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Strong Rashba-Dresselhaus Effect in Nonchiral 2D Ruddlesden-Popper Perovskites
Advanced Optical Materials ( IF 8.0 ) Pub Date : 2021-10-18 , DOI: 10.1002/adom.202101232 Minh T. Pham 1 , Eric Amerling 2 , Tu Anh Ngo 1 , Hoang M. Luong 1 , Kameron Hansen 2 , Huy T. Pham 3 , Tuoc N. Vu 4 , Huan Tran 5 , Luisa Whittaker‐Brooks 2 , Tho D. Nguyen 1
Advanced Optical Materials ( IF 8.0 ) Pub Date : 2021-10-18 , DOI: 10.1002/adom.202101232 Minh T. Pham 1 , Eric Amerling 2 , Tu Anh Ngo 1 , Hoang M. Luong 1 , Kameron Hansen 2 , Huy T. Pham 3 , Tuoc N. Vu 4 , Huan Tran 5 , Luisa Whittaker‐Brooks 2 , Tho D. Nguyen 1
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Chirality transfer from organic chiral molecules to lead halides is theorized as the origin of the strong Rashba-Dresselhaus effect causing large circular dichroism (CD) and circularly polarized luminescence (CPL) in metal halide perovskites (MHPs). Here, a concrete empirical evidence is provided that such strong CD and CPL can occur even in nonchiral 2D Ruddlesden-Popper perovskites (RPPs) (BA)2(MA)n−1PbnI3n+1 (where MA = CH3NH3 and BA = CH3(CH2)3NH3). The CD and CPL responses occurring at the excitonic transition of the MHPs are strongest (≈100 mdeg and 4.8%, respectively) when a single lead halide octahedral [PbI6]4− layer is repeatedly stacked between two nonchiral molecules BA+ (n = 1). However, they are rapidly quenched as n increases. It is hypothesized that strong Rashba-Dresselhaus splitting in the 2D RPPs originates the strong CD and CPL signatures. Density functional theory calculations reveal that the large interlayer distortions in the inorganic layers at the organic/inorganic interface give rise to the strong Rashba-Dresselhaus splitting. A Rashba-Dresselhaus field of ≈600 and ≈50 mT for n = 1 and 2, respectively, is estimated by magnetic circular dichroism spectroscopy. The studies may have significant impact on designing 2D RPPs with large Rashba-Dresselhaus effects at room temperature for spintronic applications.
中文翻译：
非手性二维 Ruddlesden-Popper 钙钛矿中的强 Rashba-Dresselhaus 效应
从有机手性分子到卤化铅的手性转移被认为是强 Rashba-Dresselhaus 效应的起源，导致金属卤化物钙钛矿 (MHP) 中的大圆二色性 (CD) 和圆偏振发光 (CPL)。在这里，提供了一个具体的经验证据，即使在非手性二维 Ruddlesden-Popper 钙钛矿 (RPP) (BA) 2 (MA) n -1 Pb n I 3 n +1（其中 MA = CH 3 NH 3和BA = CH 3 (CH 2 ) 3 NH 3）。当单个卤化铅八面体 [PbI 6 ] 4−层在两个非手性分子 BA + ( n = 1）。然而，随着n 的增加，它们会迅速淬火。假设二维 RPP 中的强 Rashba-Dresselhaus 分裂源于强 CD 和 CPL 特征。密度泛函理论计算表明，有机/无机界面处无机层的大层间变形导致强烈的 Rashba-Dresselhaus 分裂。≈600 和 ≈50 mT 的 Rashba-Dresselhaus 场，对于n = 1 和 2 分别是通过磁圆二色光谱估计的。这些研究可能对在室温下为自旋电子应用设计具有大 Rashba-Dresselhaus 效应的 2D RPP 产生重大影响。
更新日期：2021-10-18
中文翻译：
非手性二维 Ruddlesden-Popper 钙钛矿中的强 Rashba-Dresselhaus 效应
从有机手性分子到卤化铅的手性转移被认为是强 Rashba-Dresselhaus 效应的起源，导致金属卤化物钙钛矿 (MHP) 中的大圆二色性 (CD) 和圆偏振发光 (CPL)。在这里，提供了一个具体的经验证据，即使在非手性二维 Ruddlesden-Popper 钙钛矿 (RPP) (BA) 2 (MA) n -1 Pb n I 3 n +1（其中 MA = CH 3 NH 3和BA = CH 3 (CH 2 ) 3 NH 3）。当单个卤化铅八面体 [PbI 6 ] 4−层在两个非手性分子 BA + ( n = 1）。然而，随着n 的增加，它们会迅速淬火。假设二维 RPP 中的强 Rashba-Dresselhaus 分裂源于强 CD 和 CPL 特征。密度泛函理论计算表明，有机/无机界面处无机层的大层间变形导致强烈的 Rashba-Dresselhaus 分裂。≈600 和 ≈50 mT 的 Rashba-Dresselhaus 场，对于n = 1 和 2 分别是通过磁圆二色光谱估计的。这些研究可能对在室温下为自旋电子应用设计具有大 Rashba-Dresselhaus 效应的 2D RPP 产生重大影响。
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