Anisotropic phonon properties in SiP2 monolayer: A first-principles study

Abstract

Recently, the micromechanical exfoliation method has effectively separated the two-dimensional (2D) SiP2 flake, which exhibits superior performance in field-effect transistors and photodetectors. In this paper, first-principles calculations were utilized to investigate the phononic properties of a SiP2 monolayer, which would be significant to explain the thermal deformation of 2D SiP2-based devices. We found that the acoustic phonon branches of SiP2 monolayer demonstrate significant in-plane anisotropy. The anisotropic ratios for the group velocities are 2.41 and 1.66 for the longitudinal and transverse acoustic modes, respectively. Meanwhile, the anisotropic ratio of the negative thermal expansion coefficient only considering the contribution from acoustic phonons is 0.14, while this ratio is ∼0.279 occurs at 120 K when both acoustic and optical phonons are taken into account. For the Raman-active optical phonons, the largest Grüneisen constant of these Raman-active phonons reaches 22.76, while the largest anisotropic ratio of phonon frequency is up to 2.16. To interpret this significant in-plane anisotropy, we calculated the electron density distribution, crystal orbital Hamilton populations (COHP) and interatomic force constants (IFCs), and found the maximal IFC in the x-direction is 5.79 times greater than y-direction, suggesting it as a major origin of the phononic anisotropy.