Accelerating discovery of infrared nonlinear optical materials with large shift current via high-throughput screening

Discovering nonlinear optical (NLO) materials with strong shift current response, particularly in the infrared (IR) regime, is essential for next-generation optoelectronics yet remains highly challenging in both experiments and theory, which still largely relies on case-by-case studies. Here, we employ a high-throughput screening strategy, applying a multi-step filter to the Materials Project database (>154,000 materials), which yielded 2519 candidate materials for detailed first-principles evaluation. From these calculations, we identify 32 NLO materials with strong shift current response ( σ > 100 μA/V 2 ). Our work reveals that layered structures with C 3 v symmetry and heavy p -block elements (e.g., Te and Sb) exhibit apparent superiority in enhancing shift current. More importantly, 9 of these compounds show shift current response peaks in the IR region, with the strongest reaching 616 μA/V 2 , holding significant application potential in fields such as IR photodetection, sensing, and energy harvesting. Beyond identifying promising candidates, this work establishes a comprehensive and high-quality first-principles dataset for NLO response, providing a solid foundation for future AI-driven screening and accelerated discovery of high-performance NLO materials, as demonstrated by a prototype machine-learning application.