Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals

作者：Weiqiang Chen, Saikat Bhaumik, Sjoerd A. Veldhuis, Guichuan Xing, Qiang Xu, Michaël Grätzel, Subodh G. Mhaisalkar, Nripan Mathews, Tze Chien Sum · 发表于：Nature Communications · 年份：2017 · DOI：10.1038/ncomms15198 · 被引用次数：245 · 研究领域：Nonlinear Optical Materials Studies、Perovskite Materials and Applications、Luminescence and Fluorescent Materials

Multiphoton absorption processes enable many technologically important applications, such as in vivo imaging, photodynamic therapy and optical limiting, and so on. Specifically, higher-order nonlinear absorption such as five-photon absorption offers significant advantages of greater spatial confinement, increased penetration depth, reduced autofluorescence, enhanced sensitivity and improved resolution over lower orders in bioimaging. Organic chromophores and conventional semiconductor nanocrystals are leaders in two-/three-photon absorption applications, but face considerable challenges from their small five-photon action cross-sections. Herein, we reveal that the family of halide perovskite colloidal nanocrystals transcend these constraints with highly efficient five-photon-excited upconversion fluorescence-unprecedented for semiconductor nanocrystals. Amazingly, their multidimensional type I (both conduction and valence band edges of core lie within bandgap of shell) core-shell (three-dimensional methylammonium lead bromide/two-dimensional octylammonium lead bromide) perovskite nanocrystals exhibit five-photon action cross-sections that are at least 9 orders larger than state-of-the-art specially designed organic molecules. Importantly, this family of halide perovskite nanocrystals may enable fresh approaches for next-generation multiphoton imaging applications.