Dual‐Stimuli‐Responsive Photoluminescence of Enantiomeric Two‐Dimensional Lead Halide Perovskites.

2D hybrid organic–inorganic perovskites (HOIPs) are highly responsive to external stimuli and therefore have application potential as sensing materials. Though their optical properties upon singular thermal or pressure stimulation have been recently investigated, their dual‐stimuli‐responsive behaviors have not yet been explored. Here, the dual‐stimuli‐responsive luminescence of a pair of new enantiomeric 2D Dion–Jacobson HOIPs, R+[(4‐aminophenyl)ethylamine]PbI4 and S‐[(4‐aminophenyl)ethylamine]PbI4, is reported. The photoluminescence results show that their 485 nm emissions can be red‐shifted by ≈6 nm upon heating, and further increased to 529 nm under pressure. Such dual‐stimuli‐responsive emissions expand their Commission Internationale de L'Eclairage coordinates successively from (0.140, 0.272) to (0.283, 0.473). Detailed structural analysis and first principles calculations reveal that the temperature‐ and pressure‐responsive behaviors arise from the predominant electron–phonon interactions over thermal expansion effect and pressure‐induced in‐plane PbI bond contraction, respectively. The findings open up a new pathway to successively tune the optical emission of 2D HOIPs via a dual‐stimuli‐responsive approach. [ABSTRACT FROM AUTHOR]