arXiv subjects

Henrik Grönbeck

Publications and source records attributed to Henrik Grönbeck.

3 recordsLinked to original sources

arXiv2026

Selectivity in tip-induced skeletal editing via heteroatom substitution

Skeletal editing enables precise structural modifications of molecules at late stages of a synthetic sequence, with applications in drug discovery and materials science. We recently demonstrated skeletal editing on the single-molecule scale. Voltage pulses applied by the tip of a scanning probe microscope to an oxygen-containing seven-membered heterocycle led to both oxygen deletion and ring-contraction rearrangement reactions. An open question is whether selective skeletal editing of a heterocyclic core can be achieved by an appropriate choice of the heteroatom. Here, we show that tip-induced reactions of an analogous sulfur-containing seven-membered ring results in sulfur deletion in virtually all cases. Our results demonstrate that the combination of tip-induced chemistry and heteroatom selection in the molecular design is a powerful strategy for single-molecule skeletal editing, with the potential to enable diverse structural transformations of heterocyclic frameworks.

cond-mat.mes-hall↗

arXiv2025

Skeletal editing by tip-induced chemistry

Skeletal editing of cyclic molecules has garnered considerable attention in the context of drug discovery and green chemistry, with notable examples in solution-phase synthesis. Here, we extend the scope of skeletal editing to the single-molecule scale. We demonstrate tip-induced oxygen deletion and ring contraction of an oxygen-containing seven-membered ring on bilayer NaCl films to generate molecules containing the perylene skeleton. The products were identified and characterized by atomic force and scanning tunneling microscopies, which provided access to bond-resolved molecular structures and orbital densities. Insights into the reaction mechanisms were obtained by density functional theory calculations. Our work expands the toolbox of tip-induced chemistry for single-molecule synthesis.

cond-mat.mes-hall↗

arXiv2023

The effect of different In$_2$O$_3$(111) surface terminations on CO$_2$ adsorption

In$_2$O$_3$-based catalysts have shown high activity and selectivity for CO$_2$ hydrogenation to methanol, however the origin of the high performance of In$_2$O$_3$ is still unclear. To elucidate the initial steps of CO$_2$ hydrogenation over In$_2$O$_3$, we have combined X-ray Photoelectron Spectroscopy (XPS) and Density Functional Theory (DFT) calculations to study the adsorption of CO$_2$ on the In$_2$O$_3$(111) crystalline surface with different terminations, namely the stoichiometric, the reduced, and the hydroxylated surface, respectively. The combined approach confirms that the reduction of the surface results in the formation of In ad-atoms and that water dissociates on the surface at room temperature. A comparison of the experimental spectra and the computed core-level-shifts (using methanol and formic acid as benchmark molecules) suggests that CO$_2$ adsorbs as a carbonate on all surface terminations. We find that CO$_2$ adsorption is hindered by hydroxyl groups on the hydroxylated surface.

cond-mat.mtrl-sci↗