Photoinduced Ultrafast Multielectron Transfer and Long-lived Charge-accumulated State in a Fullerene-indacenodithiophene Dumbbell Triad

Overview

Journal Proc Natl Acad Sci U S A

Specialty Science

Date 2024 Dec 5

PMID 39636861

Authors

Chong Wang

Bo Wu

Yang Li

Ying Jiang

Tianyang Dong

Shen Zhou

Chunru Wang

Chunli Bai

Affiliations

Soon will be listed here.

Abstract

Photoinduced ultrafast multielectron transfer (m-ET) and long-lived charge-accumulated states in single molecules hold promise for light-energy conversion and utilization. However, compared to single-electron transfer (s-ET), m-ET tends to be thermodynamically and kinetically unfavorable. Here, we construct a dumbbell-shaped fullerene-indacenodithiophene triad, , modified with two C units in the donor indacenodithiophene. Exciting the C units, ultrafast m-ET occurs with a time constant of 0.5 ps, accumulating two holes with a lifetime of 10 μs. Benefitting from a larger driving force, lower reorganization energy, and smaller structural changes, the rate of m-ET is 23 times faster than that of s-ET, and the lifetime of the m-ET product is 1.4 × 10 times longer than that of the s-ET products. These attributes endow with superior photocatalytic performance in multielectron oxidation reactions. This is an instance of achieving faster m-ET and a longer m-ET product lifetime than s-ET in a single molecule. This finding provides unique insights for the construction and application of intramolecular m-ET and charge accumulation systems in photocatalysis and molecular devices.

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