Marcus inverted region of charge transfer from low-dimensional semiconductor materials

Junhui Wang, Tao Ding, Kaimin Gao, Lifeng Wang, Panwang Zhou and Kaifeng Wu ()
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Junhui Wang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Tao Ding: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Kaimin Gao: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Lifeng Wang: Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Panwang Zhou: Shandong University
Kaifeng Wu: Dalian Institute of Chemical Physics, Chinese Academy of Sciences

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

Abstract: Abstract A key process underlying the application of low-dimensional, quantum-confined semiconductors in energy conversion is charge transfer from these materials, which, however, has not been fully understood yet. Extensive studies of charge transfer from colloidal quantum dots reported rates increasing monotonically with driving forces, never displaying an inverted region predicted by the Marcus theory. The inverted region is likely bypassed by an Auger-like process whereby the excessive driving force is used to excite another Coulomb-coupled charge. Herein, instead of measuring charge transfer from excitonic states (coupled electron-hole pairs), we build a unique model system using zero-dimensional quantum dots or two-dimensional nanoplatelets and surface-adsorbed molecules that allows for measuring charge transfer from transiently-populated, single-charge states. The Marcus inverted region is clearly revealed in these systems. Thus, charge transfer from excitonic and single-charge states follows the Auger-assisted and conventional Marcus charge transfer models, respectively. This knowledge should enable rational design of energetics for efficient charge extraction from low-dimensional semiconductor materials as well as suppression of the associated energy-wasting charge recombination.

Date: 2021
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DOI: 10.1038/s41467-021-26705-x

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