New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations

Lantibiotics are an important class of naturally occurring antimicrobial peptides containing unusual dehydrated amino acid residues. In order to enable molecular dynamics simulations of lantibiotics, we have developed empirical force field parameters for dehydroalanine and dehydrobutyrine, which are...

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Main Authors: Turpin, Eleanor R., Mulholland, S., Teale, A.M., Bonev, B.B., Hirst, J.D.
Format: Article
Published: Royal Society of Chemistry 2014
Online Access:https://eprints.nottingham.ac.uk/29534/
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author Turpin, Eleanor R.
Mulholland, S.
Teale, A.M.
Bonev, B.B.
Hirst, J.D.
author_facet Turpin, Eleanor R.
Mulholland, S.
Teale, A.M.
Bonev, B.B.
Hirst, J.D.
author_sort Turpin, Eleanor R.
building Nottingham Research Data Repository
collection Online Access
description Lantibiotics are an important class of naturally occurring antimicrobial peptides containing unusual dehydrated amino acid residues. In order to enable molecular dynamics simulations of lantibiotics, we have developed empirical force field parameters for dehydroalanine and dehydrobutyrine, which are compatible with the CHARMM all-atom force field. The parameters reproduce the geometries and energy barriers from MP2/6-31G*//MP2/cc-pVTZ quantum chemistry calculations. Experimental, predicted and calculated NMR chemical shifts for the amino protons and alpha-, beta- and carbonyl carbon atoms of the dehydrated residues are consistent with a significant charge redistribution. The new parameters are used to perform the first molecular dynamics simulations of nisin, a widely used but poorly understood lantibiotic, in an aqueous environment and in a phospholipid bilayer. The simulations show surface association of the peptide with membranes in agreement with solid state NMR data and formation of beta-turns in agreement with solution NMR.
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spelling nottingham-295342020-05-04T16:53:41Z https://eprints.nottingham.ac.uk/29534/ New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations Turpin, Eleanor R. Mulholland, S. Teale, A.M. Bonev, B.B. Hirst, J.D. Lantibiotics are an important class of naturally occurring antimicrobial peptides containing unusual dehydrated amino acid residues. In order to enable molecular dynamics simulations of lantibiotics, we have developed empirical force field parameters for dehydroalanine and dehydrobutyrine, which are compatible with the CHARMM all-atom force field. The parameters reproduce the geometries and energy barriers from MP2/6-31G*//MP2/cc-pVTZ quantum chemistry calculations. Experimental, predicted and calculated NMR chemical shifts for the amino protons and alpha-, beta- and carbonyl carbon atoms of the dehydrated residues are consistent with a significant charge redistribution. The new parameters are used to perform the first molecular dynamics simulations of nisin, a widely used but poorly understood lantibiotic, in an aqueous environment and in a phospholipid bilayer. The simulations show surface association of the peptide with membranes in agreement with solid state NMR data and formation of beta-turns in agreement with solution NMR. Royal Society of Chemistry 2014-09-22 Article PeerReviewed Turpin, Eleanor R., Mulholland, S., Teale, A.M., Bonev, B.B. and Hirst, J.D. (2014) New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations. RSC Advances, 4 . pp. 48621-48631. ISSN 2046-2069 http://pubs.rsc.org/en/Content/ArticleLanding/2014/RA/c4ra09897h doi:10.1039/C4RA09897H doi:10.1039/C4RA09897H
spellingShingle Turpin, Eleanor R.
Mulholland, S.
Teale, A.M.
Bonev, B.B.
Hirst, J.D.
New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title_full New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title_fullStr New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title_full_unstemmed New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title_short New CHARMM force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
title_sort new charmm force field parameters for dehydrated amino acid residues, the key to lantibiotic molecular dynamics simulations
url https://eprints.nottingham.ac.uk/29534/
https://eprints.nottingham.ac.uk/29534/
https://eprints.nottingham.ac.uk/29534/