Optical responses of atomically thin 2D materials are greatly influenced by electron-hole interactions. It is by far established that exciton signatures can be well identified in the optical absorption spectrum of quasi-2D materials. However, the same level of understanding of excitonic effects on nonlinear optical responses and the ability to compute them accurately is still much desired. Based on the functional integral formalisms and working in the velocity gauge, we introduce a convenient Feynman diagram approach for calculating nonlinear responses including excitonic effects. By dressing electron-photon interactions with electron-hole ladder diagrams, we derive an expression for second-order optical responses and provide a comprehensive description of excitonic effects. We apply our approach to a monolayer h-BN model and show qualitative changes in the second harmonic generation spectrum when comparing with results assuming independent particles. Our approach can be readily extended to higher-order optical responses and is feasible for first-principles calculations.

• Received 6 November 2023
• Revised 20 March 2024
• Accepted 4 April 2024

DOI:https://doi.org/10.1103/PhysRevB.109.155437