Femtosecond Spectroscopy and Nonlinear Optical Properties of aza-BODIPY Derivatives in Solution |
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Authors: | Hao-Jung Chang Mykhailo V Bondar Dr Natalia Munera Dr Sylvain David Dr Olivier Maury Dr Gerard Berginc Dr Boris Le Guennic Dr Denis Jacquemin Dr Chantal Andraud Dr David J Hagan Dr Eric W Van Stryland |
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Institution: | 1. CREOL, The College of Optics and Photonics, University of Central Florida, Orlando, FL, 32816 USA;2. Univ. Lyon, ENS Lyon, CNRS UMR 5182, Laboratoire de Chimie, 46 Allée d'Italie, 69364 Lyon, France;3. Thales LAS France, 2 Avenue Gay Lussac, 78990 Élancourt, France;4. CNRS, Institut des Sciences Chimiques de Rennes UMR 6266, Université Rennes, 35000 Rennes, France;5. CNRS, CEISAM UMR 6230, Univ. Nantes, 44000 Nantes, France |
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Abstract: | The fast relaxation processes in the excited electronic states of functionalized aza-boron-dipyrromethene (aza-BODIPY) derivatives ( 1 – 4 ) were investigated in liquid media at room temperature, including the linear photophysical, photochemical, and nonlinear optical (NLO) properties. Optical gain was revealed for nonfluorescent derivatives 3 and 4 in the near infrared (NIR) spectral range under femtosecond excitation. The values of two-photon absorption (2PA) and excited-state absorption (ESA) cross-sections were obtained for 1–4 in dichloromethane using femtosecond Z-scans, and the role of bromine substituents in the molecular structures of 2 and 4 is discussed. The nature of the excited states involved in electronic transitions of these dyes was investigated using quantum-chemical TD-DFT calculations, and the obtained spectral parameters are in reasonable agreement with the experimental data. Significant 2PA (maxima cross-sections ~2000 GM), and large ESA cross-sections ~10?20 m2 of these new aza-BODIPY derivatives 1–4 along with their measured high photostability reveal their potential for photonic applications in general and optical limiting in particular. |
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Keywords: | aza-boron dipyrromethene derivatives femtosecond transient absorption pump-probe spectroscopy TD-DFT calculations two-photon absorption |
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