Liu Shangpu, Kepenekian Mikaël, Bodnar Stanislav, Feldmann Sascha, Heindl Markus W, Fehn Natalie, Zerhoch Jonathan, Shcherbakov Andrii, Pöthig Alexander, Li Yang, Paetzold Ulrich W, Kartouzian Aras, Sharp Ian D, Katan Claudine, Even Jacky, Deschler Felix
Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 229, 69120 Heidelberg, Germany.
Walter Schottky Institute and Physics Department, Technical University of Munich, Am Coulombwall 4, 85748 Garching, Germany.
Sci Adv. 2023 Sep;9(35):eadh5083. doi: 10.1126/sciadv.adh5083. Epub 2023 Sep 1.
Hybrid perovskite semiconductor materials are predicted to lock chirality into place and encode asymmetry into their electronic states, while softness of their crystal lattice accommodates lattice strain to maintain high crystal quality with low defect densities, necessary for high luminescence yields. We report photoluminescence quantum efficiencies as high as 39% and degrees of circularly polarized photoluminescence of up to 52%, at room temperature, in the chiral layered hybrid lead-halide perovskites (R/S/Rac)-3BrMBAPbI [3BrMBA = 1-(3-bromphenyl)-ethylamine]. Using transient chiroptical spectroscopy, we explain the excellent photoluminescence yields from suppression of nonradiative loss channels and high rates of radiative recombination. We further find that photoexcitations show polarization lifetimes that exceed the time scales of radiative decays, which rationalize the high degrees of polarized luminescence. Our findings pave the way toward high-performance solution-processed photonic systems for chiroptical applications and chiral-spintronic logic at room temperature.
预计混合钙钛矿半导体材料能够将手性固定到位,并将不对称性编码到其电子态中,而其晶格的柔软性能够适应晶格应变,以保持高质量的晶体且缺陷密度低,这对于高发光产率是必要的。我们报道了在室温下,手性层状混合卤化铅钙钛矿(R/S/Rac)-3BrMBAPbI [3BrMBA = 1-(3-溴苯基)乙胺] 的光致发光量子效率高达39%,圆偏振光致发光度高达52%。通过瞬态手性光谱,我们解释了通过抑制非辐射损失通道和高辐射复合率而实现的优异光致发光产率。我们进一步发现,光激发显示出的偏振寿命超过了辐射衰变的时间尺度,这解释了高偏振发光度的原因。我们的研究结果为室温下用于手性光学应用和手性自旋电子逻辑的高性能溶液处理光子系统铺平了道路。