Abstract All‐optical artificial synaptic devices offer promising potential for neuromorphic computing, yet their development is hindered by limited spectral tunability and poor plasticity linearity. Here, a broadband all‐optical synaptic memtransistor based on organic charge transfer cocrystals (DTT‐TCNQ) is reported, which enables fully light‐driven and reversible modulation of synaptic weights across a wide wavelength range (395–808 nm). The device exhibits bidirectional excitatory and inhibitory photoresponses, and achieves highly linear long‐term potentiation and depression (LTP/LTD) characteristics with ultralow nonlinearity (α p = 0.00191, α d = 0.00305) and asymmetry ratio (AR = 0.00114), attributed to a synergistic strategy combining frequency modulation and photoelectric coupling. When integrated into a convolutional neural long short‐term memory network (CNN‐LSTM) hybrid network, the device enables rapid convergence (98.77% accuracy in 6 training epochs) and robust recognition performance under spatiotemporal noise, outperforming conventional light‐write/electric‐erasing schemes. This work bridges material‐level innovation and system‐level functionality, offering a scalable approach toward energy‐efficient, noise‐resilient neuromorphic vision systems.
Cai et al. (Tue,) studied this question.