How Exciton Interactions Control Spin-Depolarization in Layered Hybrid Perovskites

被引:34
作者
Bourelle, Sean A. [1 ]
Shivanna, Ravichandran [1 ]
Camargo, Franco V. A. [2 ]
Ghosh, Soumen [2 ]
Gillett, Alexander J. [1 ]
Senanayak, Satyaprasad P. [1 ,3 ]
Feldmann, Sascha [1 ]
Eyre, Lissa [1 ,4 ]
Ashoka, Arjun [1 ]
van de Goor, Tim W. J. [1 ]
Abolins, Haralds [1 ]
Winkler, Thomas [1 ]
Cerullo, Giulio [2 ]
Friend, Richard H. [1 ]
Deschler, Felix [4 ]
机构
[1] Univ Cambridge, Cavendish Lab, Cambridge CB3 0HE, England
[2] Politecn Milan, Dipartimento Fis, IFN CNR, I-20133 Milan, Italy
[3] CSIR Inst Minerals & Mat Technol, Bhubaneswar 751013, India
[4] Tech Univ Munich, Walter Schottky Inst, Phys Dept, D-85748 Garching, Germany
基金
英国工程与自然科学研究理事会; 欧盟地平线“2020”;
关键词
2D perovskites; many body interactions; spin; exciton; total angular momentum; transient absorption spectroscopy; LEAD IODIDE PEROVSKITE; SINGLE-CRYSTAL; FREE-CARRIERS; DYNAMICS; RELAXATION; EFFICIENCY;
D O I
10.1021/acs.nanolett.0c00867
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Using circularly polarized broadband transient absorption, time-resolved circular photoluminescence, and transient Faraday rotation spectroscopy, we report that spin-dependent interactions have a significant impact on exciton energies and spin depolarization times in layered Ruddlesden-Popper hybrid metal-halide perovskites. In BA(2)FAPb(2)I(7), we report that room-temperature spin lifetimes are largest (3.2 ps) at a carrier density of similar to 10(17) cm(-3) with increasing depolarization rates at higher exciton densities. This indicates that many-body interactions reduce spin-lifetimes and outcompete the effect of D'yakonov-Perel precessional relaxation that has been previously reported at lower carrier densities. We further observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental and application relevant insights into the spin-dependent exciton-exciton interactions in layered hybrid perovskites.
引用
收藏
页码:5678 / 5685
页数:8
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