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Two Regimes of Bandgap Red Shift and Partial Ambient Retention in Pressure-Treated Two-Dimensional Perovskites
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-10-09 00:00:00 , DOI: 10.1021/acsenergylett.7b00807 Gang Liu 1, 2 , Lingping Kong 1, 2 , Peijun Guo 3 , Constantinos C. Stoumpos 4 , Qingyang Hu 1 , Zhenxian Liu 2 , Zhonghou Cai 5 , David J. Gosztola 3 , Ho-kwang Mao 1, 2 , Mercouri G. Kanatzidis 4 , Richard D. Schaller 3, 4
ACS Energy Letters ( IF 19.3 ) Pub Date : 2017-10-09 00:00:00 , DOI: 10.1021/acsenergylett.7b00807 Gang Liu 1, 2 , Lingping Kong 1, 2 , Peijun Guo 3 , Constantinos C. Stoumpos 4 , Qingyang Hu 1 , Zhenxian Liu 2 , Zhonghou Cai 5 , David J. Gosztola 3 , Ho-kwang Mao 1, 2 , Mercouri G. Kanatzidis 4 , Richard D. Schaller 3, 4
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The discovery of elevated environmental stability in two-dimensional (2D) Ruddlesden–Popper hybrid perovskites represents a significant advance in low-cost, high-efficiency light absorbers. In comparison to 3D counterparts, 2D perovskites of organo-lead-halides exhibit wider, quantum-confined optical bandgaps that reduce the wavelength range of light absorption. Here, we characterize the structural and optical properties of 2D hybrid perovskites as a function of hydrostatic pressure. We observe bandgap narrowing with pressure of 633 meV that is partially retained following pressure release due to an atomic reconfiguration mechanism. We identify two distinct regimes of compression dominated by the softer organic and less compressible inorganic sublattices. Our findings, which also include PL enhancement, correlate well with density functional theory calculations and establish structure–property relationships at the atomic scale. These concepts can be expanded into other hybrid perovskites and suggest that pressure/strain processing could offer a new route to improved materials-by-design in applications.
中文翻译：
压力处理的二维钙钛矿中带隙红移和部分环境保留的两种状态
在二维（2D）Ruddlesden-Popper混合钙钛矿中发现提高的环境稳定性代表了低成本，高效率光吸收剂的重大进步。与3D对应物相比，有机铅卤化物的2D钙钛矿具有更宽的量子限制光学带隙，可减小光吸收的波长范围。在这里，我们将2D杂化钙钛矿的结构和光学特性表征为静水压力的函数。我们观察到由于原子重构机制，随着压力释放，在633 meV的压力下能带隙变窄。我们确定了两种不同的压缩方式，它们由较软的有机和较难压缩的无机亚晶格主导。我们的发现，其中还包括PL增强，与密度泛函理论计算紧密相关，并在原子尺度上建立结构与性质的关系。这些概念可以扩展到其他钙钛矿杂化材料中，这表明压力/应变处理可以为在设计中通过设计改进材料提供一条新途径。
更新日期：2017-10-09
中文翻译：
压力处理的二维钙钛矿中带隙红移和部分环境保留的两种状态
在二维（2D）Ruddlesden-Popper混合钙钛矿中发现提高的环境稳定性代表了低成本，高效率光吸收剂的重大进步。与3D对应物相比，有机铅卤化物的2D钙钛矿具有更宽的量子限制光学带隙，可减小光吸收的波长范围。在这里，我们将2D杂化钙钛矿的结构和光学特性表征为静水压力的函数。我们观察到由于原子重构机制，随着压力释放，在633 meV的压力下能带隙变窄。我们确定了两种不同的压缩方式，它们由较软的有机和较难压缩的无机亚晶格主导。我们的发现，其中还包括PL增强，与密度泛函理论计算紧密相关，并在原子尺度上建立结构与性质的关系。这些概念可以扩展到其他钙钛矿杂化材料中，这表明压力/应变处理可以为在设计中通过设计改进材料提供一条新途径。
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