Selectivity in single-molecule reactions by tip-induced redox chemistry

Florian Albrecht, Shadi P. Fatayer, Iago Pozo, Ivano Tavernelli, Jascha Repp, Diego Peña, Leo Gross

Research output: Contribution to journalArticlepeer-review

37 Scopus citations

Abstract

Controlling selectivity of reactions is an ongoing quest in chemistry. In this work, we demonstrate reversible and selective bond formation and dissociation promoted by tip-induced reduction-oxidation reactions on a surface. Molecular rearrangements leading to different constitutional isomers are selected by the polarity and magnitude of applied voltage pulses from the tip of a combined scanning tunneling and atomic force microscope. Characterization of voltage dependence of the reactions and determination of reaction rates demonstrate selectivity in constitutional isomerization reactions and provide insight into the underlying mechanisms. With support of density functional theory calculations, we find that the energy landscape of the isomers in different charge states is important to rationalize the selectivity. Tip-induced selective single-molecule reactions increase our understanding of redox chemistry and could lead to novel molecular machines.
Original languageEnglish (US)
Pages (from-to)298-301
Number of pages4
JournalScience
Volume377
Issue number6603
DOIs
StatePublished - Jul 14 2022

Bibliographical note

KAUST Repository Item: Exported on 2022-09-14
Acknowledgements: We thank R. Allenspach, S. Mishra, E. Guitián, and Z. Zhu for discussions. For some of the calculations, this research used the resources of the Supercomputing Laboratory at King Abdullah University of Science and Technology (KAUST) in Thuwal, Saudi Arabia.
Funding: This work was supported by the ERC Synergy Grant MolDAM (951519), ERC Consolidator Grant AMSEL (682144), European FET-OPEN project SPRING (863098), Spanish Agencia Estatal de Investigación (PID2019-107338RB-C62, PID2019-110037GB-I00, and PCI2019-111933-2), Xunta de Galicia (Centro de Investigación de Galicia accreditation 2019–2022, ED431G 2019/03), and the European Regional Development Fund (ERDF).

ASJC Scopus subject areas

  • General

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