Wang Yuan, Song Mu-Sen, Zhao Jiaqi, Li Zhen, Wang Tinglei, Wang Hai, Wang Hai-Yu, Wang Yu
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
State Key Laboratory of Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.
ACS Nano. 2024 Aug 20;18(33):22334-22343. doi: 10.1021/acsnano.4c06631. Epub 2024 Aug 9.
This work reports the synthesis of chiral perovskite heterostructure films by combining a two-dimensional (2D) chiral (R-/S-MBA)PbI perovskite with CsPbBr 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 CsPbBr 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.
这项工作报道了通过将二维(2D)手性(R-/S-MBA)PbI钙钛矿与CsPbBr量子点(QDs)相结合来合成手性钙钛矿异质结构薄膜。所合成的手性异质结构薄膜表现出明显的圆偏振发光(CPL)特性,尽管纯的二维手性钙钛矿无法呈现光致发光。这表明量子点激发态的手性源自二维手性钙钛矿。圆偏振分辨瞬态吸收(TA)光谱进一步证明,异质结构薄膜的CPL响应源自手性钙钛矿层与量子点层之间的能量转移以及自旋弛豫的抑制,这导致量子点层中激发态自旋布居的不平衡。此外,这些异质结构薄膜的光致发光(PL)、圆二色性(CD)和CPL光谱可以通过改变手性钙钛矿层的厚度和组分来控制,这表明手性钙钛矿与CsPbBr量子点之间的阴离子交换能够调节化学成分和光电性质,因为它们之间的键能差较低,并且能够降低量子点层内的应变以缩短辐射复合寿命。这项工作为合成具有强CPL响应的手性钙钛矿提供了指导,并进一步深入了解了CPL的起源。