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However, their practical applications in high-current-density LEDs are fundamentally constrained by severe efficiency roll-off, primarily caused by nonradiative recombination and carrier-induced structural instabilities. In this study, we introduce a molecular N,N\u2032-diphenylthiourea (DPTA)-engineered tin perovskite semiconductor (CsSnI3) that achieves a photoluminescence quantum efficiency (PLQE) of 36% at a carrier concentration of 1018 cm\u20133. Our approach enables precise control over the charge-carrier concentration and lattice growth. High-resolution transmission electron microscopy further demonstrates that the uniform local strain distribution in the doped films enhances carrier wave-function overlap, leading to a substantial boost in PLQE. Leveraging the enhanced optoelectronic properties of DPTA-treated CsSnI3, we fabricate near-infrared LEDs that exhibit an external quantum efficiency (EQE) of 13.4% and an unprecedented peak radiance of 1248 W sr\u20131 m\u20132, with minimal efficiency roll-off even at high current densities exceeding 3500 mA cm\u20132 in pulse-mode operation. This work introduces a new material-doping strategy for lead-free perovskites, demonstrating their potential for high-power optoelectronic applications and advancing the feasibility of electrically pumped perovskite laser diodes.<\/jats:p>","DOI":"10.1021\/jacs.6c05302","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T12:40:54Z","timestamp":1784119254000},"page":"30989-30997","source":"Crossref","is-referenced-by-count":0,"title":["Ultrabright Near-Infrared\nLead-Free Perovskite Light-Emitting\nDiodes with Negligible Efficiency Roll-Off"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3630-0414","authenticated-orcid":true,"given":"Tianjun","family":"Liu","sequence":"first","affiliation":[{"name":"University of Cambridge , , ,","place":["Cambridge, U.K., CB3 0HE"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qichun","family":"Gu","sequence":"additional","affiliation":[{"name":"University of 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