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Optical gain was revealed for nonfluorescent derivatives <jats:bold>3<\/jats:bold> and <jats:bold>4<\/jats:bold> in the near infrared (NIR) spectral range under femtosecond excitation. The values of two\u2010photon absorption (2PA) and excited\u2010state absorption (ESA) cross\u2010sections were obtained for <jats:bold>1\u20134<\/jats:bold> in dichloromethane using femtosecond Z\u2010scans, and the role of bromine substituents in the molecular structures of <jats:bold>2<\/jats:bold> and <jats:bold>4<\/jats:bold> is discussed. The nature of the excited states involved in electronic transitions of these dyes was investigated using quantum\u2010chemical TD\u2010DFT calculations, and the obtained spectral parameters are in reasonable agreement with the experimental data. Significant 2PA (maxima cross\u2010sections \u223c2000\u2005GM), and large ESA cross\u2010sections \u223c10<jats:sup>\u221220<\/jats:sup>\u2005m<jats:sup>2<\/jats:sup> of these new aza\u2010BODIPY derivatives <jats:bold>1\u20134<\/jats:bold> along with their measured high photostability reveal their potential for photonic applications in general and optical limiting in particular.<\/jats:p>","DOI":"10.1002\/chem.202104072","type":"journal-article","created":{"date-parts":[[2022,2,14]],"date-time":"2022-02-14T12:46:12Z","timestamp":1644842772000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Femtosecond Spectroscopy and Nonlinear Optical Properties of aza\u2010BODIPY Derivatives in Solution"],"prefix":"10.1002","volume":"28","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4207-1056","authenticated-orcid":false,"given":"Hao\u2010Jung","family":"Chang","sequence":"first","affiliation":[{"name":"CREOL, The College of Optics and Photonics University of Central Florida  Orlando FL 32816 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2657-4654","authenticated-orcid":false,"given":"Mykhailo V.","family":"Bondar","sequence":"additional","affiliation":[{"name":"CREOL, The College of Optics and Photonics University of Central Florida  Orlando FL 32816 USA"},{"name":"Institute of Physics NASU  Prospect Nauki, 46 Kyiv-28 03028 Ukraine"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4618-4290","authenticated-orcid":false,"given":"Natalia","family":"Munera","sequence":"additional","affiliation":[{"name":"CREOL, The College of Optics and Photonics University of Central Florida  Orlando FL 32816 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sylvain","family":"David","sequence":"additional","affiliation":[{"name":"Univ. 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