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Caption : figure s1. the total energy of the mos2/crocl heterojunction as a function of the kinetic energy cutoff for the planewave basis.

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Caption : figure s2. details for the dz and dthickness used in this study.

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Caption : figure s3. snapshot structure of mos2/crocl heterostructure after 8 ps of aimd simulations at 500k. the black rhombus represents the supercell used for aimd.

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Caption : figure s4. band structure of (a) mos2 monolayer and (b) crocl monolayer.

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Caption : figure s5. (a) top and side views of monolayer crocl. (b-e) top views of monolayer crocl with different antiferromagnetic configurations. only cr atoms are shown.

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Caption : figure s6. non-zero second-order non-linear coefficients of (a-b) crocl and (c-d) mos2/crocl as functions of photon energy with different u values.

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Caption : figure s7. shift photoconductivity versus photon energy of (a-b) crocl and (c-d) mos2/crocl with different u values.