, AV;
  • Mandrus, DG;
  • Bechtel, HA;
  • Carr, GL;
  • Haule, K;
  • Vanderbilt, D;
  • Musfeldt, JL
  • et al.

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We measured the near-field infrared response of MnPS3 in bulk, few-, and single-layer form and compared our findings with traditional far-field vibrational spectroscopies, a symmetry analysis, and first-principles lattice dynamics calculations. Trends in the Bu mode near 450cm-1 are striking, with the disappearance of this structure in the thinnest sheets. Combined with the amplified response of the activated Ag mode and analysis of the Au+Bu features, we find that symmetry is unexpectedly increased in few- and single-sheet MnPS3 due to a restoration of the threefold axes of rotation. Monoclinicity in this system is therefore a consequence of the long-range stacking pattern and temperature rather than local structure.

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