Water Dimer-Driven DNA Base Superstructure with Mismatched Hydrogen Bonding

Thumbnail Image
Journal Title
Journal ISSN
Volume Title
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Degree programme
Journal of the American Chemical Society, Volume 144, issue 44
The existence of water dimers in equilibrium water vapor at room temperature and their anomalous properties revealed by recent studies suggest the benchmark role of water dimers in both experiment and theory. However, there has been a limited observation of individual water dimers due to the challenge of water separation and generation at the single-molecule level. Here, we achieve real-space imaging of individual confined water dimers embedded inside a self-assembled layer of a DNA base, adenine, on Ag(111). The hydration of the adenine layers by these water dimers causes a local surface chiral inversion in such a way that the neighboring homochiral adenine molecules become heterochiral after hydration, resulting in a mismatched hydrogen-bond pattern between neighboring adenine molecules. Furthermore, the mutual influence between the adenine superstructure and these dynamic confined water dimers is corroborated by theoretical simulation and calculations. The observation of single confined water dimers offersan unprecedented approach to studying the fundamental forms of water clusters and their interaction with the local chemical environment.
Funding Information: We thank Dr. Ondřej Krejčí for useful discussions. This research made use of the Aalto Nanomicroscopy Center (Aalto NMC) facilities and was supported by the European Research Council (ERC 2017 AdG no. 788185 “Artificial Designer Materials”) and the Academy of Finland (project nos. 347611, 347319, 346824, 314862, Centres of Excellence Program project no. 284621, and Academy professor funding nos. 318995 and 345066). A.S.F. has been supported by the World Premier International Research Center Initiative (WPI), MEXT, Japan. C.X. acknowledges funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement “EIM” no. 897828. This work was undertaken as part of the FinnCERES competence centre. Computing resources from the Aalto Science-IT project and CSC, Helsinki are gratefully acknowledged. | openaire: EC/H2020/788185/EU//E-DESIGN | openaire: EC/H2020/897828/EU//EIM
Other note
Cai , S , Kurki , L , Xu , C , Foster , A S & Liljeroth , P 2022 , ' Water Dimer-Driven DNA Base Superstructure with Mismatched Hydrogen Bonding ' , Journal of the American Chemical Society , vol. 144 , no. 44 , pp. 20227-20231 . https://doi.org/10.1021/jacs.2c09575