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The quantum-confined Stark effect in layered hybrid perovskites mediated by orientational polarizability of confined dipoles

机译:受限偶极子的定向极化率介导的层状混杂钙钛矿中的量子限制斯塔克效应

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摘要

The quantum-confined Stark effect (QCSE) is an established optical modulation mechanism, yet top-performing modulators harnessing it rely on costly fabrication processes. Here, we present large modulation amplitudes for solution-processed layered hybrid perovskites and a modulation mechanism related to the orientational polarizability of dipolar cations confined within these self-assembled quantum wells. We report an anomalous (blue-shifting) QCSE for layers that contain methylammonium cations, in contrast with cesium-containing layers that show normal (red-shifting) behavior. We attribute the blue-shifts to an extraordinary diminution in the exciton binding energy that arises from an augmented separation of the electron and hole wavefunctions caused by the orientational response of the dipolar cations. The absorption coefficient changes, realized by either the red- or blue-shifts, are the strongest among solution-processed materials at room temperature and are comparable to those exhibited in the highest-performing epitaxial compound semiconductor heterostructures.
机译:量子限制斯塔克效应(QCSE)是一种已建立的光学调制机制,但利用它的性能最佳的调制器则依赖于昂贵的制造工艺。在这里,我们提出了溶液处理的层状混合钙钛矿的大调制幅度,以及与局限在这些自组装量子阱中的偶极阳离子的取向极化率有关的调制机制。我们报告了含有甲基铵阳离子层的异常(蓝移)QCSE,与显示正常(红移)行为的含铯层相反。我们将蓝移归因于激子结合能的异常减少,这是由于偶极阳离子的定向响应引起的电子和空穴波函数的分离增加而引起的。通过红移或蓝移实现的吸收系数变化在室温下是固溶处理材料中最强的,并且与表现最高的外延化合物半导体异质结构中的吸收系数变化相当。

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