Generative Screening of Multi‐Resonance Molecules for Narrowband Pure Violet OLEDs

Abstract Narrowband emission from organic light‐emitting diodes (OLEDs) is essential for a wide color gamut in displays. Herein, a pioneering small‐data‐driven computational workflow is developed that, for the first time, applies bond order difference (ΔBO) screening to the rational design of narrowband‐emitting multi‐resonance (MR) molecules. This strategy enables the efficient generation and high‐throughput screening of 10 000 candidates. The ΔBO descriptor, calculated with an efficient GFN2‐xTB/simplified time‐dependent density functional theory (sTD‐DFT) protocol, provides a ≈490‐fold acceleration over conventional methods and shows a moderate correlation (R ² = 0.59) with experimental full‐width at half‐maximum (FWHM). Analysis reveals that hybridization of short‐ and long‐range charge transfer (SRCT/LRCT) states is key to their sharp, efficient emission. This workflow guides the synthesis and testing of two promising MR emitters, v‐tDIDCzCz and u‐tDIDCzCz. Critically, in OLED devices, they deliver narrow FWHMs of 13 and 15 nm at ≈400 nm emission, representing the narrowest reported for pure violet bottom‐emitters. A pure violet emission is achieved, with Commission Internationale de l'Éclairage (CIE) y‐coordinates of 0.022 and 0.018, significantly surpassing the BT.2020 standard (0.046). This scalable computational workflow provides a powerful strategy to overcome broad emission limitations, paving the way for next‐generation OLED materials in advanced displays and optoelectronics.