Density-functional embedding theory (DFET) has emerged as a very promising multi-scale method to obtain energetics of surface catalysis with chemical accuracy.[1] It has a proven track record in tackling many challenging surface science problems, including explaining the adsorption of carbon monoxide on copper surface [2] and resolving the controversial mechanism of aluminum oxidation.[3] The basic idea of DFET is to partition a large system into two parts: the “cluster” (the region of interest) and the “environment”. Embedding potential, that represents the effect from environment on cluster, is then obtained in an ab initio way. Embedded correlated wave-function calculations on the cluster are then performed to obtain highly accurate energies and electronic structures of the cluster. Previous DFET applications mainly involved non-spin-polarized systems. In this talk, I will discuss why it is numerically very challenging to generate embedding potentials, the key quantity in DFET, for spin-polarized quantum mechanics systems. I will then present our latest development of DFET to completely overcome such numerical difficulty in a simple way. Our work paves the way to obtain energetics of chemical accuracy for heterogeneous catalysis involving spin-polarized catalysts, such as the Fischer-Tropsch and nitrogen fixation processes, both of which often employ iron as the catalysts. [1] F Libisch, C Huang, EA Carter, Accounts of chemical research 47 (9), 2768-2775; [2] Chen Huang, Michele Pavone, and Emily A. Carter, The Journal of Chemical Physics 134, 154110 (2011); [3] Florian Libisch, Chen Huang, Peilin Liao, Michele Pavone, and Emily A. Carter, Phys. Rev. Lett. 109, 198303 (2012).

Extending density-functional embedding theory to tackling heterogeneous catalysis that involves spin-polarized materials

251st National Meeting (2016)

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