期刊
NANO LETTERS
卷 20, 期 8, 页码 5678-5685出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c00867
关键词
2D perovskites; many body interactions; spin; exciton; total angular momentum; transient absorption spectroscopy
类别
资金
- EPSRC Centre for Doctoral Training in Graphene Technology [EP/L016087/1]
- EPSRC project Strategic University Network to Revolutionise Indian Solar Energy-SUNRISE [EP/P032591/1]
- Royal Society Newton-Bhabha International Fellowship
- Royal Society
- Engineering and Physical Sciences Research Council (EPSRC) [EP/M005143/1]
- Newton International Fellowship Alumni funding [AL\191021]
- Studienstiftung des deutschen Volkes
- EPSRC
- Winton Programme for the Physics of Sustainability
- EPSRC Cambridge NanoDTC [EP/L015978/1]
- Cambridge Trust
- Inlaks Shivdasani Foundation
- Marie Curie actions [H2020-MSCA-IF-2018841356]
- Winton Advanced Research Fellowship
- DFG Emmy Noether Program
- EPSRC NI grant [EP/R044481/1]
- EPSRC [EP/P032591/1, EP/M005143/1, EP/M000524/1] Funding Source: UKRI
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.
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