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Dielectric polymers typically exhibit a low dielectric constant, while their energy density at elevated temperatures is limited by drastically increased conduction. To address this challenge, it is reported that proton irradiation enables concurrently enhanced dielectric constant and energy storage properties at high temperatures. The combined atomic force microscopy\u2010infrared spectroscopy and first\u2010principles calculations reveal that proton irradiation facilitates local rotation of ether bonds in aromatic polymers, producing greatly increased local polar states leading to markedly improved polarizability while preserving dense chain packing. Consequently, an ultrahigh discharged energy density of 6.9 J cm\n                    <jats:sup>\u22123<\/jats:sup>\n                    with an efficiency &gt; 95% is achieved in irradiated poly(ether imide) at 150\u00a0\u00b0C, exceeding current dielectric polymers and nanocomposites. The results suggest an alternative postprocessing method toward rational design of high\u2010performance dielectrics for capacitive energy storage.\n                  <\/jats:p>","DOI":"10.1002\/advs.202522035","type":"journal-article","created":{"date-parts":[[2025,11,30]],"date-time":"2025-11-30T17:07:27Z","timestamp":1764522447000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Ultrahigh High\u2010temperature Capacitive Energy Storage Via Proton Irradiation"],"prefix":"10.1002","volume":"13","author":[{"given":"Chenyi","family":"Li","sequence":"first","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"},{"name":"Guangdong HUST Industrial Technology Research Institute Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization Dongguan Guangdong 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hanxiao","family":"Gao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"},{"name":"Guangdong HUST Industrial Technology Research Institute Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization Dongguan Guangdong 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yutie","family":"Gong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yen\u2010Ting","family":"Lin","sequence":"additional","affiliation":[{"name":"Guangdong HUST Industrial Technology Research Institute Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization Dongguan Guangdong 523808 China"},{"name":"Department of Chemical Engineering and Materials Research Institute Pennsylvania State University University Park PA 16802 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuquan","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuanqi","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"},{"name":"Guangdong HUST Industrial Technology Research Institute Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization Dongguan Guangdong 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lan","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hangyao","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Material Processing and Die &amp; Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 China"},{"name":"Guangdong HUST Industrial Technology Research Institute Guangdong Provincial Key Laboratory of Manufacturing Equipment Digitization Dongguan Guangdong 523808 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ling","family":"Cheng","sequence":"additional","affiliation":[{"name":"RICOTON Technology Co., Ltd. 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