Transferable excited-state dynamics enable screening of fluorescent protein chromophores

TL;DR

This paper introduces X-MACE, a machine-learning framework for efficient excited-state dynamics simulations, enabling rapid screening and design of fluorescent protein chromophores with diverse structures.

Contribution

The authors develop a transferable ML potential combined with curvature-driven surface hopping, allowing accurate, data-efficient excited-state simulations across various chromophore derivatives.

Findings

Structural modifications influence excited-state relaxation and lifetimes.

Steric crowding lowers torsional barriers, speeding up non-radiative decay.

Conjugation extension stabilizes planar states, enhancing fluorescence.

Abstract

Transferable excited-state dynamics offer a route to efficient screening of photophysical behavior across molecular systems, but conventional nonadiabatic simulations remain prohibitively expensive. Here we introduce X-MACE, a transferable machine-learning potential for excited-state dynamics that predicts multiple potential energy surfaces, forces and oscillator strengths, and combine it with curvature-driven surface hopping to enable data-efficient screening of photochemical pathways. We apply this framework to fluorescent chromophores as an example application, using green fluorescent protein chromophore variants to demonstrate how subtle structural modifications reshape excited-state relaxation, lifetimes and photoisomerization yields. Fine-tuning a single pretrained model with fewer than 100 reference geometries per derivative yields accurate dynamics across a chemically diverse set of analogues. The screening reveals two governing design principles: steric crowding on the phenolate ring lowers the torsional barrier and accelerates access to twisted conical intersections, whereas conjugation extension stabilizes planar excited-state configurations, suppresses non-radiative decay and prolongs fluorescence. More broadly, this workflow provides a general framework for scalable excited-state screening and interpretable design of photophysical properties.