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Alkali doping leads to charge-transfer salt formation in a two-dimensional metal–organic framework
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Blowey, Phil J., Sohail, Billal, Rochford, Luke A., Lafosse, Timothy, Duncan, David A., Ryan, Paul T. P., Warr, Daniel, Lee, Tien-Lin, Costantini, Giovanni, Maurer, Reinhard J. and Woodruff, D. P. (2020) Alkali doping leads to charge-transfer salt formation in a two-dimensional metal–organic framework. ACS Nano, 14 (6). pp. 7475-7483. doi:10.1021/acsnano.0c03133 ISSN 1936-086X.
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Official URL: https://doi.org/10.1021/acsnano.0c03133
Abstract
Efficient charge transfer across metal–organic interfaces is a key physical process in modern organic electronics devices, and characterization of the energy level alignment at the interface is crucial to enable a rational device design. We show that the insertion of alkali atoms can significantly change the structure and electronic properties of a metal–organic interface. Coadsorption of tetracyanoquinodimethane (TCNQ) and potassium on a Ag(111) surface leads to the formation of a two-dimensional charge transfer salt, with properties quite different from those of the two-dimensional Ag adatom TCNQ metal–organic framework formed in the absence of K doping. We establish a highly accurate structural model by combination of quantitative X-ray standing wave measurements, scanning tunnelling microscopy, and density-functional theory (DFT) calculations. Full agreement between the experimental data and the computational prediction of the structure is only achieved by inclusion of a charge-transfer-scaled dispersion correction in the DFT, which correctly accounts for the effects of strong charge transfer on the atomic polarizability of potassium. The commensurate surface layer formed by TCNQ and K is dominated by strong charge transfer and ionic bonding and is accompanied by a structural and electronic decoupling from the underlying metal substrate. The consequence is a significant change in energy level alignment and work function compared to TCNQ on Ag(111). Possible implications of charge-transfer salt formation at metal–organic interfaces for organic thin-film devices are discussed.
| Item Type: | Journal Article | |||||||||||||||||||||
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| Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry Faculty of Science, Engineering and Medicine > Science > Physics |
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| SWORD Depositor: | Library Publications Router | |||||||||||||||||||||
| Library of Congress Subject Headings (LCSH): | Surfaces (Physics) , Charge transfer , Surface extended X-ray absorption fine structure, Standing waves, Density functionals | |||||||||||||||||||||
| Journal or Publication Title: | ACS Nano | |||||||||||||||||||||
| Publisher: | American Chemical Society (ACS) | |||||||||||||||||||||
| ISSN: | 1936-086X | |||||||||||||||||||||
| Official Date: | 23 June 2020 | |||||||||||||||||||||
| Dates: |
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| Volume: | 14 | |||||||||||||||||||||
| Number: | 6 | |||||||||||||||||||||
| Page Range: | pp. 7475-7483 | |||||||||||||||||||||
| DOI: | 10.1021/acsnano.0c03133 | |||||||||||||||||||||
| Status: | Peer Reviewed | |||||||||||||||||||||
| Publication Status: | Published | |||||||||||||||||||||
| Access rights to Published version: | Open Access (Creative Commons) | |||||||||||||||||||||
| Copyright Holders: | Copyright © 2020 American Chemical Society | |||||||||||||||||||||
| Date of first compliant deposit: | 1 June 2020 | |||||||||||||||||||||
| Date of first compliant Open Access: | 30 June 2020 | |||||||||||||||||||||
| RIOXX Funder/Project Grant: |
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