期刊
ACS NANO
卷 9, 期 4, 页码 4508-4526出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.5b01109
关键词
selenolate; self-assembly; self-assembled monolayers; charge transfer; bond strength; metal surfaces
类别
资金
- Deutsche Forschungsgemeinschaft [ZH 63/14-2, MAP B.1.4]
- National Science Centre Poland [DEC-2013/10/E/ST5/00060]
- European Community [312284]
- European Regional Development Fund [POIG.02.02.00-12-023/08]
Selenolate is considered as an alternative to thiolate to serve as a headgroup mediating the formation of self-assembled monolayers (SAMs) on coinage metal substrates. There are, however, ongoing vivid discussions regarding the advantages and disadvantages of these anchor groups, regarding, in particular, the energetics of the headgroup-substrate interface and their efficiency in terms of charge transport/transfer. Here we introduce a well-defined model system of 6-cyanonaphthalene-2-thiolate and -selenolate SAMs on Au(111) to resolve these controversies. The exact structural arrangements in both types of SAMs are somewhat different, suggesting-a better SAM-building ability in the case of selenolates. At the same time, both types of SAMs have similar packing densities and molecular orientations. This permitted reliable competitive exchange and ion-beam-induced desorption experiments which provided unequivocal evidence for a stronger bonding of selenolates to the substrate as compared to the thiolates. Regardless of this difference, the dynamic charge transfer properties of the thiolate- and selenolate-based adsorbates were found to be nearly identical, as determined by the core-hole-clock approach, which is explained by a redistribution of electron density along the molecular framework, compensating the difference in the substrate-headgroup bond strength.
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