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Bifurcation of excited state trajectories toward energy transfer or electron transfer directed by wave function symmetry.

Abstract：

:This work explores the concept that differential wave function overlap between excited states can be engineered within a molecular chromophore. The aim is to control excited state wave function symmetries, so that symmetry matches or mismatches result in differential orbital overlap and define low-energy trajectories or kinetic barriers within the excited state surface, that drive excited state population toward different reaction pathways. Two donor-acceptor assemblies were explored, where visible light absorption prepares excited states of different wave function symmetry. These states could be resolved using transient absorption spectroscopy, thanks to wave function symmetry-specific photoinduced optical transitions. One of these excited states undergoes energy transfer to the acceptor, while another undertakes a back-electron transfer to restate the ground state. This differential behavior is possible thanks to the presence of kinetic barriers that prevent excited state equilibration. This strategy can be exploited to avoid energy dissipation in energy conversion or photoredox catalytic schemes.

journal_name

Proc Natl Acad Sci U S A

journal_title

Proceedings of the National Academy of Sciences of the United States of America

authors

Oviedo PS,Baraldo LM,Cadranel A

doi

10.1073/pnas.2018521118

subject

Has Abstract

pub_date

2021-01-26 00:00:00

issue

4

eissn

0027-8424

issn

1091-6490

pii

2018521118

journal_volume

118

pub_type

杂志文章

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