Real-time observation of two distinctive non-thermalized hot electron dynamics at MXene/molecule interfaces

Qi Zhang, Wei Li, Ruixuan Zhao, Peizhe Tang, Jie Zhao, Guorong Wu, Xin Chen, Mingjun Hu, Kaijun Yuan (), Jiebo Li () and Xueming Yang
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Qi Zhang: Beihang University
Wei Li: Suzhou Laboratory
Ruixuan Zhao: Beihang University
Peizhe Tang: Beihang University
Jie Zhao: Chinese Academy of Sciences
Guorong Wu: Chinese Academy of Sciences
Xin Chen: Suzhou Laboratory
Mingjun Hu: Beihang University
Kaijun Yuan: Chinese Academy of Sciences
Jiebo Li: Beihang University
Xueming Yang: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract The photoinduced non-thermalized hot electrons at an interface play a pivotal role in determining plasmonic driven chemical events. However, understanding non-thermalized electron dynamics, which precedes electron thermalization (~125 fs), remains a grand challenge. Herein, we simultaneously captured the dynamics of both molecules and non-thermalized electrons in the MXene/molecule complexes by femtosecond time-resolved spectroscopy. The real-time observation allows for distinguishing non-thermalized and thermalized electron responses. Differing from the thermalized electron/heat transfer, our results reveal two non-thermalized electron dynamical pathways: (i) the non-thermalized electrons directly transfer to attached molecules at an interface within 50 fs; (ii) the non-thermalized electrons scatter at the interface within 125 fs, inducing adsorbed molecules heating. These two distinctive pathways are dependent on the irradiating wavelength and the energy difference between MXene and adsorbed molecules. This research sheds light on the fundamental mechanism and opens opportunities in photocatalysis and interfacial heat transfer theory.

Date: 2024
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DOI: 10.1038/s41467-024-48842-9

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