Resonantly enhanced multiple exciton generation through below-band-gap multi-photon absorption in perovskite nanocrystals.

Manzi, Aurora; Tong, Yu; Feucht, Julius; Yao, En-Ping; Polavarapu, Lakshminarayana; Urban, Alexander S; Feldmann, Jochen · Nat Commun · 2018

basic_science · Level V

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Abstract

Multi-photon absorption and multiple exciton generation represent two separate strategies for enhancing the conversion efficiency of light into usable electric power. Targeting below-band-gap and above-band-gap energies, respectively, to date these processes have only been demonstrated independently. Here we report the combined interaction of both nonlinear processes in CsPbBr<sub>3</sub> perovskite nanocrystals. We demonstrate nonlinear absorption over a wide range of below-band-gap excitation energies (0.5-0.8 E<sub>g</sub>). Interestingly, we discover high-order absorption processes, deviating from the typical two-photon absorption, at specific energetic positions. These energies are associated with a strong enhancement of the photoluminescence intensity by up to 10<sup>5</sup>. The analysis of the corresponding energy levels reveals that the observed phenomena can be ascribed to the resonant creation of multiple excitons via the absorption of multiple below-band-gap photons. This effect may open new pathways for the efficient conversion of optical energy, potentially also in other semiconducting materials.