Uncovering temperature-dependent exciton-polariton relaxation mechanisms in hybrid organic-inorganic perovskites

被引:24
作者
Laitz, Madeleine [1 ]
Kaplan, Alexander E. K. [2 ]
Deschamps, Jude [2 ]
Barotov, Ulugbek [2 ]
Proppe, Andrew H. [2 ]
Garcia-Benito, Ines [3 ]
Osherov, Anna [1 ]
Grancini, Giulia [4 ,5 ]
deQuilettes, Dane W. [6 ]
Nelson, Keith A. [2 ]
Bawendi, Moungi G. [2 ]
Bulovic, Vladimir [1 ]
机构
[1] MIT, Dept Elect Engn & Comp Sci, Cambridge, MA 02142 USA
[2] MIT, Dept Chem, Cambridge, MA USA
[3] Univ Complutense Madrid, Dept Organ Chem, Madrid, Spain
[4] Univ Pavia, Dept Chem, Pavia, Italy
[5] Univ Pavia, INSTM, Pavia, Italy
[6] MIT, Res Lab Elect, Cambridge, MA 02139 USA
基金
美国国家科学基金会; 加拿大自然科学与工程研究理事会; 欧洲研究理事会;
关键词
FINE-STRUCTURE; SPIN-FLIP; MICROCAVITY; DYNAMICS;
D O I
10.1038/s41467-023-37772-7
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Hybrid perovskites have emerged as a promising material candidate for exciton-polariton (polariton) optoelectronics. Thermodynamically, low-threshold Bose-Einstein condensation requires efficient scattering to the polariton energy dispersionminimum, and many applications demand precise control of polariton interactions. Thus far, the primary mechanisms by which polaritons relax in perovskites remains unclear. In this work, we perform temperature-dependent measurements of polaritons in low-dimensional perovskite wedged microcavities achieving a Rabi splitting of (sic)Omega Rabi = 260 +/- 5meV. We change the Hopfield coefficients by moving the optical excitation along the cavity wedge and thus tune the strength of the primary polariton relaxation mechanisms in this material. We observe the polariton bottleneck regime and show that it can be overcome by harnessing the interplay between the different excitonic species whose corresponding dynamics are modified by strong coupling. This work provides an understanding of polariton relaxation in perovskites benefiting from efficient, material-specific relaxation pathways and intracavity pumping schemes from thermally brightened excitonic species.
引用
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页数:11
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