Multimodal Characterization of Crystal Structure and Formation in Rubrene Thin Films Reveals Erasure of Orientational Discontinuities

Journal Article · Wed Jan 18 23:00:00 EST 2023 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202207867· OSTI ID:1963117

Tan, Jenna A. ^[1]; Dull, Jordan T. ^[2]; Zeltmann, Steven E. ^[3]; Tulyagankhodjaev, Jakhangirkhodja A. ^[4]; Johnson, Holly M. ^[2]; Liebman‐Peláez, Alex ^[5]; Folie, Brendan D. ^[5]; Dönges, Sven A. ^[6]; Khatib, Omar ^[6]; Raybin, Jonathan G. ^[1]; Roberts, Trevor D. ^[1]; Hamerlynck, Leo M. ^[1]; Tanner, Christian P. N. ^[1]; Lee, Jina ^[7]; Ophus, Colin ^[8]; Bustillo, Karen C. ^[8]; Raschke, Markus B. ^[6]; Ohldag, Hendrik ^[9]; Minor, Andrew M. ^[10]; Rand, Barry P. ^[11] ; Ginsberg, Naomi S. ^[12]

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1. Department of Chemistry University of California Berkeley CA 94720 USA, NSF Science &, Technology Center STROBE Berkeley CA 94720 USA
2. Department of Electrical and Computer Engineering Princeton University Princeton NJ 08544 USA
3. NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Department of Materials Science and Engineering University of California Berkeley CA 94720 USA
4. NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Department of Chemistry University of California Los Angeles CA 90095 USA
5. Department of Physics University of California Berkeley CA 94720 USA
6. NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Department of Physics and JILA University of Colorado Boulder CO 80309 USA
7. NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Division of Geological and Planetary Sciences California Institute of Technology Pasadena CA 91125 USA
8. National Center for Electron Microscopy Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
9. Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Department of Material Sciences and Engineering Stanford University Stanford CA 94305 USA, Department of Physics University of California Santa Cruz Santa Cruz CA 94064 USA
10. NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Department of Materials Science and Engineering University of California Berkeley CA 94720 USA, National Center for Electron Microscopy Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
11. Department of Electrical and Computer Engineering Princeton University Princeton NJ 08544 USA, Andlinger Center for Energy and the Environment Princeton University Princeton NJ 08544 USA
12. Department of Chemistry University of California Berkeley CA 94720 USA, NSF Science &, Technology Center STROBE Berkeley CA 94720 USA, Department of Physics University of California Berkeley CA 94720 USA, Materials Science Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA, Molecular Biophysics and Integrated Bioimaging Division Lawrence Berkeley National Laboratory Berkeley CA 94720 USA

Abstract

Multimodal multiscale characterization provide opportunities to study organic semiconducting thin films with multiple length scales, across multiple platforms, to elucidate crystallization mechanisms of the various microstructures that impact functionality. With polarized scanning transmission X‐ray and 4D‐scanning transmission electron microscopy, hybrid crystalline structures in rubrene thin films in which large crystalline domains surround a common nucleus and transition to a spherulite morphology at larger radii is observed. These high‐resolution techniques reveal how azimuthal orientational discontinuities at smaller radii are erased as spherulite morphology takes hold. In situ crystallization in the films with optical microscopy is also captured, discovering the importance of considering the initial temperature increase of a film during thermal annealing over the crystallization timescale. This kinetic information of the radial crystallization rate and of corresponding film heating kinetics is used to estimate the temperature at which the larger crystalline regions transition into a spherulite. By combining the results obtained from the different characterization modes, it is learned that thermal conditions can sensitively affect the crystallization of rubrene and other organic thin films. The observations suggest opportunities for more complex temperature‐dependent processing to maximize hybrid structures’ functionality in organic thin films and demonstrate that multimodal studies deepen the understanding of structure‐function dynamics.

• Sponsoring Organization: USDOE
• Grant/Contract Number: AC02-05CH11231
• OSTI ID: 1963117
• Journal Information: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 13 Vol. 33; ISSN 1616-301X
• Publisher: Wiley Blackwell (John Wiley & Sons)
• Country of Publication: Germany
• Language: English