In-Plane Anisotropic Nonlinear Optical Properties of Two-Dimensional Organic-Inorganic Hybrid Perovskite

Zhihui Chen; Qi Zhang; Menglong Zhu; Hao Chen; Xinyun Wang; Si Xiao; Kian Ping Loh; Goki Eda; Jianqiao Meng; Jun He

doi:10.1021/acs.jpclett.1c01890

In-Plane Anisotropic Nonlinear Optical Properties of Two-Dimensional Organic-Inorganic Hybrid Perovskite

J Phys Chem Lett. 2021 Jul 29;12(29):7010-7018. doi: 10.1021/acs.jpclett.1c01890. Epub 2021 Jul 21.

Authors

Zhihui Chen¹, Qi Zhang², Menglong Zhu³, Hao Chen², Xinyun Wang³, Si Xiao¹, Kian Ping Loh³, Goki Eda², Jianqiao Meng¹, Jun He¹

Affiliations

¹ Hunan Key Laboratory of Nanophononics and Devices, School of Physics and Electronics, Central South University, 932 South Lushan Road, Changsha, Hunan 410083, P.R. China.
² Department of Physics, National University of Singapore, 2 Science Drive 3, 117542, Singapore.
³ Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore.

PMID: 34286998
DOI: 10.1021/acs.jpclett.1c01890

Abstract

Two-dimensional (2D) organic-inorganic hybrid perovskites (OIHPs) with superior nonlinear optical (NLO) properties show great versatility in frequency upconversion applications. Optical anisotropy plays an indispensable role in interpreting the interactions between incoming photons and crystal structure. Recently, the in-plane anisotropic NLO properties of 2D OIHPs have been reported and attracted much attention. However, the structure-related NLO anisotropy of the 2D OIHP framework is not well-established. Here, NLO properties of (C₆H₅(CH₂)₂NH₃)₂PbI₄ (PEPI), (C₆H₁₁NH₃)₂PbI₄ (C6H11), and (C₄H₉NH₃)₂PbI₄ (C4PI) were systematically studied to interrogate the correlation between the in-plane anisotropic NLO responses and its lattice structure. In-plane nonparametric NLO responses, e.g., two-photon photoluminescence (2PPL) and three-photon photoluminescence (3PPL), manifest similar anisotropy configurations for PEPI, C6H11, and C4PI regardless of aromatic, cyclic, or linear organic molecules; however, the anisotropies of THG signals are strongly dependent on the specific crystal structures of the individual flakes, and they are much higher than that of the multiphoton excited photoluminescence.