Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators

Meng Wu, Zhenglu Li, Ting Cao and Steven G. Louie ()
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Meng Wu: University of California at Berkeley
Zhenglu Li: University of California at Berkeley
Ting Cao: University of California at Berkeley
Steven G. Louie: University of California at Berkeley

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract The recent discovery of magnetism in atomically thin layers of van der Waals crystals has created great opportunities for exploring light–matter interactions and magneto-optical phenomena in the two-dimensional limit. Optical and magneto-optical experiments have provided insights into these topics, revealing strong magnetic circular dichroism and giant Kerr signals in atomically thin ferromagnetic insulators. However, the nature of the giant magneto-optical responses and their microscopic mechanism remain unclear. Here, by performing first-principles GW and Bethe-Salpeter equation calculations, we show that excitonic effects dominate the optical and magneto-optical responses in the prototypical two-dimensional ferromagnetic insulator, CrI3. We simulate the Kerr and Faraday effects in realistic experimental setups, and based on which we predict the sensitive frequency- and substrate-dependence of magneto-optical responses. These findings provide physical understanding of the phenomena as well as potential design principles for engineering magneto-optical and optoelectronic devices using two-dimensional magnets.

Date: 2019
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DOI: 10.1038/s41467-019-10325-7

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