Modeling Heat Dissipation at the Nanoscale: An Embedding Approach for Chemical Reaction Dynamics on Metal Surfaces

Abstract

We present an embedding technique for metallic systems that makes it possible to model energy dissipation into substrate phonons during surface chemical reactions from first principles. The separation of chemical and elastic contributions to the interaction potential provides a quantitative description of both electronic and phononic band structure. Application to the dissociation of O${}_2$ at Pd(100) predicts translationally "hot" oxygen adsorbates as a consequence of the released adsorption energy (ca. 2.6 eV). This finding questions the instant thermalization of reaction enthalpies generally assumed in models of heterogeneous catalysis.

6 pages, 2 figures

References in corpus (3)

• Nearsightedness of Electronic Matter
• On the accuracy of first-principles lateral interactions: Oxygen at Pd(100)
• Competition between electron and phonon excitations in the scattering of nitrogen atoms and molecules off tungsten and silver surfaces

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