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

被引：255

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.

引用

页数：5

共 24 条

[1] Photoluminescence spectroscopy of pure pentacene, perfluoropentacene, and mixed thin films
Anger, F.
Osso, J. O.
Heinemeyer, U.
Broch, K.
Scholz, R.
Gerlach, A.
Schreiber, F.
[J]. JOURNAL OF CHEMICAL PHYSICS, 2012, 136 (05)
[2] Electronic Processes at Organic-Organic Interfaces: Insight from Modeling and Implications for Opto-electronic Devices
Beljonne, David
Cornil, Jerome
Muccioli, Luca
Zannoni, Claudio
Bredas, Jean-Luc
Castet, Frederic
[J]. CHEMISTRY OF MATERIALS, 2011, 23 (03) : 591 - 609
[3] Microscopic theory of singlet exciton fission. II. Application to pentacene dimers and the role of superexchange
Berkelbach, Timothy C.
Hybertsen, Mark S.
Reichman, David R.
[J]. JOURNAL OF CHEMICAL PHYSICS, 2013, 138 (11)
[4] Observing the Multiexciton State in Singlet Fission and Ensuing Ultrafast Multielectron Transfer
Chan, Wai-Lun
Ligges, Manuel
Jailaubekov, Askat
Kaake, Loren
Miaja-Avila, Luis
Zhu, X. -Y.
[J]. SCIENCE, 2011, 334 (6062) : 1541 - 1545
[5] Diagrammatic exciton-basis valence-bond theory of linear polyenes
Chandross, M
Shimoi, Y
Mazumdar, S
[J]. PHYSICAL REVIEW B, 1999, 59 (07) : 4822 - 4838
[6] Maximizing Singlet Fission in Organic Dimers Theoretical Investigation of Triplet Yield in the Regime of Localized Excitation and Fast Coherent Electron Transter
Greyson, Eric C.
Vura-Weis, Josh
Michl, Josef
Ratner, Mark A.
[J]. JOURNAL OF PHYSICAL CHEMISTRY B, 2010, 114 (45) : 14168 - 14177
[7] High Triplet Yield from Singlet Fission in a Thin Film of 1,3-Diphenylisobenzofuran
Johnson, Justin C.
Nozik, Arthur J.
Michl, Josef
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (46) : 16302 - 16303
[8] Ultrafast singlet and triplet dynamics in microcrystalline pentacene films
Marciniak, Henning
Pugliesi, Igor
Nickel, Bert
Lochbrunner, Stefan
[J]. PHYSICAL REVIEW B, 2009, 79 (23):
[9] Exciton fission and fusion in bis(tetracene) molecules with different covalent linker structures
Mueller, Astrid M.
Avlasevich, Yuri S.
Schoeller, Wolfgang W.
Muellen, Klaus
Bardeen, Christopher J.
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (46) : 14240 - 14250
[10] RECONSIDERATION OF THE ELECTROABSORPTION SPECTRA OF THE TETRACENE AND PENTACENE CRYSTALS
PETELENZ, B
PETELENZ, P
SHURVELL, HF
SMITH, VH
[J]. CHEMICAL PHYSICS, 1988, 119 (01) : 25 - 39

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