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Sulfur-to-Metal Single-Atom Editing of a Thiourea Self-Assembled Monolayer into an Adatom-Bound N-Heterocyclic Carbene Monolayer on Coinage Metal Surfaces.

Created on 17 Jul 2026

Authors

Xiao Han, Arne Nalop, Alex-Cristian Tomut, Dominik Schwab, Lei Li, Jinfeng Xu, Hong-Jun Gao, Nikos L Doltsinis, Frank Glorius, Jindong Ren

Published in

Angewandte Chemie (International ed. in English). Pages e3064564. Jul 17, 2026. Epub Jul 17, 2026.

Abstract

N-Heterocyclic carbene (NHC) self-assembled monolayers (SAMs) are emerging as robust and versatile surface ligands, yet their direct on-surface construction with atomic precision remains elusive. Here, we report a reagent-free, thermally driven on-surface strategy for single-atom editing, providing an alternative to convert a heteroatom-anchored SAM into a functional NHC layer. N-Heterocyclic thiourea (NHT) with carefully chosen substituents undergoes a S-to-metal adatom exchange, yielding adatom-bound NHC on coinage metal surfaces. Using low-temperature scanning tunneling microscopy (LT-STM), synchrotron-radiation X-ray photoelectron spectroscopy (SR-XPS), time of flight secondary ion mass spectrometry (ToF-SIMS) and density functional theory (DFT), we identify two distinct classes of SAMs: (i) NHT-SAM, in which sulfur coordinates to the metal surface and (ii) NHC-SAM, characterized by M─C σ-bonds between the carbene center and a surface adatom. NHT undergoes a clean SAM-to-SAM conversion, achieving covalent single-atom editing within an intact monolayer. DFT calculations show this transformation is energetically favorable and highly tunable by substrates and N-substituents, establishing a general framework for atom-precise molecular editing at surfaces.

PMID:
42464665
Bibliographic data and abstract were imported from PubMed on 17 Jul 2026.

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