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However, only a limited number of SICTERS\u2011active molecules have been reported to date, constraining their broader applications. Herein, we reported a rational strategy to transform conventional fluorophores into SICTERS probes based on two fundamental findings. One is that sulfur\u2010to\u2010selenium substitution is capable of suppressing radiative decay for fluorescence quenching, distinct from its conventional role in red\u2010shifting emission. The other is that N\u2010alkylation enables tuning the absorption profile for Raman enhancement, beyond its traditional use in improving molecular solubility. Mechanistic studies validate these findings. Consequently, a novel SICTERS\u2010active molecule (ATSe) was synthesized from a representative fluorophore (HTS). ATSe exhibited pronounced fluorescence quenching (quantum yield as low as 0.01%) and superior Raman sensitivity (detection limit of 0.014\u00a0\u00b5g\u00a0mL\n                    <jats:sup>\u22121<\/jats:sup>\n                    ). ATSe also displayed an exceptional photothermal conversion efficiency of 71.37%, arising from its accelerated nonradiative dissipation. In an orthotopic colon tumor model, ATSe enabled highly effective Raman imaging\u2011guided photothermal therapy. This work introduces a general method to convert conventional fluorophores into SICTERS probes, opening new avenues for SICTERS\u2011based biological applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.5300342","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T04:07:55Z","timestamp":1788149275000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Tailoring of Fluorescent Agents Toward SICTERS\u2010Active Raman Probes"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-4553-2398","authenticated-orcid":false,"given":"Wenxian","family":"Zhang","sequence":"first","affiliation":[{"name":"Department of Pharmacology and Chemical Biology Institute of Molecular Medicine Key Laboratory of Cell Differentiation and Apoptosis of Chinese Ministry of Education Shanghai Jiao Tong University School of Medicine  Shanghai 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