Group Theory Analysis of Phonons in Monolayer Chromium Trihalides and Their Janus Structures

TL;DR

This paper uses group theory to analyze phonons in monolayer chromium trihalides and their Janus structures, predicting their vibrational properties and potential observable effects like spin-phonon coupling and chirality.

Contribution

It provides a comprehensive symmetry classification and phonon eigenfunctions for Janus chromium trihalide monolayers, clarifying Raman activity discrepancies and predicting novel magneto-optical effects.

Findings

Raman and infrared spectra are distinct for X3-Cr2-X3 but coincident for Janus Y3-Cr2-X3.

Symmetry-matched phonon eigenfunctions reveal phonon chirality and magnetism origins.

Predicted observable effects include spin-phonon coupling and magneto-optical phenomena in Janus monolayers.

Abstract

A contrastive investigation of the symmetry aspects of phonons in monolayer chromium trihalides and their Janus structures Y$_3$-Cr$_2$-X$_3$ (X, Y = F, Cl, Br, I) by group theory is presented. We first classify all phonons at the Brillouin-zone center ($\Gamma$) into the irreducible representation. Then the infrared and Raman activity of optic phonons, Raman tensors, and the possible polarization assignments of R active phonons are predicted. Base on these results, we clarify the the discrepancy about the Raman activity o optic modes in monolayer CrI$_3$. Besides, we find that the Raman and infrared spectra for X$_3$-Cr$_2$-X$_3$ are exclusive, whereas that for Janus Y$_3$-Cr$_2$-X$_3$ are coincident. This distinction is vital for optic spectra identification of Janus Y$_3$-Cr$_2$-X$_3$ monolayer from X$_3$-Cr$_2$-X$_3$ monolayer. In addition, we derive the symmetry-matched phonon eigenfunctions and corresponding schematic representations of the eigenvectors for both F$_3$-Cr$_2$-I$_3$ and I$_3$-Cr$_2$-I$_3$ monolayer, which demonstrate intuitively the origin of phonon chirality and magnetism. At last, our analysis indicates that the spin-phonon coupling, the magneto-optical effect of infrared and Raman active phonons, and phonon chirality should be observed in Janus Y$_3$-Cr$_2$-X$_3$ monolayer as that and even easier than that in X$_3$-Cr$_2$-X$_3$ monolayer. Our work provides a detailed guiding map for experimental characterization of Y$_3$-Cr$_2$-X$_3$ monolayer, and also reveals important effects of optic phonons in Janus Y$_3$-Cr$_2$-X$_3$ monolayer.