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Construction of New Electronic Density Functionals with Error Estimation Through Fitting

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Abstract

We investigate the possibilities and limitations for the development of new electronic density functionals through large-scale fitting to databases of binding energies obtained experimentally or through high-quality calculations. We show that databases with up to a few hundred entries allow for up to of the order ten parameters to be adjusted in the exchange enhancement factor. The transferability of models between data is analyzed, and it is shown to be difficult to transfer a model trained exclusively on molecular atomization energies to the treatment of chemisorption systems.

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Notes

  1. The reference values calculated from the reference values of the atomization energies database (which probably yields more accurate values) deviate from the reference values that involve RPBE vibrations by 0.02eV, on average.

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Acknowledgements

We thank James P. Sethna, Jens K. Nørskov, Karoliina Honkala, Andreas Møgelhøj, Jess Wellendorff, and Keld T. Lundgaard for many inspiring discussions. The authors acknowledge support from the Danish Center for Scientific Computing and the U.S. Department of Energy—Office of Basic Energy Sciences through the funding of SUNCAT. The Center for Atomic-scale Materials Design is sponsored by the Lundbeck Foundation.

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Authors and Affiliations

  1. Center for Atomistic-scale Materials Design (CAMD), Department of Physics, Building 307, Nano DTU, Technical University of Denmark, DK-2800 Kgs, Lyngby, Denmark

    V. Petzold, T. Bligaard & K. W. Jacobsen

  2. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA, 94025, USA

    T. Bligaard

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  1. V. Petzold
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  2. T. Bligaard
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  3. K. W. Jacobsen
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Correspondence to T. Bligaard.

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Petzold, V., Bligaard, T. & Jacobsen, K.W. Construction of New Electronic Density Functionals with Error Estimation Through Fitting. Top Catal 55, 402–417 (2012). https://doi.org/10.1007/s11244-012-9801-7

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