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Oxygen as a Classifier of Superatomic Electronic States in Au-Based Clusters
Yaochen Han1, Qingyan Wang1, Yaotao Shan1
1State Key Laboratory of Quantum Functional Materials, School of Physical Science and Technology, Shanghai Tech University, Shanghai201210, China.
Journal of the American Chemical Society
|August 12, 2026
Summary
Oxygen distinguishes electronic states in gold superatoms. Closed-shell clusters bind molecular oxygen, while open-shell clusters bind atomic oxygen, aiding materials design.
Area of Science:
- Materials Science
- Surface Chemistry
- Quantum Chemistry
Background:
- The electronic structure of gold superatomic clusters dictates their properties.
- Experimental methods for classifying these electronic states are limited.
Purpose of the Study:
- To develop a facile experimental method for classifying electronic states in gold superatomic clusters.
- To correlate oxygen reactivity with superatomic electronic shell character.
Main Methods:
- Utilized a custom plasma source delivering atomic and molecular oxygen.
- Performed collisional cross-sectional area measurements.
- Conducted global geometric structure searches and density functional theory (DFT) analyses.
Main Results:
- Demonstrated oxygen as a classifier for open-/closed-shell-like electronic manifolds.
- Observed preferential molecular oxygen adduct formation in closed-shell clusters.
- Found atomic oxygen incorporation in open-shell clusters.
- Extended the method to Au-Ag, Au-Cu, and Au-W alloy clusters.
Conclusions:
- Oxygen uptake stoichiometry directly correlates with superatomic shell character.
- This method provides a practical route to link structure, electronic states, and functionality.
- Implications for cluster-based catalysis and materials design.
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