One-dimensional self-confinement promotes polymorph selection in large-area organic semiconductor thin films

Gaurav Giri, Ruipeng Li, Detlef-M Smilgies, Er Qiang Li, Ying Diao, Kristina M. Lenn, Melanie Chiu, Debora W. Lin, Ranulfo Allen, Julia Reinspach, Stefan C. B. Mannsfeld, Sigurdur T. Thoroddsen, Paulette Clancy, Zhenan Bao () and Aram Amassian ()
Additional contact information
Gaurav Giri: Stanford University
Ruipeng Li: King Abdullah University of Science and Technology (KAUST)
Detlef-M Smilgies: Cornell High Energy Synchrotron Source (CHESS)
Er Qiang Li: King Abdullah University of Science and Technology (KAUST)
Ying Diao: Stanford University
Kristina M. Lenn: School of Chemical and Biomolecular Engineering, Cornell University
Melanie Chiu: Stanford University
Debora W. Lin: Stanford University
Ranulfo Allen: Stanford University
Julia Reinspach: Stanford University
Stefan C. B. Mannsfeld: SLAC National Accelerator Laboratory
Sigurdur T. Thoroddsen: King Abdullah University of Science and Technology (KAUST)
Paulette Clancy: School of Chemical and Biomolecular Engineering, Cornell University
Zhenan Bao: Stanford University
Aram Amassian: King Abdullah University of Science and Technology (KAUST)

Nature Communications, 2014, vol. 5, issue 1, 1-8

Abstract: Abstract A crystal’s structure has significant impact on its resulting biological, physical, optical and electronic properties. In organic electronics, 6,13(bis-triisopropylsilylethynyl)pentacene (TIPS-pentacene), a small-molecule organic semiconductor, adopts metastable polymorphs possessing significantly faster charge transport than the equilibrium crystal when deposited using the solution-shearing method. Here, we use a combination of high-speed polarized optical microscopy, in situ microbeam grazing incidence wide-angle X-ray-scattering and molecular simulations to understand the mechanism behind formation of metastable TIPS-pentacene polymorphs. We observe that thin-film crystallization occurs first at the air–solution interface, and nanoscale vertical spatial confinement of the solution results in formation of metastable polymorphs, a one-dimensional and large-area analogy to crystallization of polymorphs in nanoporous matrices. We demonstrate that metastable polymorphism can be tuned with unprecedented control and produced over large areas by either varying physical confinement conditions or by tuning energetic conditions during crystallization through use of solvent molecules of various sizes.

Date: 2014
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DOI: 10.1038/ncomms4573

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