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We show that excitonic resonances and interexciton transitions can enhance the probability of spontaneous parametric down-conversion, a second-order optical response that generates entangled photon pairs. We benchmark our ab initio many-body calculations using experimental polar plots of second harmonic generation in NbOI₂, clearly demonstrating the relevance of excitons in the nonlinear response. A strong double-exciton resonance in 2D NbOCl₂ leads to giant enhancement in the second order susceptibility. Our work paves the way for the realization of efficient ultrathin quantum light sources.
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Xuan et al. (2024) studied this question.
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