Inverse Engineering of Optical Constants in Photochromic Micron-Scale Hybrid Films

Abstract

Photochromic materials enable dynamic optical modulation through reversible transitions between distinct absorption states, with broad potential for smart windows, adaptive optics, and reconfigurable photonic devices. Micron-scale photochromic hybrid films present a particularly attractive platform for these applications, combining straightforward preparation with substantial optical modulation and scalability for high-volume fabrication. However, rational design of such films remains fundamentally constrained by the absence of well-defined optical constants. Unlike homogeneous thin films, micron-scale hybrid photochromic materials comprise active particles dispersed non-uniformly within polymer matrices. Conventional first-principles electromagnetic simulations face substantial computational costs and discrepancies between simulated and experimental particle distributions. Here, we introduce a data-driven framework that extracts effective optical constants directly from minimal experimental transmittance measurements. Our dual-state effective model approximates the complex inhomogeneous photochromic layer as a compressed homogeneous medium characterized by pseudo-refractive indices and pseudo-extinction coefficients for both pristine and UV-irradiated states. Through systematic optimization against experimental data from tungsten oxide-polyvinylpyrrolidone hybrid films, we determine wavelength-dependent pseudo-optical constants and compression ratios that enable accurate prediction of optical modulation within the tested thickness range. Our methodology establishes a framework for engineering hybrid photochromic systems and demonstrates how data-driven modeling can overcome limitations in characterizing complex nanostructured materials.