Zone-Folded Phonons and the Commensurate-Incommensurate Charge-Density-Wave Transition in 1T-TaSe2 Thin Films

Bulk 1T-TaSe2 exhibits unusually high charge density wave (CDW) transition temperatures of 600 and 473 K below which the material exists in the incommensurate (I-CDW) and the commensurate (C-CDW) charge-density-wave phases, respectively. The (13)(1/2) × (13)(1/2) C-CDW reconstruction of the lattice coincides with new Raman peaks resulting from zone-folding of phonon modes from middle regions of the original Brillouin zone back to Γ. The C-CDW transition temperatures as a function of film thickness are determined from the evolution of these new Raman peaks, and they are found to decrease from 473 to 413 K as the film thicknesses decrease from 150 to 35 nm. A comparison of the Raman data with ab initio calculations of both the normal and C-CDW phases gives a consistent picture of the zone-folding of the phonon modes following lattice reconstruction. The Raman peak at ∼154 cm(-1) originates from the zone-folded phonons in the C-CDW phase. In the I-CDW phase, the loss of translational symmetry coincides with a strong suppression and broadening of the Raman peaks. The observed change in the C-CDW transition temperature is consistent with total energy calculations of bulk and monolayer 1T-TaSe2.