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Fig 1.

The glycosidic link in a GlcNH2 -GlcNH2 dimer.

a) The dihedral angles ϕ and ψ. Atoms defining ϕ and ψ are lablled. b) CG Topology. Atoms and bonds in the CG Model are drawn thick and in color. The all atom structure of the monomers is shown in gray for orientation. The centers of the CG interaction sites are shown in black, while the transparent gray spheres illustrate the range of steric interactions. c) A free energy map for ϕ and ψ.

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Fig 1 Expand

Fig 2.

Components of the persistence length.

Decay of the bond vector correlation for simulations with and without electrostatic contributions.

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Fig 2 Expand

Table 1.

Radius of gyration from different water models.

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Table 1 Expand

Fig 3.

Complete set of nine PMF maps for the nine possible combinations of monomers in a chitosan polymer.

Arrows indicate links that can change when the charge on monomer changes in a titration move.

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Fig 3 Expand

Table 2.

Features of the PMF maps for all possible links.

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Table 2 Expand

Fig 4.

PMF specific persistence length.

a) Decay of the bond vector correlation for the nine different link types, and b) the correlation between the polymer stiffness (LP,0) and the energy of the second minimum (ΔG2).

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Fig 4 Expand

Table 3.

Effects of map swapping.

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Table 3 Expand

Table 4.

Radius of gyration from simulation and experiment.

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Table 4 Expand

Fig 5.

MC acceptance rates as a function of DD and pH.

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Fig 5 Expand

Fig 6.

Fitting pKi to titration data.

Comparison of simulated and experimental titration data for a) DD = 80% and pKi from 6.1 to 7.0; b) DD = 80% and pKi 6.5-6.7; c) DD = 76% and pKi 6.5-6.7.

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Fig 6 Expand

Fig 7.

Effect of cs on titration.

a) degree of dissociation vs pH. b) pKapp and c) n parameter as a function of cs for a polymer with DP = 1000 and DD = 89.4%.

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Fig 7 Expand

Fig 8.

Equilibrium conformations at different pH and cs for chitosan with DD 89.4% and DP 1000.

Red numbers above each structure gives the root mean square RG (nm). Orange regions indicate regions where the conditions for model validity are no longer fulfilled.

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Fig 8 Expand

Fig 9.

Contributions to the persistence length.

a)comparison of LP and LP,0 for cs = 0.1 and DD 59%, DP = 500; b) and c) effect of cs on LP,0 (b) and LP (c) for 89.4% DD for DP = 1000.

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Fig 9 Expand

Fig 10.

pKapp versus degree of dissociation for different DD of (a) 95%, (b) 68% (c) 50% and (d) 30% for three different values of cs.

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Fig 10 Expand

Fig 11.

Titration parameters as a function of DD.

(a)pKapp and (b) n parameter from a linear fit of pH vs in the range 0.5.

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Fig 11 Expand

Fig 12.

The effect of DD on a) RG and (b and c) the contributions to LP at pH 4.5 (b) and pH 6.5 (c) for Chitosan with DP = 500.

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Fig 12 Expand

Fig 13.

Effect of the pattern of acetylation RG of chitosan with 50% DD and DP = 500 for acetylation patterns with different blocksize and a random distribution.

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Fig 13 Expand

Fig 14.

Characteristic ratio vs DP for different force field contributions at pH 4.5 and cs = 0.1.

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Fig 14 Expand