Regioisomeric Benzidine-Fullerenes: Tuning of the Diverse Hole-Distribution to Influence Charge Separation Patterns.
Angew Chem Int Ed Engl
; 62(15): e202300377, 2023 Apr 03.
Article
em En
| MEDLINE
| ID: mdl-36790824
ABSTRACT
Understanding the influence of molecular structure on charge distribution and charge separation (CS) provides essential guidance for optoelectronic materials design. Here we propose a regioisomeric strategy to tune the diverse hole-distribution, and probe the influence on CS patterns. Para-, meta- and ortho-substituted benzidine-fullerene, named 1 p, 1 m and 1 o are designed. Following CS, hole-delocalization occurs in 1 p, while hole-localization exists in 1 m and 1 o. The rates of charge separation (4.02×1011 â
s-1 ) and recombination (9.8×109 â
s-1 ) of 1 p is about 20 and 12â
times faster than 1 m and 1 o, indicating that para-determined delocalization promotes ultrafast CS, while meta- and ortho-generated localization contributes to long-lived CS states. Computational analysis further implies that localization results from the destruction of electronic conjugation for 1 m, and limitation of conformational relaxation for 1 o. Given that the universality and simplicity of regional isomerism, this work opens up new thoughts for molecular design with tunable charge separation patterns.
Texto completo:
1
Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2023
Tipo de documento:
Article
País de afiliação:
China