The flexible organic amine cations on the interfaces of two-dimensional (2D) hybrid organic− inorganic perovskite nanosheets could form relaxed structures, which would lead to exotic optoelectronic properties but are hard to understand. Here, the unusual interfacial relaxation of nanosheets exfoliated from an o r t h o r h o m b i c 2 D l e a d h a l i d e p e r o v s k i t e , [(C 6 H 5 CH 2 NH 3 ) 2 ]PbCl 4 , is interrogated via ultrafast second-harmonic generation (SHG) spectroscopy. The in-plane SHG intensity anisotropy of these nanosheets is found to decrease with reducing layer thickness. Combined first-principles calculations and Monte Carlo simulations reveal that the induced second-order polarization arises primarily from the (C 6 H 5 CH 2 NH 3 ) + cations; and these organic amine cations form significantly reorganized conformations with decreasing nanosheet thickness due to weakened van der Waals interactions. Because the orientations of organic components at the interface determine their electric properties and specifically the dipolar susceptibility, the resulting structure leads to striking changes in the SHG properties.
The fundamental electronic structures and elastic properties of a family of metal-free perovskites were systematically investigated using a combined theoretical-experimental approach.
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