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Statistical Mechanical Studies of Aqueous solutions and Biomolecular Systems

Da Silva, Fernando Luis Barroso LU (1999)
Abstract
This thesis is concerned with theoretical studies of aqueous solutions and biomolecular systems. Part of the present work is to understand equilibrium solvent and solute properties, while the other part is to study processes that occur in these solutions. Three points were focused: (a) the study of structure and dynamics of 1M aqueous NaCl electrolyte solution at a molecular level, which revealed particular features of these solutions such as the formation of large clusters; (b) the development of a new simulation algorithm for the Reverse Monte Carlo technique aimed to study aqueous solutions and disordered systems. Results for spherical molecules and liquid water are presented; (c) the study of binding small ions to macromolecules... (More)
This thesis is concerned with theoretical studies of aqueous solutions and biomolecular systems. Part of the present work is to understand equilibrium solvent and solute properties, while the other part is to study processes that occur in these solutions. Three points were focused: (a) the study of structure and dynamics of 1M aqueous NaCl electrolyte solution at a molecular level, which revealed particular features of these solutions such as the formation of large clusters; (b) the development of a new simulation algorithm for the Reverse Monte Carlo technique aimed to study aqueous solutions and disordered systems. Results for spherical molecules and liquid water are presented; (c) the study of binding small ions to macromolecules (proteins and micelles). The Tanford-Kirkwood model is critically analysed for models of biomolecules by means of Monte Carlo calculations. Anomalous behaviour found for the binding of ions to macromolecules in the presence of highly charged macroparticles is also reported. And, a titration study is performed to characterize interfacial properties of a prototropic molecule in self-assembled surfactant aggregates.



The core of our discussion is based on electrostatic interactions and statistical mechanics. The studied systems were modeled by effective Hamiltonians within the Born-Oppenheimer and McMillan-Mayer model levels. These Hamiltonians were solved by computer simulations (Monte Carlo and Molecular Dynamics), and, in some cases, also by solving the Poisson-Boltzmann equation. Dielectric continuum models are largely used, and a discussion of uniform and non-uniform cases for studies with biomolecules and micellar systems is also included. (Less)
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author
opponent
  • Prof Berendsen, Herman J. C.
organization
publishing date
type
Thesis
publication status
published
subject
keywords
highly charged macromolecules, dielectric discontinuity, dissociation constant, Tanford-Kirkwood model, protein mutation, electrostatic interactions, chemical potential, titration, biomolecules, computer simulations, radial distribution function, electrolyte solutions, continuum model., Theoretical chemistry, quantum chemistry, Teoretisk kemi, kvantkemi
pages
264 pages
publisher
Department of Theoretical Chemistry, Lund University
defense location
room G, Chemical Center, Sölvegatan 39, Lund, Sweden
defense date
2000-01-14 10:15
external identifiers
  • other:ISRN: LUNKDL/NKTC--99/1011--SE
ISBN
91-628-3903-9
language
English
LU publication?
yes
id
5a555836-0988-437c-a54b-c9ca0e4b7bda (old id 40175)
date added to LUP
2007-10-14 17:12:33
date last changed
2016-09-19 08:45:07
@phdthesis{5a555836-0988-437c-a54b-c9ca0e4b7bda,
  abstract     = {This thesis is concerned with theoretical studies of aqueous solutions and biomolecular systems. Part of the present work is to understand equilibrium solvent and solute properties, while the other part is to study processes that occur in these solutions. Three points were focused: (a) the study of structure and dynamics of 1M aqueous NaCl electrolyte solution at a molecular level, which revealed particular features of these solutions such as the formation of large clusters; (b) the development of a new simulation algorithm for the Reverse Monte Carlo technique aimed to study aqueous solutions and disordered systems. Results for spherical molecules and liquid water are presented; (c) the study of binding small ions to macromolecules (proteins and micelles). The Tanford-Kirkwood model is critically analysed for models of biomolecules by means of Monte Carlo calculations. Anomalous behaviour found for the binding of ions to macromolecules in the presence of highly charged macroparticles is also reported. And, a titration study is performed to characterize interfacial properties of a prototropic molecule in self-assembled surfactant aggregates.<br/><br>
<br/><br>
The core of our discussion is based on electrostatic interactions and statistical mechanics. The studied systems were modeled by effective Hamiltonians within the Born-Oppenheimer and McMillan-Mayer model levels. These Hamiltonians were solved by computer simulations (Monte Carlo and Molecular Dynamics), and, in some cases, also by solving the Poisson-Boltzmann equation. Dielectric continuum models are largely used, and a discussion of uniform and non-uniform cases for studies with biomolecules and micellar systems is also included.},
  author       = {Da Silva, Fernando Luis Barroso},
  isbn         = {91-628-3903-9},
  keyword      = {highly charged macromolecules,dielectric discontinuity,dissociation constant,Tanford-Kirkwood model,protein mutation,electrostatic interactions,chemical potential,titration,biomolecules,computer simulations,radial distribution function,electrolyte solutions,continuum model.,Theoretical chemistry,quantum chemistry,Teoretisk kemi,kvantkemi},
  language     = {eng},
  pages        = {264},
  publisher    = {Department of Theoretical Chemistry, Lund University},
  school       = {Lund University},
  title        = {Statistical Mechanical Studies of Aqueous solutions and Biomolecular Systems},
  year         = {1999},
}