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Summary

Gold clusters induce atomic-scale directional photoreactions on titanium dioxide surfaces. This study reveals anisotropic decomposition rates for benzoic acid, driven by electron conduction along specific crystal directions.

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Area of Science:

Surface Science
Photochemistry
Materials Chemistry

Background:

Titanium dioxide (TiO2) is a widely studied semiconductor photocatalyst.
Understanding surface reactions at the atomic scale is crucial for catalyst design.
Gold clusters can modify the electronic and catalytic properties of TiO2.

Purpose of the Study:

To investigate the influence of gold clusters on the atomic-scale anisotropy of surface carboxylate photoreactions on rutile TiO2(110).
To explore the role of gold clusters in directing the photoreaction of benzoic acid, a model hole-scavenger molecule.

Main Methods:

Scanning Tunneling Microscopy (STM) to observe surface morphology and reaction sites.
Density Functional Theory with onsite Coulomb interaction (DFT+U) to model electronic structure and reaction mechanisms.
UV/visible photoreaction experiments monitoring adsorbate depletion at room temperature.

Main Results:

Benzoic acid adsorption caused significant displacement of gold clusters (Au9) on TiO2 surfaces.
DFT calculations indicated distortion of Au9 clusters upon benzoic acid adsorption.
Photoreaction of benzoic acid exhibited anisotropic depletion rates, with a ~3-fold higher rate along the [001] direction compared to [110].
Empty sites formed elongated chains along specific crystallographic directions after photoexcitation.

Conclusions:

Gold clusters induce unprecedented atomic-scale anisotropy in the photoreaction of surface carboxylates on TiO2.
The observed anisotropy is attributed to anisotropic conduction of excited electrons along the [001] direction, leading to preferential hole accumulation and decomposition.
This work represents the first report of atomic-scale directionality in a semiconductor photo-induced chemical reaction.