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Here, we report the synthesis of TaFeTe\n                    <jats:sub>2<\/jats:sub>\n                    single crystals that can be mechanically exfoliated to the 2D limit. The as\u2010grown crystals display characteristic spin\u2010glass behavior and intrinsic unsaturated negative magnetoresistance up to 9 T, likely arising from the orbital effect associated with variable\u2010range hopping transport and\/or magnetic disordering. Notably, TaFeTe\n                    <jats:sub>2<\/jats:sub>\n                    \u2010based photodetectors exhibit robust photocurrent responses in the sample's interior under self\u2010powered conditions, primarily arising from an additional charge separation mechanism induced by the optical\u2010phonon\u2010triggered non\u2010centrosymmetric phase. Under standard bias, the detectors achieve a high responsivity of 0.18 A W\n                    <jats:sup>\u22121<\/jats:sup>\n                    and broadband photoresponse spanning the visible to mid\u2010infrared spectrum. These features highlight the material's strong potential for advanced multifunctional optoelectronic applications.\n                  <\/jats:p>","DOI":"10.1002\/advs.202523555","type":"journal-article","created":{"date-parts":[[2026,1,27]],"date-time":"2026-01-27T12:20:58Z","timestamp":1769516458000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Intrinsic Negative Magnetoresistance and Broadband Photoresponse in Magnetic van der Waals Crystal TaFeTe\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"13","author":[{"given":"Changcun","family":"Li","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering University of Jinan  Jinan China"},{"name":"Yangtze Delta Region Institute (Huzhou) and School of Optoelectronic Science and Engineering University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Jiazhen","family":"Wu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Quantum Functional Materials Department of Materials Science and Engineering Southern University of Science and Technology  Shenzhen China"},{"name":"Guangdong Provincial Key Laboratory of Functional Oxide Materials and Devices Southern University of Science and Technology  Shenzhen China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Sirong","family":"Lu","sequence":"additional","affiliation":[{"name":"Department of Physics Southern University of Science and Technology  Shenzhen China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Lei","family":"Liang","sequence":"additional","affiliation":[{"name":"Yangtze Delta Region Institute (Huzhou) and School of Optoelectronic Science and Engineering University of Electronic Science and Technology of China  Chengdu China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Wenying","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering University of Jinan  Jinan China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Bingke","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering University of Jinan  Jinan China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Degang","family":"Zhao","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering University of Jinan  Jinan China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1275-0573","authenticated-orcid":false,"given":"Fucai","family":"Liu","sequence":"additional","affiliation":[{"name":"Yangtze Delta Region Institute (Huzhou) and School of Optoelectronic Science and Engineering University of Electronic Science and 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