Lin, Chia-YangChia-YangLinChen, Mei-NungMei-NungChenKimpel, JoostJoostKimpelHe, WanerWanerHeGUEY-SHENG LIOUChiu, Yu-ChengYu-ChengChiuMichinobu, TsuyoshiTsuyoshiMichinobu2026-01-152026-01-152025-07-25https://www.scopus.com/record/display.uri?eid=2-s2.0-105024757598&origin=resultslisthttps://scholars.lib.ntu.edu.tw/handle/123456789/735333Response time and lifetime are imperative in photoresponsive organic field-effect transistor (OFET) memory devices. In this study, we demonstrate the improvement of these properties through postpolymerization functionalization of an alkyne-containing conjugated copolymer. By subjecting a synthesized Tröger’s base and carbazole copolymer (pTBC) to a [2 + 2] cycloaddition–retroelectrocyclization (CA-RE) click reaction with tetracyanoethylene, the electronic character of the polymer changes from donor to donor–acceptor characters. The postfunctionalized tetracyanobutadiene (TCBD) polymer, pTBC-TCBD, showcases much shorter photoerasing speeds (0.2 s, five times faster) and a longer retention time of 50,000 s in a pentacene-based device, as compared to the precursor polymer (pTBC). Both factors originate from the cyano groups: faster photoerasure originates from the assisted dissociation of excitons and higher stability comes from better hole trapping of pTBC-TCBD. Accordingly, [2 + 2] CA-RE click postfunctionalization proves a viable design strategy for polymer-based photoresponsive OFET memories.donor−acceptor conjugated polymerphotoinduced recoveryphotoresponsive OFET memoryTröger’s base copolymer[2 + 2] CA-RE click reaction[SDGs]SDG7journal article10.1021/acsapm.5c01667