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Molecular Adsorption Changes the Quantum Structure of Oxide-Supported Gold Nanoparticles: Chemisorption versus Physisorption

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Stiehler,  Christian
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Calaza,  Florencia
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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Schneider,  Wolf-Dieter
Chemical Physics, Fritz Haber Institute, Max Planck Society;
Ecole Polytechnique Fédérale de Lausanne;

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Nilius,  Niklas
Chemical Physics, Fritz Haber Institute, Max Planck Society;
Carl von Ossietzky Universität;

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Freund,  Hans-Joachim
Chemical Physics, Fritz Haber Institute, Max Planck Society;

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PhysRevLett.115.pdf
(Publisher version), 2MB

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Citation

Stiehler, C., Calaza, F., Schneider, W.-D., Nilius, N., & Freund, H.-J. (2015). Molecular Adsorption Changes the Quantum Structure of Oxide-Supported Gold Nanoparticles: Chemisorption versus Physisorption. Physical Review Letters, 115(3): 036804. doi:10.1103/PhysRevLett.115.036804.


Cite as: http://hdl.handle.net/11858/00-001M-0000-0027-BD02-C
Abstract
STM conductance spectroscopy and mapping has been used to analyze the impact of molecular adsorption on the quantized electronic structure of individual metal nanoparticles. For this purpose, isophorone and CO2, as prototype molecules for physisorptive and chemisorptive binding, were dosed onto monolayer Au islands grown on MgO thin films. The molecules attach exclusively to the metal-oxide boundary, while the interior of the islands remains pristine. The Au quantum well states are perturbed due to the adsorption process and increase their mutual energy spacing in the CO2 case but move together in isophorone-covered islands. The shifts disclose the nature of the molecule-Au interaction, which relies on electron exchange for the CO2 ligands but on dispersive forces for the organic species. Our experiments reveal how molecular adsorption affects individual quantum systems, a topic of utmost relevance for heterogeneous catalysis.