@article{913571d48d29426aad36a398bd97833e,
title = "Multimodal Characterization of Crystal Structure and Formation in Rubrene Thin Films Reveals Erasure of Orientational Discontinuities",
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{\textquoteright} functionality in organic thin films and demonstrate that multimodal studies deepen the understanding of structure-function dynamics.",
keywords = "crystallization, microstructures, morphology, multiscale/multimodal imaging, thin films",
author = "Tan, {Jenna A.} and Dull, {Jordan T.} and Zeltmann, {Steven E.} and Tulyagankhodjaev, {Jakhangirkhodja A.} and Johnson, {Holly M.} and Alex Liebman-Pel{\'a}ez and Folie, {Brendan D.} and D{\"o}nges, {Sven A.} and Omar Khatib and Raybin, {Jonathan G.} and Roberts, {Trevor D.} and Hamerlynck, {Leo M.} and Tanner, {Christian P.N.} and Jina Lee and Colin Ophus and Bustillo, {Karen C.} and Raschke, {Markus B.} and Hendrik Ohldag and Minor, {Andrew M.} and Rand, {Barry P.} and Ginsberg, {Naomi S.}",
note = "Funding Information: The authors thank J. Utterback for helpful heat transport discussions. The authors thank C. Zhu for valuable discussion on GIWAXS interpretation and analysis. The authors also thank H.‐G. Steinr{\"u}ck for advice on the Scherrer analysis. The authors thank M. Marcus for guidance on preliminary STXM measurements at the 5.3.2.2 beamline at the Advanced Light Source at the Lawrence Berkeley National Laboratory. STXM, POM, 4D‐STEM, GIWAXS, IR ‐SNOM, and AFM and subsequent analysis had been supported by STROBE, A National Science Foundation Science & Technology Center under Grant No. DMR 1548924. The TEM imaging at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231. GIWAXS, SINS, and STXM were performed as part of the Advanced Light Source user program, supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231. J. A. T. acknowledges a National Defense Science and Engineering Graduate Fellowship, and N.S.G. acknowledges an Alfred P. Sloan Research Fellowship, a David and Lucile Packard Foundation Fellowship for Science and Engineering, and a Camille and Henry Dreyfus Teacher‐Scholar Award. J.T.D. and B.P.R. acknowledge support from a Princeton SEAS Project X award. s Funding Information: The authors thank J. Utterback for helpful heat transport discussions. The authors thank C. Zhu for valuable discussion on GIWAXS interpretation and analysis. The authors also thank H.-G. Steinr{\"u}ck for advice on the Scherrer analysis. The authors thank M. Marcus for guidance on preliminary STXM measurements at the 5.3.2.2 beamline at the Advanced Light Source at the Lawrence Berkeley National Laboratory. STXM, POM, 4D-STEM, GIWAXS, IR s-SNOM, and AFM and subsequent analysis had been supported by STROBE, A National Science Foundation Science & Technology Center under Grant No. DMR 1548924. The TEM imaging at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. GIWAXS, SINS, and STXM were performed as part of the Advanced Light Source user program, supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. J. A. T. acknowledges a National Defense Science and Engineering Graduate Fellowship, and N.S.G. acknowledges an Alfred P. Sloan Research Fellowship, a David and Lucile Packard Foundation Fellowship for Science and Engineering, and a Camille and Henry Dreyfus Teacher-Scholar Award. J.T.D. and B.P.R. acknowledge support from a Princeton SEAS Project X award. Publisher Copyright: {\textcopyright} 2023 Wiley-VCH GmbH.",
year = "2023",
month = mar,
day = "23",
doi = "10.1002/adfm.202207867",
language = "English (US)",
volume = "33",
journal = "Advanced Functional Materials",
issn = "1616-301X",
publisher = "Wiley-VCH Verlag",
number = "13",
}