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Chiral Nonlinear Optical Response in Achiral Quasi-2D Perovskite Ferroelectric Featuring Unusually Large A-Site

Chang-Chun Fan^1,2, Shu-Lin Jiao³, Qiang-Qiang Bi²

¹School of Materials Engineering, Jinling Institute of Technology, Nanjing, China.

Angewandte Chemie (International Ed. in English)

|March 16, 2026

Abstract

None:

The exploration of 2D perovskites and chiral nonlinear optical materials has drawn significant interest due to their structural tunability and strong optical responses. However, the development of quasi-2D perovskites has long been constrained by the limited choice of A-site cations imposed by the traditional tolerance factor. In this study, we present a new 2D tri-layered lead bromide perovskite (4AM)₄Pb₃Br₁₀ (n = 3) with the general formula (A^')₂(A)_n _-1M_nX₃ _n ₊₁, in which 4-aminomonpholine cations (4AM) that act simultaneously as A-site and spacer components, exhibiting an ultrahigh tolerance factor of 1.74-far beyond conventional limits. Crystallizing in the polar space group Cc, the compound shows an order-disorder ferroelectric phase transition at 418 K. Interestingly it also exhibits notable chiral nonlinear optical properties, including strong second-harmonic generation circular dichroism (g_SHG-CD ≈ 0.63). This work breaks the classic tolerance factor constraint and opens a pathway for designing new chiral nonlinear optical materials in low-dimensional perovskites.

Keywords:

chiral nonlinear optical response molecule‐based ferroelectric quasi‐2D perovskite

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