From Static Spectra to Operando Infrared Dynamics: Physics Informed Flow Modeling and a Benchmark

Abstract

The Solid Electrolyte Interphase (SEI) is critical to the performance of lithium-ion batteries, yet its analysis via Operando Infrared (IR) spectroscopy remains experimentally complex and expensive, which limits its accessibility for standard research facilities. To overcome this bottleneck, we formulate a novel task, Operando IR Prediction, which aims to forecast the time-resolved evolution of spectral ``fingerprints'' from a single static spectrum. To facilitate this, we introduce OpIRSpec-7K, the first large-scale operando dataset comprising 7,118 high-quality samples across 10 distinct battery systems, alongside OpIRBench, a comprehensive evaluation benchmark with carefully designed protocols. Addressing the limitations of standard spectrum, video, and sequence models in capturing voltage-driven chemical dynamics and complex composition, we propose Aligned Bi-stream Chemical Constraint (ABCC), an end-to-end physics-aware framework. It reformulates MeanFlow and introduces a novel Chemical Flow to explicitly model reaction trajectories, employs a two-stream disentanglement mechanism for solvent-SEI separation, and enforces physics and spectrum constraints such as mass conservation and peak shifts. ABCC significantly outperforms state-of-the-art static, sequential, and generative baselines. ABCC even generalizes to unseen systems and enables interpretable downstream recovery of SEI formation pathways, supporting AI-driven electrochemical discovery.