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However, the interfacial dipolar mechanisms governing memory window (\u0394V) formation and modulation remain insufficiently understood. Here, polyacrylonitrile (PAN) is selected as a representative polar polymer interlayer to exploit nitrile (C\uf8fdN) dipolar relaxation for temporal acoustic reservoir computing (RC). It is found that the \u0394V varies nonmonotonically with PAN concentration, suggesting a dipolar competition mechanism between interfacial polarization strength and dipole relaxation capability. Accordingly, dipolar relaxation underpins multiscale synaptic responses and fading memory for temporal RC. The device further exhibits stable and symmetric weight updates, with a low asymmetry ratio (AR) of 5.06% and cycle\u2010to\u2010cycle variations (CCVs) below 1%. Notably, the PAN\u2010OST operates with an ultralow event energy of 50\u00a0aJ while maintaining a high signal\u2010to\u2010noise ratio (SNR) of 50.47\u00a0dB. The PAN reservoir achieves 97.17% accuracy in spoken digit recognition and a maximum accuracy of 94.8% in the more challenging speech emotion recognition. Overall, this work establishes an interfacial polarization\u2010driven pathway for energy\u2010efficient neuromorphic computing and next\u2010generation intelligent hardware.<\/jats:p>","DOI":"10.1002\/advs.78389","type":"journal-article","created":{"date-parts":[[2026,10,21]],"date-time":"2026-10-21T04:48:01Z","timestamp":1792558081000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Interfacial Polarization Dynamics of Nitrile Dipoles in Organic Synaptic Transistors for Acoustic Reservoir Computing"],"prefix":"10.1002","author":[{"given":"Yutian","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou 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