Robust Nonvolatile Memory and Synaptic Emulation via Dual‐Mode Modulation in ReS ₂ /h‐BN/Ta ₂ NiSe ₅ Floating‐Gate Device

The integration of optical sensing with neuromorphic computing offers a promising pathway to overcome the von Neumann bottleneck in data‐intensive artificial intelligence applications. However, realizing robust nonvolatile storage with synergistic electrical and optical modulation in 2D devices remains a challenge. Here, we demonstrate a high‐performance floating‐gate memory based on a ReS 2 /h‐BN/Ta 2 NiSe 5 van der Waals heterostructure. Under precise photo‐electrical cooperative modulation, the device exhibits excellent nonvolatile memory characteristics, including a large memory window of 96.2 V, long retention exceeding 10 4 s, and stable endurance over 1000 cycles. Additionally, it features multi‐bit storage capabilities enabled by optical erasure and electrical writing. Beyond digital storage, the device effectively mimics biological synaptic plasticity, such as paired‐pulse facilitation and learning processes. Validating its potential for neuromorphic vision systems, a simulated three‐layer artificial neural network achieves a high recognition accuracy of 96.43% on the MNIST dataset. This work establishes a promising paradigm for future integrated sensing, storage, and computation applications based on 2D materials.