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An investigation of broadband optical nonlinear absorption and transient nonlinear refraction in a fluorenone-based compound.

ABSTRACT: A novel fluorenone derivative, FO52, is designed and synthesized. The fluorenone group is introduced to provide the central π-conjugated system in the molecule and triphenylamine is substituted at both sides. Intramolecular Charge Transfer (ICT) from the terminal groups to the molecular center is confirmed via DFT calculations. Ultrafast optical nonlinearities are investigated via Z-scan and transient absorption spectroscopy (TAS) studies with a 190 fs laser. Reverse saturable absorption, two-photon induced excited-state absorption, and pure two-photon absorption are observed at 532 nm, 650 nm, and 800 nm, respectively. The different mechanisms at these wavelengths are discussed and interpreted with assistance from the results from TAS. Furthermore, strong excited-state refraction and ultrafast negative refraction from the bound electron response are resolved and discussed in phase object pump probe (POPP) experiments. The results suggest that the ICT-enhanced optical nonlinearities provide FO52 with strong optical limiting capabilities at visible wavelengths and ultrafast refraction with tiny attenuation in the near infrared region. The combination of these properties in one compound could be attractive for applications like laser protection and low-loss all-optical switching.

SUBMITTER: Wu X

PROVIDER: S-EPMC9031121 | biostudies-literature | 2021 Apr

REPOSITORIES: biostudies-literature

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An investigation of broadband optical nonlinear absorption and transient nonlinear refraction in a fluorenone-based compound.

Wu Xingzhi X Xiao Jinchong J Han Yanbing Y Xu Jiabei J Zhou Wenfa W Li Yang Y Fang Yu Y Chen Yongqiang Y Wu Quanying Q Song Yinglin Y

RSC advances 20210429 26

A novel fluorenone derivative, FO52, is designed and synthesized. The fluorenone group is introduced to provide the central π-conjugated system in the molecule and triphenylamine is substituted at both sides. Intramolecular Charge Transfer (ICT) from the terminal groups to the molecular center is confirmed <i>via</i> DFT calculations. Ultrafast optical nonlinearities are investigated <i>via</i> Z-scan and transient absorption spectroscopy (TAS) studies with a 190 fs laser. Reverse saturable abso ...[more]

PMID: 35481210

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Project description:Nonlinear optical (NLO) pigments are compounds insoluble in solvents that exhibit phenomena related to nonlinear optical susceptibilities (χ(n) where n = 2,3,...), e.g., two-photon absorption (2PA) which is related to the imaginary part of χ(3). Determination of spectrally-resolved 2PA properties for NLO pigments of macromolecular nature, such as coordination polymers or crosslinked polymers, has long been a challenging issue due to their particulate form, precluding characterizations with standard techniques such as Z-scan. In this contribution, we investigate thus far unknown spectrally-resolved 2PA properties of a new subclass of NLO pigments-crosslinked conjugated polymers. The studied compounds are built up from electron-donating (triphenylamine) and electron-withdrawing (2,2'-bipyridine) structural fragments joined by vinylene (Pol1) or vinyl(4-ethynylphenyl) (Pol2) aromatic bridges. 2PA properties of these polymers have been characterized in broad spectral range by specially modified two-photon excited fluorescence (TPEF) techniques: solid state TPEF (SSTPEF) and internal standard TPEF (ISTPEF). The impact of self-aggregation of aromatic backbones on the 2PA properties of the polymers has been evaluated through extended comparisons of NLO parameters, i.e., 2PA cross sections (σ2) and molar-mass normalized 2PA merit factors (σ2/M) with those of small-molecular model compounds: Mod1 and Mod2. By doing this, we found that the 2PA response of Pol1 and Pol2 is improved 2-3 times versus respective model compounds in the solid state form. Further comparisons with 2PA results collected for diluted solutions of Mod1 and Mod2 supports the notion that self-aggregated structure contributes to the observed enhancement of 2PA response. On the other hand, it is clear that Pol1 and Pol2 suffer from aggregation-caused quenching phenomenon, well reflected in time-resolved fluorescence properties as well as in relatively low values of quantum yield of fluorescence. Accordingly, despite improved intrinsic 2PA response, the effective intensity of two-photon excited emission for Pol1 and Pol2 is slightly lower relative to Mod1 and Mod2. Finally, we explore temperature-resolved luminescence properties under one- (377 nm), two- (820 nm), and three-photon excitation (1020 nm) conditions of postsynthetically Eu3+-functionalized material, Pol1-Eu, and discuss its suitability for temperature sensing applications.

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An investigation of broadband optical nonlinear absorption and transient nonlinear refraction in a fluorenone-based compound.

Publications

An investigation of broadband optical nonlinear absorption and transient nonlinear refraction in a fluorenone-based compound.

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