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Functional materials displaying large ultrafast third-order optical nonlinearities across a wide spectral region and broad temporal domain are required for all-optical signal processing. Particularly desirable is nonlinear optical (NLO) activity at near-infrared (NIR) wavelengths with femtosecond pulses. Herein the first triply-fused porphyrin dimer (TFP)-functionalized single-walled carbon nanotube (SWCNT) nanohybrid was successfully constructed by covalently grafting TFPs onto SWCNT. The results of Z-scan techniques demonstrate that the newly obtained TFP-SWCNT nanohybrid was found with a strong NLO performance under both nanosecond and femtosecond irradiation. In the nanosecond regime, an enhancement in optical limiting (OL) of the TFP-SWCNT nanohybrid is seen at 532 nm when compared with the performance of porphyrin monomer-functionalized SWCNT nanohybrid Por-SWCNT. Under femtosecond irradiation, the TFP-SWCNT nanohybrid exhibits a particularly strong OL effect with a giant two-photon absorption (TPA) cross section value (ca. 15,500 GM) at 800 nm pulses that mainly stems from intense TPA of TFP, in sharp contrast to the Por-SWCNT nanohybrid which exhibits only saturable absorption under identical irradiation. These results demonstrate that the newly-developed TFP-SWCNT nanohybrid is a very promising OL candidate for practical applications across wide spectral and temporal domains, and that covalently functionalizing carbon-based materials with triply-fused chromophores may be a useful approach to engineering adaptable photonic devices with broad-ranging NLO activity.
The authors acknowledge financial support from the National Natural Science Foundation of China (No. 51432006), the Ministry of Science and Technology of China for the International Science Linkages Program (No. 2011DFG52970), the Ministry of Education of China for the Changjiang Innovation Research Team (No. IRT14R23), the Ministry of Education and the State Administration of Foreign Experts Affairs for the 111 Project (No. B13025), and the Innovation Program of Shanghai Municipal Education Commission. M. G. H thanks the Australian Research Council (No. DP170100411) for support.