Polymorphism influences singlet fission rates in tetracene thin films

Arias, Dylan H.; Ryerson, Joseph L.; Cook, Jasper D.; Damrauer, Niels H.; Johnson, Justin C.

doi:10.1039/C5SC03535J

Title: Polymorphism influences singlet fission rates in tetracene thin films

Journal Article · Fri Nov 06 00:00:00 EST 2015 · Chemical Science

DOI:https://doi.org/10.1039/C5SC03535J· OSTI ID:1238105

Arias, Dylan H. ^[1]; Ryerson, Joseph L. ^[1]; Cook, Jasper D. ^[2]; Damrauer, Niels H. ^[2]; Johnson, Justin C. ^[3]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Univ. of Colorado, Boulder, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Here, we report the effect of crystal structure and crystallite grain size on singlet fission (SF) in polycrystalline tetracene, one of the most widely studied SF and organic semiconductor materials. SF has been comprehensively studied in one polymoprh (Tc I), but not in the other, less stable polymorph (Tc II). Using carefully controlled thermal evaporation deposition conditions and high sensitivity ultrafast transient absorption spectroscopy, we found that for large crystallite size samples, SF in nearly pure Tc II films is significantly faster than SF in Tc I films. We also discovered that crystallite size has a minimal impact on the SF rate in Tc II films, but a significant influence in Tc I films. Large crystallites exhibit SF times of 125 ps and 22 ps in Tc I and Tc II, respectively, whereas small crystallites have SF times of 31 ps and 33 ps. Our results demonstrate first, that attention must be paid to polymorphism in obtaining a self-consistent rate picture for SF in tetracene and second, that control of polymorphism can play a significant role towards achieving a mechanistic understanding of SF in polycrystalline systems. In this latter context we show that conventional theory based on non-covalent tetracene couplings is insufficient, thus highlighting the need for models that capture the delocalized and highly mobile nature of excited states in elucidating the full photophysical picture.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1238105

Report Number(s):: NREL/JA-5900-65001; CSHCBM

Journal Information:: Chemical Science, Vol. 7, Issue 2; Related Information: Chemical Science; ISSN 2041-6520

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 105 works

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Related Subjects

14 SOLAR ENERGY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
singlet fission
tetracene
exciton
transport
polymorph