论文标题
通过层厚度的逐步转化,相纯2D钙壶岩的确定性合成
Deterministic synthesis of phase pure 2D perovskites via progressive transformation of layer thickness
论文作者
论文摘要
二维(2D)卤化物钙钛矿已成为半导体平台,用于实现高效且耐用的光电设备。但是,由于缺乏每个层厚度的动力学控制(温度,时间,化学计量),可再现的2D钙钛矿晶体具有所需层厚度(或n值)大于2的层厚度(或n值),这是一个持久的挑战。在这里,我们证明了一个新的方法术语为动力学控制的空间限制(KCSC),用于相位纯ruddlesden-popper(RP)和Dion-Jacobson(DJ)2D Perovskites的确定性生长。通过逐渐增加温度(固定时间)或结晶时间(固定温度)来实现相位的生长,从而可以急性控制结晶动力学。我们还观察到从较低的n值到n = 3、4、5、6的系统转换。原位光发光光谱和成像表明,从下部到更高的N值进行的逐渐转化是通过过量前体离子的插入而发生的。这些实验使机器学习辅助的多参数相图的开发可以预测具有特定N值的2D相的增长。
Two-dimensional (2D) halide perovskites have emerged as semiconductor platforms for realizing efficient and durable optoelectronic devices. However, the reproducible synthesis of 2D perovskite crystals with desired layer thickness (or n value) greater than 2, has been an enduring challenge due to the lack of kinetic control (temperature, time, stoichiometry) for each layer thickness. Here, we demonstrate a novel method term as the kinetically controlled space confinement (KCSC) for the deterministic growth of phase pure Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) 2D perovskites. The phase-pure growth was achieved by progressively increasing the temperature (fixed time) or the crystallization time (fixed temperature), which allowed for an acute control of the crystallization kinetics. We also observe a systematic transformation from a lower n-value to n=3, 4, 5, 6 in 2D perovskites. In-situ photoluminescence spectroscopy and imaging suggest that the progressive transformation from lower to higher n-value occurs via intercalation of excess precursor ions. These experiments enabled the development of a machine learning assisted multi-parameter phase diagram, which predicts the growth of 2D phase with a specific n-value.