Unraveling the Origin of Circularly Polarized Luminescence by First-Principles Calculations

• • First-principles calculations enable prediction of g_lum values with accuracy sufficient to guide molecular design, as demonstrated by achieving g_lum as high as -0.56 in chiral cylindrical molecules through intramolecular short-range charge transfer (Ref. 64). • • The theoretical limit of absorption dissymmetry factor (g_abs) is 2, and chiral cylindrical molecules have approached this limit (Ref. 62), indicating the potential for achieving similarly high g_lum values in optimized systems. • • TD-DFT benchmarks (Ref. 54) provide validated computational protocols for predicting chiroptical properties, ensuring reliability in screening CPL-active materials. • • Integration of machine learning with first-principles calculations is emerging as a powerful strategy to accelerate the discovery of high-performance CPL materials, addressing the bottleneck of computational cost in exploring vast chemical space.