We report muon spin rotation/relaxation measurements of muonium in mesoporous silica (SBA-15) with a high specific surface area of 600 m2/g. Up to 70 percent of the incoming muons form muonium and escape efficiently into the open pores at all temperatures between 3 and 300K. We present evidence that the interaction with the silica surfaces involves both spin exchange and a transition to a diamagnetic state, possibly due to dangling bonds on the surface. At very low temperatures, below 20K, the interaction between muonium and the silica surfaces is suppressed due to a He film coating the surfaces. These results indicate that it should be possible to use muonium to probe the surfaces of uncapped nanoparticles supported in silica.

Gold nanoparticles (AuNPs) have been a subject of considerable interest in recent years due to both their magnetic and catalytic properties. This paper reports a two-fold study of the reactivity at 300 K of the isotopic hydrogen atom, muonium (Mu = μ+e-), (i) with bare uncapped AuNPs of different sizes encapsulated in mesoporous (SBA-15) silica hosts, forming a diamagnetic final state in the Mu + AuNP → MuAuNP reaction, and (ii) with surface-adsorbed benzene on these NPs forming the muoniated cyclohexadienyl radical in the Mu + C6H6 → MuĊ6H6 addition reaction. The measured muon-spin relaxation rates, λC, for the chemisorption reaction of Mu with the bare AuNPs show some variation with AuNP size. The Mu + C6H6 addition reaction has been studied over a range of benzene loadings both on bare silica and in the AuNP/silica samples. The measured muon-spin relaxation rates, λTot, exhibit a linear dependence on benzene concentration over the full range of loadings in both cases, in accord with an Eley-Rideal model of surface reactivity. Rate constants, kBz, were determined from this dependence which exhibit a 2-3-fold faster reaction rate on the AuNPs than on the bare silica, suggesting a catalytic effect due to benzene adsorbed on these NP surfaces.

μSR and ALCR techniques have been used to investigate the structure and dynamics of the Mu-cyclohexadienyl radical interacting with Au and Pt metal nanoparticles (MNPs) supported in mesoporous silica (SBA-15). Surprisingly, coherent precession signals are observed and the isotropic hyperfine coupling constants are almost the same in loaded and unloaded samples, implying that the electronic structure of MuC6H6 is only weakly perturbed by the presence of the MNPs. We propose the observed radicals are shielded from the metallic surfaces by a benzene coating on the MNPs. The Δ1 resonance is observable in MNP-loaded samples at higher temperatures than in the unloaded SBA-15. This is attributed to stronger binding of MuC6H6 to the benzene coated MNPs.

Chemisorption of muonium onto the surface of gold nanoparticles has been observed. Muonium (μ⁺e^-), a light hydrogen-like atom, reacts chemically with uncapped 7 nm gold nanoparticles embedded in mesoporous silica (SBA-15) with a strong temperature-dependent rate. The addition rate is fast enough to allow coherent spin transfer into a diamagnetic muon state on the nanoparticle surface. The muon is well established as a sensitive probe of static or slowly fluctuating magnetic fields in bulk matter. These results represent the first muon spin rotation signal on a nanoparticle surface or any metallic surface. Only weak magnetic effects are seen on the surface of these Au nanoparticles consistent with Pauli paramagnetism.