Binding of Single Gold Atoms on Thin MgO(001) Films

In the present Letter the first electron paramagnetic resonance spectra of single metal atoms on a single crystalline oxide surface are presented. For Au atoms on a MgO(001) film investigated here an analysis of the angular dependent resonance positions and the hyperfine coupling to ${}^{17}\mathrm{O}$ shows that the atoms are bound on top of oxygen ions on the terrace of the film. This result is in perfect agreement with scanning tunneling microscopy measurements at 5 K presented here. The measured hyperfine matrix components allow an experimental verification of the theoretically proposed binding mechanism of Au atoms on MgO. In particular, the large reduction of the isotropic hyperfine coupling constant of supported Au as compared to free atoms is not due to a charge transfer at the interface but a hybridization of orbitals and a resulting polarization of the unpaired electron.

Figure 1

(a) Experimental and simulated EPR spectrum of Au atoms adsorbed on $\mathrm{MgO}(001)/\mathrm{Mo}(001)$ ($\theta =90°$), green trace: spectrum for an ${}^{17}\mathrm{O}$ enriched MgO film (signal marked by a * belongs to the background). (b) Angular dependence of EPR resonance positions with respect to the polar angle $\theta$ between static magnetic field and surface normal.

Figure 2

STM image ($30\times 25{\mathrm{nm}}^2$, $V_S=+0.5\mathrm{V}$, $I_t=10\mathrm{pA}$) of Au atoms deposited at 8 K on a 6–8 ML thick MgO(001) film grown on Ag(001). The deposited amount of Au atoms corresponds to 0.035 ML.

Figure 3

(a) Spin density of an Au atom on a MgO terrace. (b) Dependence of the calculated isotropic hfcc of Au adsorbed to terrace sites of the MgO(100) surface on the distance between Au atom and O ion.