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Herein, it is designed and synthesize a multi\u2010sulfur Raman reporter, NF1064, whose maximum absorption of 1064\u00a0nm rigidly resonates with NIR\u2010II excitation laser while possessing absolutely nonfluorescent backgrounds. Ultrafast spectroscopy suggests that the fluorescence quenching mechanism of NF1064 originates from twisted intramolecular charge transfer (TICT) in the excited state. Gold nanorods (AuNRs) decorated with such nonfluorescent NF1064 (AuNR@NF1064) show remarkable SERRS performances, including zero\u2010fluorescence background, femtomolar\u2010level sensitivity as well as superb photostability without fluorescence photobleaching. More importantly, AuNR@NF1064 exhibits a nonlinear photothermal effect upon plasmonic fields of AuNRs by amplifying the non\u2010radiative decay of nonfluorescent NF1064, thus achieving a high photothermal conversion of 68.5% in NIR\u2010II window with potential for further augmentation. With remarkable SERRS and photothermal properties, the NIR\u2010II nanoprobes allow for high\u2010precision intraoperative guided tumor resection within 8\u00a0min, and high\u2010efficient hyperthermia combating of drug\u2010resistant bacterial infection within living mouse body. This work not only unlocks the potential of nonfluorescent resonant dyes for NIR\u2010II Raman imaging, but also opens up a new method for boosting photothermal conversion efficiency of nanomaterials.<\/jats:p>","DOI":"10.1002\/smll.202407787","type":"journal-article","created":{"date-parts":[[2024,11,29]],"date-time":"2024-11-29T07:10:42Z","timestamp":1732864242000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Ultrasensitive NIR\u2010II Surface\u2010Enhanced Resonance Raman Scattering Nanoprobes with Nonlinear Photothermal Effect for Optimized Phototheranostics"],"prefix":"10.1002","volume":"21","author":[{"given":"Laicui","family":"Song","sequence":"first","affiliation":[{"name":"CAS Key Laboratory of Coastal Environmental Processes and Ecological Remediation Yantai Institute of Coastal Zone Research Chinese Academy of Sciences  Yantai 264003 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