Quasiparticle Energies and Excitonic Effects of Chromium Trichloride: from Two Dimensions to Bulk

Abstract

Layered van der Waals (vdW) magnetic materials have attracted significant research interest to date. In this work, we employ the first-principles many-body perturbation theory to calculate excited-state properties of a prototype vdW magnet, chromium trichloride (CrCl3), covering monolayer, bilayer, and bulk structures. Unlike usual non-magnetic vdW semiconductors, in which many-electron interactions and excited states are sensitive to dimensionality, many-electron interactions are always enhanced and dominate quasiparticle energies and optical responses of both two-dimensional and bulk CrCl3. The electron-hole (e-h) binding energy can reach 3 eV in monolayer and remains as high as 2 eV in bulk. Because of the cancellation effect between self-energy corrections and e-h binding energies, the lowest-energy exciton (optical gap) is almost not affected by the change of dimensionality. Besides, for the excitons with similar e-h binding energies, their dipole oscillator strength can differ by a few orders of magnitude.Our analysis shows that such a big difference is from a unique interference effect between complex exciton wavefunctions and interband transitions. Finally, we find that the interlayer stacking sequence and magnetic coupling barely change quasiparticle band gaps and optical absorption spectra of CrCl3. Our calculated low-energy exciton peak positions agree with available measurements. These findings give insight into the understanding of many-electron interactions and the interplay between magnetic orders and optical excitations in vdW magnetic materials.

arXiv comment22 pages, 8 figures, and 2 tables

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Cited by in corpus (6)

• Optical and magneto-optical properties of ferromagnetic monolayer CrBr${}_3$: A first-principles $GW$ and $GW$ plus Bethe-Salpeter equation study
• Anisotropic Electron-Hole Excitation and Large Linear Dichroism in Two-Dimensional Ferromagnet CrSBr with In-Plane Magnetization
• Ab initio self-trapped excitons
• Mechanism of carrier doping induced magnetic phase transitions in two-dimensional materials
• Enhanced Magnetization by Defect-Assisted Exciton Recombination in Atomically Thin CrCl${}_3$
• Ligand Field Exciton Annihilation in Bulk CrCl3