Charge-Transfer Excitations Steer the Davydov Splitting and Mediate Singlet Exciton Fission in Pentacene

被引：257

作者：

Beljonne, D. ^{[1
,2
,3
]}

Yamagata, H. ^{[4
]}

Bredas, J. L. ^{[2
,3
]}

Spano, F. C. ^{[4
]}

Olivier, Y. ^{[1
]}

机构：

[1] Univ Mons, Lab Chem Novel Mat, B-7000 Mons, Belgium

[2] Georgia Inst Technol, Sch Chem & Biochem, Atlanta, GA 30332 USA

[3] Georgia Inst Technol, Ctr Organ Photon & Elect, Atlanta, GA 30332 USA

[4] Temple Univ, Dept Chem, Philadelphia, PA 19122 USA

来源：

PHYSICAL REVIEW LETTERS | 2013年 / 110卷 / 22期

基金：

美国国家科学基金会;

关键词：

TETRACENE; ELECTROABSORPTION; MOLECULES; CRYSTALS; FILM;

D O I：

10.1103/PhysRevLett.110.226402

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Quantum-chemical calculations are combined to a model Frenkel-Holstein Hamiltonian to assess the nature of the lowest electronic excitations in the pentacene crystal. We show that an admixture of chargetransfer excitations into the lowest singlet excited states form the origin of the Davydov splitting and mediate instantaneous singlet exciton fission by direct optical excitation of coherently coupled single and double exciton states, in agreement with recent experiments.

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页数：5

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