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  Origin of poor doping efficiency in solution processed organic semiconductors

Jha, A., Duan, H.-G., Tiwari, V., Thorwart, M., & Miller, R. J. D. (2018). Origin of poor doping efficiency in solution processed organic semiconductors. Chemical Science, 9(19), 4468-4476. doi:10.1039/c8sc00758f.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-A9C3-4 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-A9C4-3
Genre: Journal Article

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c8sc00758f.pdf (Publisher version), 987KB
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2018
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© The Royal Society of Chemistry

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https://dx.doi.org/10.1039/c8sc00758f (Publisher version)
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 Creators:
Jha, A.1, Author              
Duan, H.-G.1, 2, 3, Author              
Tiwari, V.1, 4, Author              
Thorwart, M.2, 3, Author
Miller, R. J. D.1, 3, 5, Author              
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2I. Institut für Theoretische Physik, Universität Hamburg, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, ou_persistent22              
4Department of Chemistry, University of Hamburg, ou_persistent22              
5The Departments of Chemistry and Physics, University of Toronto, ou_persistent22              

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 Abstract: Doping is an extremely important process where intentional insertion of impurities in semiconductors controls their electronic properties. In organic semiconductors, one of the convenient, but inefficient, ways of doping is the spin casting of a precursor mixture of components in solution, followed by solvent evaporation. Active control over this process holds the key to significant improvements over current poor doping efficiencies. Yet, an optimized control can only come from a detailed understanding of electronic interactions responsible for the low doping efficiencies. Here, we use two-dimensional nonlinear optical spectroscopy to examine these interactions in the course of the doping process by probing the solution mixture of doped organic semiconductors. A dopant accepts an electron from the semiconductor and the two ions form a duplex of interacting charges known as ion-pair complexes. Well-resolved off-diagonal peaks in the two-dimensional spectra clearly demonstrate the electronic connectivity among the ions in solution. This electronic interaction represents a well resolved electrostatically bound state, as opposed to a random distribution of ions. We developed a theoretical model to recover the experimental data, which reveals an unexpectedly strong electronic coupling of ∼250 cm−1 with an intermolecular distance of ∼4.5 Å between ions in solution, which is approximately the expected distance in processed films. The fact that this relationship persists from solution to the processed film gives direct evidence that Coulomb interactions are retained from the precursor solution to the processed films. This memory effect renders the charge carriers equally bound also in the film and, hence, results in poor doping efficiencies. This new insight will help pave the way towards rational tailoring of the electronic interactions to improve doping efficiencies in processed organic semiconductor thin films.

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Language(s): eng - English
 Dates: 2018-02-142018-04-072018-04-102018-05-21
 Publication Status: Published in print
 Pages: 9
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 Rev. Method: Peer
 Identifiers: DOI: 10.1039/c8sc00758f
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Project name : This work was supported by the Max Planck Society and the Excellence Cluster “ The Hamburg Center for Ultrafast Imaging – Structure, Dynamics and Control of Matter at the Atomic Scale ” of the Deutsche Forschungsgemeinscha  . H.-G. D. acknowledges  nancial support by the Joachim-Hertz- Sti  ung Hamburg within a PIER fellowship. The authors thank V. I. Prokhorenko for help with the 2D setup and for providing the 2D data analysis so  ware. Helpful discussions with Dr Jyotishman Dasgupta (TIFR) is also acknowledged. Open Access funding provided by the Max Planck Society.
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Title: Chemical Science
  Other : Chem. Sci.
Source Genre: Journal
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Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: - Volume / Issue: 9 (19) Sequence Number: - Start / End Page: 4468 - 4476 Identifier: ISSN: 2041-6520
CoNE: /journals/resource/2041-6520