Electronic and vibrational properties of V$_2$C-based MXenes: from experiments to first-principles modeling

TL;DR

This study combines experiments and first-principles calculations to analyze the electronic and vibrational properties of V$_2$C MXenes and their functionalized derivatives, providing insights into their stability, electronic behavior, and vibrational spectra.

Contribution

It offers the first computational prediction of vibrational spectra for V$_2$C MXenes and links these to experimental Raman data, enhancing characterization methods.

Findings

V$_2$C$ is metallic and stable.

Vibrational modes are predicted and linked to Raman peaks.

Terminal groups influence vibrational properties and Raman spectra.

Abstract

In the present work, the electronic and vibrational properties of both pristine V$_2$C and fully-terminated V$_2$CT$_2$ (where T = F, O, OH) 2D monolayers are investigated using density functional theory. Firstly, the atomic structures of V$_2$C-based MXene phases are optimized and their respective dynamical stabilities are discussed. Secondly, electronic band structures are computed indicating that V$_2$C is metallic as well as all the corresponding functionalized systems. Thirdly, the vibrational properties (phonon frequencies and spectra) of V$_2$C-based MXenes are computed thanks to density functional perturbation theory and reported for the first time. Both Raman (E$_g$, A$_{1g}$) and infrared active (E$_u$, A$_{2u}$) vibrational modes are predicted \textit{ab initio} with the aim to correlate the experimental Raman peaks with the calculated vibrational modes and to assign them with specific atomic motions. The effect of the terminal groups on the vibrational properties is emphasized as well as on the presence and position of the corresponding Raman peaks. Our results provide new insights for the identification and characterization of V$_2$C-based samples using Raman spectroscopy.