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This study investigates the ultrafast configuration changes and anomalous diffusion of phthalocyanine adsorbates on rare-gas nanoparticles using high-resolution two-dimensional electronic spectroscopy and molecular dynamics simulations. The research uncovers sub-diffusive surface motion and trapping of the adsorbate within single surface facets, challenging the expectation that weak adsorbate-surface interactions would lead to more fluid dynamics. These insights enhance our understanding of the kinetic behavior of adsorbates on nanostructures, which is crucial for optimizing catalytic processes in nanoreactors.
Sub-diffusive motion and trapping of adsorbates on nanoparticles defy expectations, revealing complex dynamics that could revolutionize our approach to nanocatalysis.
Nanoparticles (NPs) exhibit tunable catalytic properties and serve as nanoreactors for controlled multimolecular chemistry. The kinetics and reactivity of such systems are critically governed by the surface binding configurations of adsorbates, their stochastic fluctuations, and the adsorbate mobility across the nanosurface. However, resolving these properties with sufficient structural, spatial, and temporal resolution remains a major experimental challenge. Here, we study phthalocyanine adsorbates on rare-gas clusters as a test case. By combining high-resolution two-dimensional electronic spectroscopy and molecular dynamics simulations, we reveal the configurational dynamics of the adsorbates and establish a direct relation between these dynamics and the nanoscale properties of the clusters. Our findings indicate sub-diffusive surface motion and trapping of the adsorbate within single surface facets. Such dynamical behavior seems unexpected considering the weak adsorbate-surface interaction and cluster temperatures close to the sublimation point. These results provide direct insight into the ultrafast binding dynamics of molecular adsorbates on nanoscale objects, which is critical for our understanding of the chemistry of such systems.
