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Synaptic behavior simulations through electronic, magnetic, or photonic devices based on metal oxides, 2D materials, molecular complex and phase change materials, represent important strategies for performing computational tasks with enhanced power efficiency. Here, a special class of memristive materials based on persistent luminescent memitters (termed as a portmanteau of \u201cmemory\u201d and \u201cemitter\u201d) with optical characteristics closely resembling those of biological synapses is reported. The memory process and synaptic plasticity can be successfully emulated using such memitters under precisely controlled excitation frequency, wavelength, pulse number, and power density. The experimental and theoretical data suggest that electron\u2010coupled trap nucleation and propagation through clustering in persistent luminescent memitters can explain experience\u2010dependent plasticity. The use of persistent luminescent memitters for multichannel image memorization that allows direct visualization of subtle changes in luminescence intensity and realization of short\u2010term and long\u2010term memory is also demonstrated. These findings may promote the discovery of new functional materials as artificial synapses and enhance the understanding of memory mechanisms.<\/jats:p>","DOI":"10.1002\/adma.202101895","type":"journal-article","created":{"date-parts":[[2021,6,19]],"date-time":"2021-06-19T03:11:22Z","timestamp":1624072282000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":55,"title":["Multimodal Tuning of Synaptic Plasticity Using Persistent Luminescent Memitters"],"prefix":"10.1002","volume":"34","author":[{"given":"Hongyu","family":"Bian","sequence":"first","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 117543 Singapore"}]},{"given":"Xian","family":"Qin","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 117543 Singapore"}]},{"given":"Yiming","family":"Wu","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 117543 Singapore"}]},{"given":"Zhigao","family":"Yi","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 117543 Singapore"}]},{"given":"Sirui","family":"Liu","sequence":"additional","affiliation":[{"name":"Department of Chemistry National University of Singapore  Singapore 117543 Singapore"}]},{"given":"Yu","family":"Wang","sequence":"additional","affiliation":[{"name":"SZU\u2010NUS Collaborative Center and International Collaborative Laboratory of 2D Materials for Optoelectronic Science and Technology of Ministry of Education Institute of Microscale Optoelectronics Shenzhen University  Shenzhen 518060 China"}]},{"given":"Carlos D. 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