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Molecular orbital node engineering in pyrene: linking chemical reactivity with room-temperature phosphorescence.

Created on 13 Sep 2026

Authors

Hongping Liu, Dingcheng Zhou, Wei Zhang, Xiaolong Zhang, Chengze Yang, Baicheng Zhang, Aoyuan Cheng, Hao Su, Yang Zhang, Meng Zhou, Xuepeng Zhang, Tao Wang, Guoqing Zhang

Published in

National science review. Volume 13. Issue 17. Pages nwag394. Epub Jun 26, 2026.

Abstract

Substitutions at the nodal and anti-nodal positions of conjugated aromatics exert profound effects on their electronic properties, yet a systematic investigation is lacking on how these underlying quantum mechanical rules are manifested experimentally. Here, using polycyclic aromatic hydrocarbon derivatives as a model system, we systematically elucidate how nodal and anti-nodal substitutions dictate their chemical reactivity and physical properties. It is found that Sonogashira C-C coupling at the nodal position has a noticeably lower product yield than the anti-nodal position under identical reflux conditions due to inhibited molecular orbital amplitude. Comprehensive spectroscopic characterization of the resulting substituted products reveals two striking photophysical differences: (1) Frontier orbital symmetry is largely conserved in node-substituted molecules, whereas the anti-nodal substitution induces strong symmetry-breaking, leading to accelerated fluorescence emission in anti-node-substituted pyrenes; (2) Nodal substitution induces the formation of charge-transfer states due to a twisted geometry, which activates room-temperature phosphorescence via improved singlet-triplet intersystem crossing. This study establishes an effective structure-property relationship linking molecular orbital symmetry to macroscopic cross-coupling reactivity and molecular photophysics within these conjugated aromatics.

PMID:
42732397
Bibliographic data and abstract were imported from PubMed on 13 Sep 2026.

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