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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)

1
Department of Chemistry, Ångström Laboratory, Uppsala University, 75237 Uppsala, Sweden
2
Department of Materials and Environmental Chemistry, Stockholm University, S-10691 Stockholm, Sweden
*
Author to whom correspondence should be addressed.
Received: 17 January 2020 / Revised: 6 February 2020 / Accepted: 10 February 2020 / Published: 12 February 2020
(This article belongs to the Section Computational Chemistry)
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. View Full-Text
Keywords: free energy; metadynamics; adsorption; TiO2; amino acids; ab initio; Tight-Binding free energy; metadynamics; adsorption; TiO2; amino acids; ab initio; Tight-Binding
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MDPI and ACS Style

Agosta, L.; Brandt, E.G.; Lyubartsev, A. 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). Computation 2020, 8, 12. https://0-doi-org.brum.beds.ac.uk/10.3390/computation8010012

AMA Style

Agosta L, Brandt EG, Lyubartsev A. 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). Computation. 2020; 8(1):12. https://0-doi-org.brum.beds.ac.uk/10.3390/computation8010012

Chicago/Turabian Style

Agosta, Lorenzo, Erik G. Brandt, and Alexander Lyubartsev. 2020. "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)" Computation 8, no. 1: 12. https://0-doi-org.brum.beds.ac.uk/10.3390/computation8010012

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