Chemical transformations drive complex self-assembly of uracil on close-packed coinage metal surfaces

ACS Nano
Anthoula C PapageorgiouJohannes V Barth

Abstract

We address the interplay of adsorption, chemical nature, and self-assembly of uracil on the Ag(111) and Cu(111) surfaces as a function of molecular coverage (0.3 to 1 monolayer) and temperature. We find that both metal surfaces act as templates and the Cu(111) surface acts additionally as a catalyst for the resulting self-assembled structures. With a combination of STM, synchrotron XPS, and NEXAFS studies, we unravel a distinct polymorphism on Cu(111), in stark contrast to what is observed for the case of uracil on the more inert Ag(111) surface. On Ag(111) uracil adsorbs flat and intact and forms close-packed two-dimensional islands. The self-assembly is driven by stable hydrogen-bonded dimers with poor two-dimensional order. On Cu(111) complex structures are observed exhibiting, in addition, a strong annealing temperature dependence. We determine the corresponding structural transformations to be driven by gradual deprotonation of the uracil molecules. Our XPS study reveals unambiguously the tautomeric signature of uracil in the contact layer and on Cu(111) the molecule's deprotonation sites. The metal-mediated deprotonation of uracil and the subsequent electron localization in the molecule determine important biological reac...Continue Reading

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Citations

Jul 31, 2012·ACS Nano·Markus KittelmannAngelika Kühnle
Nov 10, 2014·The Journal of Chemical Physics·K L Svane, B Hammer
May 21, 2015·Physical Chemistry Chemical Physics : PCCP·Oksana PlekanKevin C Prince
Mar 27, 2018·Chemical Communications : Chem Comm·Yuanqi DingWei Xu
Aug 23, 2018·Chemical Communications : Chem Comm·Peter KnechtAnthoula C Papageorgiou
Dec 20, 2012·Nature Communications·Yi-Qi ZhangJohannes V Barth
May 24, 2019·Angewandte Chemie·Tobias PaintnerFlorian Klappenberger
Sep 4, 2013·Chemical Communications : Chem Comm·Fabian BebenseeTrolle Linderoth
Jul 22, 2018·Chemical Communications : Chem Comm·Yuanqi DingWei Xu
Sep 21, 2017·Langmuir : the ACS Journal of Surfaces and Colloids·Pavel BanerjeeNilmoni Sarkar

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