Spatiotemporal Programming via Asymmetric Dielectric Engineering for Nonvolatile 2D Optoelectronics

Abstract Ambipolar two-dimensional (2D) semiconductors integrated with floating-gate architectures offer a promising platform for nonvolatile, reconfigurable electronics. However, the switching between p–n and n–p junction polarities has conventionally required complex multigate designs, hindering the scalability and integration density. Here, we demonstrate a spatiotemporal programming strategy using a dual-floating-gate architecture with a symmetry-broken tunneling dielectric. An asymmetric dielectric stack creates distinct tunneling thresholds for two floating gates, enabling a single input gate to encode spatial doping profiles in the 2D channel via defined voltage pulse sequences. We achieve on-demand, nonvolatile, and reversible switching between p–n and n–p configurations with excellent retention and endurance. The reconfigurable homojunction serves as a multifunctional platform for logic encoding, rectification, photodetection, and in-sensor computing. This work establishes a design paradigm that replaces spatial input complexity with spatiotemporal programming, paving the way for high-density, multifunctional intelligent hardware.