Shallow distance-dependent triplet energy migration mediated by endothermic charge-transfer

Runchen Lai, Yangyi Liu, Xiao Luo, Lan Chen, Yaoyao Han, Meng Lv, Guijie Liang, Jinquan Chen, Chunfeng Zhang, Dawei Di, Gregory D. Scholes, Felix N. Castellano and Kaifeng Wu ()
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Runchen Lai: Chinese Academy of Sciences
Yangyi Liu: East China Normal University
Xiao Luo: Chinese Academy of Sciences
Lan Chen: Nanjing University
Yaoyao Han: Chinese Academy of Sciences
Meng Lv: East China Normal University
Guijie Liang: Hubei University of Art and Science
Jinquan Chen: East China Normal University
Chunfeng Zhang: Nanjing University
Dawei Di: Zhejiang University
Gregory D. Scholes: Princeton University
Felix N. Castellano: North Carolina State University
Kaifeng Wu: Chinese Academy of Sciences

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Conventional wisdom posits that spin-triplet energy transfer (TET) is only operative over short distances because Dexter-type electronic coupling for TET rapidly decreases with increasing donor acceptor separation. While coherent mechanisms such as super-exchange can enhance the magnitude of electronic coupling, they are equally attenuated with distance. Here, we report endothermic charge-transfer-mediated TET as an alternative mechanism featuring shallow distance-dependence and experimentally demonstrated it using a linked nanocrystal-polyacene donor acceptor pair. Donor-acceptor electronic coupling is quantitatively controlled through wavefunction leakage out of the core/shell semiconductor nanocrystals, while the charge/energy transfer driving force is conserved. Attenuation of the TET rate as a function of shell thickness clearly follows the trend of hole probability density on nanocrystal surfaces rather than the product of electron and hole densities, consistent with endothermic hole-transfer-mediated TET. The shallow distance-dependence afforded by this mechanism enables efficient TET across distances well beyond the nominal range of Dexter or super-exchange paradigms.

Date: 2021
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DOI: 10.1038/s41467-021-21561-1

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