Integrating solvation shell structure in experimentally driven molecular dynamics using x-ray solution scattering data

Hsu, Darren J.; Leshchev, Denis; Kosheleva, Irina; Kohlstedt, Kevin L.; Chen, Lin X.

doi:10.1063/5.0007158

Title: Integrating solvation shell structure in experimentally driven molecular dynamics using x-ray solution scattering data

Journal Article · 27 May 2020 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0007158 · OSTI ID:1630955

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In the past few decades, prediction of macromolecular structures beyond the native conformation has been aided by the development of molecular dynamics (MD) protocols aimed at exploration of the energetic landscape of proteins. Yet, the computed structures do not always agree with experimental observables, calling for further development of the MD strategies to bring the computations and experiments closer together. Here, we report a scalable, efficient MD simulation approach that incorporates an x-ray solution scattering signal as a driving force for the conformational search of stable structural configurations outside of the native basin. We further demonstrate the importance of inclusion of the hydration layer effect for a precise description of the processes involving large changes in the solvent exposed area, such as unfolding. Utilization of the graphics processing unit allows for an efficient all-atom calculation of scattering patterns on-the-fly, even for large biomolecules, resulting in a speed-up of the calculation of the associated driving force. The utility of the methodology is demonstrated on two model protein systems, the structural transition of lysine-, arginine-, ornithine-binding protein and the folding of deca-alanine. We discuss how the present approach will aid in the interpretation of dynamical scattering experiments on protein folding and association.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0000989; SC0014664

OSTI ID:: 1630955

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 20 Vol. 152; ISSN 0021-9606

Publisher:: American Institute of PhysicsCopyright Statement

Country of Publication:: United States

Language:: English

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