Actively Programming Battery Chemistry via Pulse Modulation

The advancement of high-energy electrochemical energy storage is increasingly throttled by the kinetic and thermodynamic bottlenecks inherent to steady-state operation. This perspective posits that pulse modulation represents a fundamental paradigm shift, moving beyond empirical charging protocols toward a sophisticated framework for the active, real-time regulation of multiscale battery chemistry. By leveraging nonequilibrium transients, pulsed excitation enables the temporal decoupling of entangled physicochemical processes, including ion solvation sheath reorganization, interfacial charge transfer, and long-range mass transport that remain inaccessible under conventional constant-current conditions. We elucidate the underlying chemical physics of this approach, examining how a high-dimensional parameter space of amplitude, frequency, and waveform morphology dictates the concentration polarization, solid-electrolyte interphase evolution, and metal deposition morphology across micro- to macroscales. Furthermore, this work evaluates the convergence of operando diagnostics with physics-informed machine learning as a strategic route to navigate the vast combinatorial spaces of pulse protocols. By integrating multiphysics modeling with closed-loop control, we outline a roadmap for software-defined chemistry, where adaptive protocols dynamically compensate for state-of-health drift and thermal fluctuations. Ultimately, this perspective advocates for a transition from treating the battery as a passive electrochemical reservoir to an actively modulated system, providing a theoretical foundation for the next-generation, closed-loop battery management capable of multisource-field cooperative regulation of the electrochemical environment.