title: Microhydration of Protonated Nα-Acetylhistidine: A Theoretical Approach.
abstract: Extensive exploration of the potential energy surfaces of protonated Nα-acetylhistidine hydrated by 0-3 molecules of water was performed. The methodology combined hierarchical and genealogical (Darwin family tree) approaches using polarizable AMOEBA force field and M06 functional. It is demonstrated that this mixed approach allows recovering a larger number of conformers than the number recovered by using any one of the two methods alone. Hydration enthalpies of protonated Nα-acetylhistidine and of model compounds have been computed using higher theoretical methods, up to the G4MP2 procedure. Excellent agreement with experiment is observed for successive hydration of methylamonium and imidazolium cations using MP2/6-311++G(2d,2p)//M06/6-311++G(d,p) and G4MP2 methods, thereby validating the theory levels used for hydrated protonated Nα-acetylhistidine. It is found that the first hydration enthalpy of protonated Nα-acetylhistidine is ca. 10 kJ mol(-1) lower than that of imidazolium, a result explained by the local environment of the positively charged imidazolium moiety.
authors.affiliation: Laboratoire de Chimie Moléculaire, Ecole Polytechnique and CNRS , 91128 Palaiseau cedex, France.
authors.forename: Vanessa
authors.initials: V
authors.lastname: Riffet
authors.affiliation: Laboratoire de Chimie Moléculaire, Ecole Polytechnique and CNRS , 91128 Palaiseau cedex, France.
authors.forename: Guy
authors.initials: G
authors.lastname: Bouchoux
authors.affiliation: Laboratoire de Chimie Moléculaire, Ecole Polytechnique and CNRS , 91128 Palaiseau cedex, France.
authors.forename: Gilles
authors.initials: G
authors.lastname: Frison
mesh_terms: D000465:Algorithms; D002412:Cations / Q000737:chemistry; D006639:Histidine / Q000031:analogs & derivatives* / Q000737:chemistry; D006860:Hydrogen Bonding; D056004:Molecular Dynamics Simulation; D009010:Monte Carlo Method; D011522:Protons; D012965:Sodium Chloride / Q000737:chemistry; D013816:Thermodynamics; D014867:Water / Q000737:chemistry*
chemical_list: D002412:Cations; D011522:Protons; D014867:Water; D012965:Sodium Chloride; D006639:Histidine; C023495:N-acetylhistidine