Nonreciprocal Second-Harmonic Generation in Few-Layer Chromium Triiodide

Abstract

It is of fundamental importance but challenging to simultaneously identify atomic and magnetic configurations of two-dimensional van der Waals materials. In this work, we show that the nonreciprocal second-harmonic generation (SHG) can be a powerful tool to answer this challenge. Despite the preserved lattice inversion symmetry, the interlayer antiferromagnetic order and spin-orbit coupling generate enhanced SHG in PT-symmetric bilayer chromium triiodide (CrI3). Importantly, the in-plane polarization-resolved SHG is sensitive to subtly different interlayer structures that cannot be told by linear optical spectra. Beyond bilayer, we further predict that the intensity and angle-resolved SHG can be employed to identify both interlayer atomic and magnetic configurations of trilayer CrI3. Our first-principles results agree with available measurements and show the potential of SHG as a non-contacting approach to explore correlations between interlayer structures and magnetic orders of emerging ultra-thin magnetic materials.

8 pages and 8 figures

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Cited by in corpus (7)

• Basic formulation and first-principles implementation of nonlinear magneto-optical effects
• Classification of second harmonic generation effect in magnetically ordered materials
• Giant and controllable nonlinear magneto-optical effects in two-dimensional magnets
• Quasiparticle Energies and Excitonic Effects of Chromium Trichloride: from Two Dimensions to Bulk
• Antiferromagnetism-induced second-order nonlinear optical responses of centrosymmetric bilayer CrI${}_3$
• Skin Effect of Nonlinear Optical Responses in Antiferromagnets
• Magnetism-induced second-order nonlinear optical responses in multiferroic BiFeO${}_3$