Crossover between the adiabatic and nonadiabatic electron transfer limits in the Landau-Zener model

Guang Yuan Zhu, Yi Qin, Miao Meng, Suman Mallick, Hang Gao, Xiaoli Chen, Tao Cheng, Ying Ning Tan, Xuan Xiao, Mei Juan Han, Mei Fang Sun and Chun Y. Liu ()
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Guang Yuan Zhu: Jinan University
Yi Qin: Jinan University
Miao Meng: Jinan University
Suman Mallick: Jinan University
Hang Gao: Jinan University
Xiaoli Chen: Jinan University
Tao Cheng: Jinan University
Ying Ning Tan: Jinan University
Xuan Xiao: Jinan University
Mei Juan Han: Jinan University
Mei Fang Sun: Jinan University
Chun Y. Liu: Jinan University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract The semiclassical models of nonadiabatic transition were proposed first by Landau and Zener in 1932, and have been widely used in the study of electron transfer (ET); however, experimental demonstration of the Landau-Zener formula remains challenging to observe. Herein, employing the Hush-Marcus theory, thermal ET in mixed-valence complexes {[Mo2]-(ph)n-[Mo2]}+ (n = 1–3) has been investigated, spanning the nonadiabatic throughout the adiabatic limit, by analysis of the intervalence transition absorbances. Evidently, the Landau-Zener formula is valid in the adiabatic regime in a broader range of conditions than the theoretical limitation known as the narrow avoided-crossing. The intermediate system is identified with an overall transition probability (κel) of ∼0.5, which is contributed by the single and the first multiple passage. This study shows that in the intermediate regime, the ET kinetic results derived from the adiabatic and nonadiabatic formalisms are nearly identical, in accordance with the Landau-Zener model. The obtained insights help to understand and control the ET processes in biological and chemical systems.

Date: 2021
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DOI: 10.1038/s41467-020-20557-7

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