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Improved Sampling in Ab Initio Free Energy Calculations of Biomolecules at Solid-Liquid Interfaces: Tight-Binding Assessment of Charged Amino Acids on TiO2 Anatase (101)
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Number of Authors: 32020 (English)In: Computation, E-ISSN 2079-3197, Vol. 8, no 1, article id 12Article in journal (Refereed) Published
Abstract [en]

Atomistic simulations can complement the scarce experimental data on free energies of molecules at bio-inorganic interfaces. In molecular simulations, adsorption free energy landscapes are efficiently explored with advanced sampling methods, but classical dynamics is unable to capture charge transfer and polarization at the solid-liquid interface. Ab initio simulations do not suffer from this flaw, but only at the expense of an overwhelming computational cost. Here, we introduce a protocol for adsorption free energy calculations that improves sampling on the timescales relevant to ab initio simulations. As a case study, we calculate adsorption free energies of the charged amino acids Lysine and Aspartate on the fully hydrated anatase (101) TiO2 surface using tight-binding forces. We find that the first-principle description of the system significantly contributes to the adsorption free energies, which is overlooked by calculations with previous methods.

Place, publisher, year, edition, pages
2020. Vol. 8, no 1, article id 12
Keywords [en]
free energy, metadynamics, adsorption, TiO2, amino acids, ab initio, Tight-Binding
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-181199DOI: 10.3390/computation8010012ISI: 000525032300006OAI: oai:DiVA.org:su-181199DiVA, id: diva2:1427122
Available from: 2020-04-28 Created: 2020-04-28 Last updated: 2022-03-23Bibliographically approved

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Brandt, Erik G.Lyubartsev, Alexander

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