Seven-photon absorption from Na+/Bi3+-alloyed Cs2AgInCl6 perovskites

Shiling Jin; Renfu Li; Jiwen Zhu; Tao Pang; Tianmin Wu; Hongbing Zhan; Yuanhui Zheng; Feng Huang; Xueyuan Chen; Daqin Chen

doi:10.1039/D2MH01396G

Seven-photon absorption from Na⁺/Bi³⁺-alloyed Cs₂AgInCl₆ perovskites†

Shiling Jin,‡^a Renfu Li,

‡^b Jiwen Zhu,^a Tao Pang,

^c Tianmin Wu,*^d Hongbing Zhan,^e Yuanhui Zheng,

^fg Feng Huang,

^a Xueyuan Chen

*^b and Daqin Chen

*^afh

Author affiliations

* Corresponding authors

^a College of Physics and Energy, Fujian Normal University, Fujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials, Fuzhou, Fujian, China
E-mail: dqchen@fjnu.edu.cn

^b CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Key Laboratory of Nanomaterials and State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, China
E-mail: xchen@fjirsm.ac.cn

^c Huzhou Key Laboratory of Materials for Energy Conversion and Storage, College of Science, Huzhou University, Zhejiang, Huzhou, China

^d Key Laboratory of Opto-Electronic Science and Technology for Medicine of Ministry of Education, Fujian Provincial Key Laboratory of Photonics Technology, College of Photonic and Electronic Engineering, Fujian Normal University, Fuzhou, Fujian, China
E-mail: wtm@fjnu.edu.cn

^e College of Materials Science and Engineering, Fuzhou University, Fuzhou, Fujian, China

^f Fujian Science & Technology Innovation Laboratory for Optoelectronic Information, Fuzhou, Fujian, China

^g College of Chemistry, Fuzhou University, Fuzhou, Fujian, China

^h Fujian Provincial Collaborative Innovation Center for Advanced High-Field Superconducting Materials and Engineering, Fuzhou, Fujian, China

Abstract

Nonlinear multi-phonon (2–7) absorption in the Na⁺/Bi³⁺-alloyed Cs₂AgInCl₆ lead-free double perovskites with ∼100% photoluminescence quantum yield and superior stability is observed for the first time, which can be pumped by a femtosecond laser in a wide spectral range (800–2600 nm). First-principles calculations verify that the parity-forbidden transition from the valence band maximum and conduction band minimum (at the Γ point) is not broken by Na⁺/Bi³⁺ doping, and strong optical band-to-band absorption occurs at the L&X points. Time-resolved emission spectra evidence that single-photon and multi-photon pumping leads to the same self-trapped exciton transition and high-order nonlinear absorption will not induce a remarkable thermal effect. Finally, we demonstrate that the Cs₂Na_0.4Ag_0.6In_0.99Bi_0.01Cl₆ DP shows great potential for next-generation wavelength-selective and highly sensitive multiphoton imaging applications.

Materials Horizons

Seven-photon absorption from Na⁺/Bi³⁺-alloyed Cs₂AgInCl₆ perovskites†

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Seven-photon absorption from Na⁺/Bi³⁺-alloyed Cs₂AgInCl₆ perovskites

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