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

来源：

NANO LETTERS | 2020年 / 20卷 / 08期

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

页码：5678 / 5685

页数：8

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