Ultrafast Spin Relaxation of Charge Carriers in Strongly Quantum Confined Methylammonium Lead Bromide Perovskite Magic-Sized Clusters

IF 3.7 Q2 CHEMISTRY, PHYSICAL ACS Physical Chemistry Au Pub Date : 2024-09-16 DOI:10.1021/acsphyschemau.4c00051
David C. Zeitz, Vivien L. Cherrette, Sarah A. Creech, Yan Li, Yuan Ping, Jin Z. Zhang
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Abstract

Spin relaxation of charge carriers in strongly quantum confined perovskite magic-sized clusters has been probed, for the first time, by using polarization-controlled femtosecond transient absorption (fs-TA) spectroscopy. Fs-TA measurements with a circularly polarized pump and probe allowed for the determination of the exciton spin relaxation lifetime (∼1.5 ps) at room temperature based on the dynamics of a photoinduced absorption (PIA) feature peaked at 458 nm. This spin lifetime is shorter than that of perovskite quantum dots (PQDs) with a larger size, and the results suggest that exciton confinement and defects likely play a more important role in these strongly quantum confined magic-sized clusters with a larger surface-to-volume ratio.

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强量子约束的甲基溴化铅过氧化物魔型簇中电荷载流子的超快自旋弛豫
利用偏振控制飞秒瞬态吸收(fs-TA)光谱学,首次探测了强量子约束包晶魔法尺寸团簇中电荷载流子的自旋弛豫。利用圆极化泵浦和探针进行飞秒瞬态吸收测量,可以根据在 458 纳米波长处达到峰值的光诱导吸收(PIA)特征的动态,确定激子在室温下的自旋弛豫寿命(1.5 ps)。这一自旋寿命比尺寸更大的过氧化物量子点(PQDs)更短,结果表明激子约束和缺陷可能在这些具有更大表面体积比的强量子约束魔法尺寸团簇中发挥了更重要的作用。
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期刊介绍: ACS Physical Chemistry Au is an open access journal which publishes original fundamental and applied research on all aspects of physical chemistry. The journal publishes new and original experimental computational and theoretical research of interest to physical chemists biophysical chemists chemical physicists physicists material scientists and engineers. An essential criterion for acceptance is that the manuscript provides new physical insight or develops new tools and methods of general interest. Some major topical areas include:Molecules Clusters and Aerosols; Biophysics Biomaterials Liquids and Soft Matter; Energy Materials and Catalysis
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Issue Publication Information Issue Editorial Masthead Roundabout Mechanism of Ion–Molecule Nucleophilic Substitution Reactions Ultrafast Spin Relaxation of Charge Carriers in Strongly Quantum Confined Methylammonium Lead Bromide Perovskite Magic-Sized Clusters Direct Detection of Bound Water in Hydrated Powders of Lysozyme by Differential Scanning Calorimetry
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