Mechanistic Modeling of Absorber-Driven Optical Darkening and Long-Timescale Feedback-Mediated Structural Evolution
Rashad Hall, To Dang, Daniel B. Erenso, Horace T. CrogmanLocalized optical absorption by nanoscale inclusions can profoundly alter energy deposition in optical traps, giving rise to nonlinear and long-timescale dynamics. Recent experiments have reported the formation of expanding optically darkened regions and episodic plasma-like emission during pulsed near-infrared optical trapping of magnetic beads interacting with biological cells. Here, we develop a reduced-order mechanistic model to investigate whether absorber-driven optical–thermal feedback associated with Fe3O4 inclusions is sufficient to reproduce the observed pre-plasma darkening dynamics. The model is constructed progressively from first-principles electromagnetic absorption and pulse-scale thermal diffusion to nonlinear feedback mediated by an evolving optically modified region. Single-pulse and multi-pulse simulations demonstrate that isolated iron-oxide absorbers cool too rapidly to sustain long-timescale thermal accumulation through linear heating alone. However, incorporation of a bubble-mediated optical feedback channel produces bounded growth, partial optical darkening, and slow relaxation dynamics consistent with experimentally observed minute-scale evolution. Electromagnetic absorption was computed using full core–shell Mie theory, yielding absorption cross-sections sufficient to support strong localized optical attenuation under experimentally relevant trapping conditions. The resulting reduced-order feedback framework reproduces stable growth–relaxation cycles, finite transmission plateaus, and self-limited optical darkening without requiring runaway heating or catastrophic cavitation. To evaluate the model quantitatively, simulated transmission dynamics were compared against experimentally measured normalized transmission traces digitized from previously reported optical trapping experiments. The fitted model reproduced the observed finite transmission plateau and slow post-activation relaxation with good agreement (R2≈0.86, RMSE ≈1.3×10−2). These results support the interpretation that experimentally observed optical darkening arises from a feedback-regulated optical–thermal process involving slowly evolving structural modification of the trapping region rather than cumulative thermal storage within isolated absorbers. The present framework provides a quantitatively constrained reduced-order description of feedback-mediated optical darkening under pulsed optical trapping conditions and establishes iron-oxide absorption as a physically plausible ignition mechanism for dark-state formation in the pre-plasma regime.