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The Commensurate-Incommensurate Charge-Density-Wave Transition and Phonon Zone Folding in 1T-TaSe2 Thin Films

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 Added by Alexander Balandin
 Publication date 2015
  fields Physics
and research's language is English




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Bulk 1T-TaSe2 exhibits unusually high charge density wave (CDW) transition temperatures of 600 K and 473 K below which the material exists in the incommensurate (I-CDW) and the commensurate (C-CDW) charge-density-wave phases, respectively. The 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 the Gamma point. 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 473K to 413K as the film thicknesses decrease from 150 nm 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. 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.



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When a crystal is subjected to a periodic potential, under certain circumstances (such as when the period of the potential is close to the crystal periodicity; the potential is strong enough, etc.) it might adjust itself to follow the periodicity of the potential, resulting in a, so called, commensurate state. Such commensurate-incommensurate transitions are ubiquitous phenomena in many areas of condensed matter physics: from magnetism and dislocations in crystals, to vortices in superconductors, and atomic layers adsorbed on a crystalline surface. Of particular interest might be the properties of topological defects between the two commensurate phases: solitons, domain walls, and dislocation walls. Here we report a commensurate-incommensurate transition for graphene on top of hexagonal boron nitride (hBN). Depending on the rotational angle between the two hexagonal lattices, graphene can either stretch to adjust to a slightly different hBN periodicity (the commensurate state found for small rotational angles) or exhibit little adjustment (the incommensurate state). In the commensurate state, areas with matching lattice constants are separated by domain walls that accumulate the resulting strain. Such soliton-like objects present significant fundamental interest, and their presence might explain recent observations when the electronic, optical, Raman and other properties of graphene-hBN heterostructures have been notably altered.
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In the sake of connecting the charge-density-wave (CDW) of TaSe$_2$ and single-emph{textbf{q}} CDW-type distortion of TaTe$_2$, we present an overall electronic phase diagram of 1emph{T}-TaSe$_{2-x}$Te$_x$ ($0 leq x leq 2$). In the experimentally prepared single crystals, the CDW is completely suppressed as $0.5 < x < 1.5$, while superconductivity emerges as $0.2 < x < 1.2$. Theoretically, similar to 1emph{T}-TaSe$_2$ and 1emph{T}-TaTe$_2$, the hypothetic 1emph{T}-TaSeTe with ordered Se/Ta/Te stacking shows instability in the phonon dispersion, indicating the presence of CDW in the ideally ordered sample. The contradictory between experimental and theoretical results suggests that the CDW is suppressed by disorder in 1emph{T}-TaSe$_{2-x}$Te$_x$. The formation and suppression of CDW are found to be independent with Fermi surface nesting based on the generated electron susceptibility calculations. The calculation of phonon linewidth suggests the strong textbf{emph{q}}-dependent electron-phonon coupling induced period-lattice-distortion (PLD) should be related to our observation: The doping can largely distort the TaX$_6$ (X = Se, Te) octahedra, which are disorderly distributed. The resulted puckered Ta-Ta layers are not compatible with the two-dimensional PLD. Therefore, CDW is suppressed in 1emph{T}-TaSe$_{2-x}$Te$_x$. Our results offer an indirect evidence that PLD, which can be influenced by strong disorder, is the origin of CDW in the system.
We study the coupled charge-lattice dynamics in the commensurate charge density wave (CDW) phase of the layered compound 1T-TaS$_{2}$ driven by an ultrashort laser pulse. For describing its electronic structure, we employ a tight-binding model of previous studies including the effects of lattice distortion associated with the CDW order. We further add on-site Coulomb interactions and reproduce an energy gap at the Fermi level within a mean-field analysis. On the basis of coupled equations of motion for electrons and the lattice distortion, we numerically study their dynamics driven by an ultrashort laser pulse. We find that the CDW order decreases and even disappears during the laser irradiation while the lattice distortion is almost frozen. We also find that the lattice motion sets in on a longer time scale and causes a further decrease in the CDW order even after the laser irradiation.
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