Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling
Organic-to-inorganic structural chirality transfer in a 2D hybrid perovskite and impact on Rashba-Dresselhaus spin-orbit coupling
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DOI：
10.1038/s41467-020-18485-7
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发表时间：
2020-09-17
影响因子：
16.6
通讯作者：
Mitzi, David B.
中科院分区：
文献类型：
--
作者：
Jana, Manoj K.;Song, Ruyi;Mitzi, David B.
手性和不对称性在结构基序和长度尺度上的翻译在自然界中起着重要作用，在从生物系统到合成材料的各种环境中实现了独特的功能。在这里，我们介绍了一个结构手性转移的有机-无机界面在二维混合钙钛矿使用适当的手性有机阳离子。手性间隔基阳离子R-（+）-或S-（-）-1-（1-萘基）乙基铵的优选分子构型以及它们与溴化铅基层的不对称氢键相互作用导致无机层中的螺旋破坏性螺旋扭曲，否则当采用有机间隔基的外消旋混合物时不存在。第一性原理模型预测了大量的散装Rashba-Dresselhaus自旋分裂的无机衍生的导带与相反的自旋纹理之间的R-和S-杂化由于破坏反转对称性和强的自旋轨道耦合。使用从一个结构单元到另一个结构单元的手性转移来打破对称性的能力提供了用于涌现性质的合成设计范例，包括用于混合钙钛矿自旋电子学和相关应用的Rashba-Dresselhaus自旋极化。
Translation of chirality and asymmetry across structural motifs and length scales plays a fundamental role in nature, enabling unique functionalities in contexts ranging from biological systems to synthetic materials. Here, we introduce a structural chirality transfer across the organic-inorganic interface in two-dimensional hybrid perovskites using appropriate chiral organic cations. The preferred molecular configuration of the chiral spacer cations, R-(+)- or S-(-)-1-(1-naphthyl)ethylammonium and their asymmetric hydrogen-bonding interactions with lead bromide-based layers cause symmetry-breaking helical distortions in the inorganic layers, otherwise absent when employing a racemic mixture of organic spacers. First-principles modeling predicts a substantial bulk Rashba-Dresselhaus spin-splitting in the inorganic-derived conduction band with opposite spin textures between R- and S-hybrids due to the broken inversion symmetry and strong spin-orbit coupling. The ability to break symmetry using chirality transfer from one structural unit to another provides a synthetic design paradigm for emergent properties, including Rashba-Dresselhaus spin-polarization for hybrid perovskite spintronics and related applications.