Differentiable hybrid force fields support scalable autonomous electrolyte discovery

Autonomous electrolyte discovery demands a computational engine that satisfies a critical trilemma: it must be fast enough for high-throughput screening, accurate enough for quantitative property prediction, and calibratable enough for online refinement. Classical empirical force fields (FFs) are fast but rely heavily on error cancellation, while standard machine learning interatomic potentials (MLIPs) are computationally expensive, lack rigorous long-range physics, and resist gradient-based calibration. In this Perspective, we highlight that differentiable hybrid FFs resolve this trilemma by fusing physically motivated functional forms with neural-network short-range corrections. Grounded in Energy Decomposition Analysis (EDA), state-of-the-art models such as PhyNEO-Electrolyte and ByteFF-Pol achieve zero-shot generalization to bulk phases, delivering throughputs on the order of tens of ns/day (up to $\sim$50 ns/day, depending on model complexity) for 10,000-atom systems. Crucially, their physical skeletons provide a well-conditioned parameter space for differentiable molecular dynamics (dMD). This enables a dual-calibration paradigm: bottom-up \textit{ab initio} parameterization combined with top-down fine-tuning from macroscopic experimental observables. We propose that this architecture meets the requirements of a ``ChemRobot-ready'' digital twin by integrating physics-grounded simulation with experimentally calibratable refinement, thereby enabling closed-loop autonomous electrolyte discovery.