Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films
Jimison, Leslie H.
Northrup, John E.
Toney, Michael F.
Marks, Tobin J.
KAUST Grant NumberKUS-C1-015-21
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AbstractSolution-processable organic semiconductors are central to developing viable printed electronics, and performance comparable to that of amorphous silicon has been reported for films grown from soluble semiconductors. However, the seemingly desirable formation of large crystalline domains introduces grain boundaries, resulting in substantial device-to-device performance variations. Indeed, for films where the grain-boundary structure is random, a few unfavourable grain boundaries may dominate device performance. Here we isolate the effects of molecular-level structure at grain boundaries by engineering the microstructure of the high-performance n-type perylenediimide semiconductor PDI8-CN 2 and analyse their consequences for charge transport. A combination of advanced X-ray scattering, first-principles computation and transistor characterization applied to PDI8-CN 2 films reveals that grain-boundary orientation modulates carrier mobility by approximately two orders of magnitude. For PDI8-CN 2 we show that the molecular packing motif (that is, herringbone versus slip-stacked) plays a decisive part in grain-boundary-induced transport anisotropy. The results of this study provide important guidelines for designing device-optimized molecular semiconductors. © 2009 Macmillan Publishers Limited. All rights reserved.
CitationRivnay J, Jimison LH, Northrup JE, Toney MF, Noriega R, et al. (2009) Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films. Nat Mater 8: 952–958. Available: http://dx.doi.org/10.1038/nmat2570.
SponsorsPortions of this research were carried out at the Stanford Synchrotron Radiation Lightsource, a national user facility operated by Stanford University on behalf of the US DOE, Office of Basic Energy Sciences. J.R. gratefully acknowledges financial support from ONR in the form of an NDSEG Fellowship, and A.S. and L.H.J. gratefully acknowledge financial support from NSF in the form of, respectively, a Career Award and a Graduate Student Fellowship. This publication was partially based on work supported by the Center for Advanced Molecular Photovoltaics (Award No KUS-C1-015-21, made by King Abdullah University of Science and Technology, KAUST). J.E.N. thanks AFOSR (FA9550-09-1-0436), and T.J.M. and A.F. thank AFOSR (FA9550-08-1-0331) for support of this research.
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