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Hot-carrier tunable abnormal nonlinear absorption conversion in quasi-2D perovskite

Gang Wang, Tanghao Liu, Bingzhe Wang, Hao Gu, Qi Wei, Zhipeng Zhang, Jun He (), Mingjie Li () and Guichuan Xing ()
Additional contact information
Gang Wang: Avenida da Universidade
Tanghao Liu: Avenida da Universidade
Bingzhe Wang: Avenida da Universidade
Hao Gu: Avenida da Universidade
Qi Wei: The Hong Kong Polytechnic University
Zhipeng Zhang: Avenida da Universidade
Jun He: Central South University
Mingjie Li: The Hong Kong Polytechnic University
Guichuan Xing: Avenida da Universidade

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Controlling the high-power laser transmittance is built on the diverse manipulation of multiple nonlinear absorption (NLA) processes in the nonlinear optical (NLO) materials. According to standard saturable absorption (SA) and reverse saturable absorption (RSA) model adapted for traditional semiconductor materials, the coexistence of SA and RSA will result in SA induced transparency at low laser intensity, yet switch to RSA with pump fluence increasing. Here, we observed, in contrast, an unusual RSA to SA conversion in quasi-two-dimensional (2D) perovskite film with a low threshold around 2.6 GW cm−2. With ultrafast transient absorption (TA) spectra measurement, such abnormal NLA is attributed to the competition between excitonic absorption enhancement and non-thermalized carrier induced bleaching. TA singularity from non-thermalized “Fermi Sea” is observed in quasi-2D perovskite film, indicating an ultrafast carrier thermalization within 100 fs. Moreover, the comparative study between the 2D and 3D perovskites uncovers the crucial role of hot-carrier effect to tune the NLA response. The ultrafast carrier cooling of quasi-2D perovskite is pointed out as an important factor to realize such abnormal NLA conversion process. These results provide fresh insights into the NLA mechanisms in low-dimensional perovskites, which may pave a promising way to diversify the NLO material applications.

Date: 2022
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DOI: 10.1038/s41467-022-34705-8

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