Accurate density functional theory prediction of low-dimensional yttrium nitride: From 2D hexagonal and square monolayers to 1D zizag single walled nanotubes

Abstract

Through this contribution, we aim to highlight the structural stability of low dimensional YN structures ranging from the 3D bulk to the 2D square and hexagonal monolayers and their corresponding 1D zigzag single walled nanotubes. For all arrangements, geometry optimization is achieved at the DFT/B3LYP level of theory using a Gaussian basis set. Then, the coupled perturbed Kohn-Sham and Hartree-Fock (CPKS/HF) computational approach is used to simulate Raman and IR spectrum. Rolling, cohesive and relaxation energies, electronic and vibrational contributions to the polarizability and equilibrium lattice parameters are also reported. Insights into their structural stability are provided by combining optimized parameters and vibrational phonon spectra. For the optimized 3D bulks, 2D monolayers and 1D square nanotubes, no imaginary frequency has been recorded in their vibrational spectra which reveals a dynamic stability. Likewise, imaginary frequencies appeared only for relatively large YN (n,0) single walled hexagonal nanotubes (n > 6) indicating that the optimized structures are not a real global minimum and implying a dynamic instability. A scaning mode procedure along the largest imaginary vibrational mode has been adopted to obtain the equilibrium geometry of (22,0) YN hexagonal nanotube. Therefore, it must be emphasized that the obtained potential energy surface presents two minima between a saddle point. These minima corresponds to a stable structures slightly distorted compared to the initial one. The absence of imaginary phonon frequencies in the Raman and IR spectra of the optimized (22,0) YN hexagonal nanotube confirms its structural stability.

Keywords: DFT; Dynamic stability; Imaginary phonon mode; Monolayer; Nanotubes.