Chiral Perovskite Heterostructure Films of CsPbBr3 Quantum Dots and 2D Chiral Perovskite with Circularly Polarized Luminescence Performance and Energy Transfer.

This work reports the synthesis of chiral perovskite heterostructure films by combining a two-dimensional (2D) chiral (R-/S-MBA)2PbI4 perovskite with CsPbBr3 quantum dots (QDs). The as-synthesized chiral heterostructure films exhibit obvious circularly polarized luminescence (CPL) properties, even though pure 2D chiral perovskite cannot present photoluminescence. It indicates that the chirality of the excited state of the QDs originates from the 2D chiral perovskite. The circular polarization-resolved transient absorption (TA) spectra further demonstrate that the CPL response of heterostructure films originates from the energy transfer between the chiral perovskite layer and QDs layer and the suppression of spin relaxation, which induces the imbalance of the spin population of excited states in QDs layer. In addition, the photoluminescence (PL), circular dichroism (CD), and CPL spectra of these heterostructure films can be controlled by varying the thickness and component of the chiral perovskite layer, which demonstrates that the anion exchange between chiral perovskite and CsPbBr3 QDs can tune the chemical composition and optoelectronic properties due to the low bonding energy difference between them and decrease the strain within the QDs layer to reduce the radiative recombination lifetime. This work provides guidance for the synthesis of chiral perovskites with a strong CPL response and further provides insight into the origination of CPL.

The Role of Polaronic States on the Spin Dynamics in Solution-Processed Two-Dimensional Layered Perovskite with Different Layer Thickness.

2D lead halide perovskites (LHPs) show strong excitonic and spin-orbit coupling effects, generating a facile spin injection. Besides, they possess a polaron character due to the soft crystal lattice, which can prolong the spin lifetime, making them favorable materials for spintronic applications. Here, the spin dynamics of 2D PEA2 PbI4 (MAPbI3 )n -l thin films with different layers by temperature- and pump fluence-dependent circularly polarization-resolved transient absorption (TA) measurements is studied. These results indicate that the spin depolarization mechanism is gradually converted from the Maialle-Silva-Sham (MSS) mechanism to the polaronic states protection mechanism with the layer number increasing from = 1 to 3, which is determined by the interplay between the strength of Coulomb exchange interaction and the strength of polaronic effect. While for ≥ 4, the Elliot-Yafet (EY) impurities mechanism is proposed, in which the formed polaronic states with free charge carriers no longer play the protective role.

Exciton-Phonon Coupling of Chiral One-Dimensional Lead-Free Hybrid Metal Halides at Room Temperature.

The interaction between organic cations and inorganic metal halide octahedral units strongly affects the properties of organic-inorganic hybrid metal halides. The "soft" property of the lattice provides the possibility of its strong exciton-phonon interaction. Here we report one-dimensional (1D) lead-free chiral organic-inorganic hybrid metal halide single crystals of (R/S)-methylbenzylamine bismuth iodide (R/S-MBA)2Bi2I8, which exhibits a high level of octahedral bond distortion. The introduction of chiral amines leads to a strong chiroptical response in the range of 200-600 nm. The strong exciton-phonon coupling can be observed through the coherent oscillation spectrum of transient absorption dynamics at room temperature. The coherent phonon oscillation frequencies are ∼97 and ∼130 cm-1, corresponding to the symmetrical stretching or bending of the Bi-I octahedron. Our work provides new insights for the study of exciton-phonon coupling in 1D chiral hybrid metal halides.