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Title: Polymorphism influences singlet fission rates in tetracene thin films

Abstract

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 couplingsmore » 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.« less

Authors:
 [1];  [1];  [2];  [2];  [3]
+ Show Author Affiliations
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
  2. Univ. of Colorado, Boulder, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1238105
Report Number(s):
NREL/JA-5900-65001
Journal ID: ISSN 2041-6520; CSHCBM
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Science
Additional Journal Information:
Journal Volume: 7; Journal Issue: 2; Related Information: Chemical Science; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; singlet fission; tetracene; exciton; transport; polymorph

Citation Formats

Arias, Dylan H., Ryerson, Joseph L., Cook, Jasper D., Damrauer, Niels H., and Johnson, Justin C. Polymorphism influences singlet fission rates in tetracene thin films. United States: N. p., 2015. Web. doi:10.1039/C5SC03535J.
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Arias, Dylan H., Ryerson, Joseph L., Cook, Jasper D., Damrauer, Niels H., & Johnson, Justin C. Polymorphism influences singlet fission rates in tetracene thin films. United States. https://doi.org/10.1039/C5SC03535J
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Arias, Dylan H., Ryerson, Joseph L., Cook, Jasper D., Damrauer, Niels H., and Johnson, Justin C. Fri . "Polymorphism influences singlet fission rates in tetracene thin films". United States. https://doi.org/10.1039/C5SC03535J. https://www.osti.gov/servlets/purl/1238105.
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@article{osti_1238105,
title = {Polymorphism influences singlet fission rates in tetracene thin films},
author = {Arias, Dylan H. and Ryerson, Joseph L. and Cook, Jasper D. and Damrauer, Niels H. and Johnson, Justin C.},
abstractNote = {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.},
doi = {10.1039/C5SC03535J},
journal = {Chemical Science},
number = 2,
volume = 7,
place = {United States},
year = {Fri Nov 06 00:00:00 EST 2015},
month = {Fri Nov 06 00:00:00 EST 2015}
}
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Journal Article:
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https://doi.org/10.1039/C5SC03535J
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Figures / Tables:

Fig. 1 Fig. 1 : (a) XRD showing the (001) peak for the four film types. (b) AFM images of Tc I (top) and Tc II (bottom) films, with small (left) and large (right) crystallites. Scale bars = 2 μm. (c) Orientation of the dimers in the ab-plane corresponding to an [amore » b] translation vector of [1/2 1/2] in Tc I (top) and Tc II (bottom). (d) View of the herringbone structure in the ab-plane. Centroid molecule distances between the centre molecule and the nearest-neighbours are Tc I [1 0] = 6.056 Å, [-1/2 1/2] = 4.773 Å, and [1/2 1/2] = 5.125 Å; Tc II [1 0] = 5.909 Å, [-1/2 1/2] = 4.711 Å, and [1/2 1/2] = 4.787 Å. See ESI† for details of dimer distances and labelling.« less
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