Ultrafast All-Optical Modulation in 2D Hybrid Perovskites. 2019

Gustavo Grinblat, and Ibrahim Abdelwahab, and Michael P Nielsen, and Paul Dichtl, and Kai Leng, and Rupert F Oulton, and Kian Ping Loh, and Stefan A Maier
The Blackett Laboratory, Department of Physics , Imperial College London , London SW7 2AZ , United Kingdom.

Two-dimensional (2D) hybrid organic-inorganic Ruddlesden-Popper perovskites (RPPs) have been recently shown to exhibit large nonlinear optical properties due to the strong excitonic effects present in their multiple quantum wells. In this work, we use nondegenerate pump-probe spectroscopy in the 600-1000 nm wavelength range to study the influence of nonlinear effects on the ultrafast dynamics of 2D RPP thin flakes. We find that, under sub-bandgap excitation, ∼100 nm thick perovskite sheets allow up to ∼2% reflectivity modulation within a 20 fs period, due to the nonlinear optical Kerr effect and two-photon absorption, surpassing by a factor of ∼5 the reported nonlinear performance of photonic metasurfaces and single nanoantennas. When the excitation is resonant with the excitonic absorption, the ultrafast nature of the nonlinear response is lost due to the presence of linear absorption creating long-lived free carriers. Our results suggest that 2D RPPs are potential nanoscale all-optical modulators in the visible/near-infrared waveband for applications such as ultrafast information processing, optical data transmission, and high-performance computing.

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