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Fig 1.

Hydrogen-bonding alternatives; linear H-bond assumed by the Pauling/Donohue groups; three-centered hydrogen bonds to carbonyl oxygens that dominate crystal structures of small organic molecules [6].

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Fig 1 Expand

Fig 2.

Schematic stick-figure diagrams of α-helix (top left and middle) and 310-helix (bottom left and right) helices.

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Fig 2 Expand

Fig 3.

Reproduction of Fig 1 from Némethy et al. [9] showing an intermediate N-helix (3.613/10) with the helical parameters of the classical α-helix and bifurcated amide H-bonds (used with permission).

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Fig 3 Expand

Fig 4.

The appearance of electron density as a function of the nominal resolution of the experimental crystallographic data, (adapted from similar figure for the N-terminal fragment (Lys1—Val2—Phe3) of triclinic lysozyme (PDB: 2vb1) from Wlodawer et al. [33] for which permission to reproduce by the journal was not granted).

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Fig 4 Expand

Fig 5.

Left: Distribution of helical backbone torsion angles (Φ, Ψ) for 1.0–1.5 Å nominal resolution of 3,462 protein structures from the PDB.

Right: Conversion of density of high-resolution helices to a relative energy scale by Boltzmann-weighting the distribution.

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Fig 5 Expand

Fig 6.

Average values of Φ (Phi) and Ψ (Psi) torsion angles of helical residues in PDB binned by nominal crystallographic resolution.

This compensatory change in Φ, Ψ is due to a “crankshaft” motion [39] of the amide bond that maintains the relative positions of the α-carbons of the peptide backbone despite significant deviations in Φ, Ψ torsions.

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Fig 6 Expand

Table 1.

Hydrogen-bond analysis of the PDB as a function of nominal crystallographic resolution.

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Table 1 Expand

Table 2.

Structural Percentage of the PDB as a function of nominal crystallographic resolution.

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Table 2 Expand

Table 3.

Hydrogen-bond analyses for neutron-diffraction data for 26 proteins.

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Table 3 Expand

Fig 7.

Definition of helical parameters with an oligopeptide helix backbone (nitrogens in blue).

Left: Helix winding (Ω) is the angle between two adjacent Cα vectors (n = residues-per-turn/360). Right: Helix pitch (p) is the rise-per-residue, or vertical distance between Ω adjacent residues, projected on the helical axis.

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Fig 7 Expand

Fig 8.

Contours and 3D surface helical pitch (n d) overlaid on 2D φ, ψ plot.

Positions of classic α-helix (φ = −57, ψ = −47), 310-helix (φ = −49, ψ = −26), and experimental Némethy-, N- or 3.613/10-helix (φ = −62, ψ = −43) are indicated. Note that the helical pitch is nearly identical for the α- and 3.613/10-helices—they lie on a contour of essentially equal value.

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Fig 8 Expand

Fig 9.

Contours and 3D surface showing rise-per-residue (d in Å) overlaid on 2D φ,ψ plot.

Positions of classic α-helix (φ = −57, ψ = −47), 310-helix (φ = −49, ψ = −26), and Némethy-, N- or 3.613/10-helix (φ = −62, ψ = −43) are indicated. Note that d is approximately the same for the α- and 3.613/10-helices.

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Fig 9 Expand

Fig 10.

Contours and 3D surface showing number of residues-per-turn (n) overlaid on 2D φ, ψ plot.

Positions of classic α-helix (φ = −57, ψ = −47), 310-helix (φ = −49, ψ = −26), and experimental Némethy-, N- or 3.613/10-helix (φ = −62, ψ = −43) are indicated. Note that n is approximately the same for the α- and 3.613/10-helices.

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Fig 10 Expand

Fig 11.

Helix 8–18 from the crambin crystal structure [PDB:1ejg], viewed from above the N-terminus.

The average φ value along the helix was between the experimental Némethy-, N- or 3.613/10-helix and the α-helix. However, the average ψ value was between the experimental 3.613/10-helix and a 310-helix.

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Fig 11 Expand

Table 4.

Backbone Torsional Angles of High-resolution (1ejg, 0.54 Å) Structure of Crambin 7–18 Helix (Fig 11).

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Table 4 Expand

Fig 12.

Transition of oligoalanine from its starting α-helical conformation to intermediate states that includes near α-, 310- and polyglycine conformations.

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Fig 12 Expand

Fig 13.

Ramachandran plot of backbone torsional angles from the AMOEBA BIO09 MD simulation of 12-residue oligoalanine.

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Fig 13 Expand

Fig 14.

The Φ, Ψ angles distribution of the data filtered with H-bond distance (<4 Å) and Φ, Ψ angles range (-100 -> 0, -70 -> 0).

The median of Φ, Ψ angles was Φ-72.8, Ψ-33.4.

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Fig 14 Expand

Fig 15.

Distance distribution of observed H-bonds filtered by H-bond distance (<4 Å) and Φ, Ψ angles range (-100 -> 0, -70 -> 0).

The medians of i+3 and i+4 distances were 2.97 Å and 2.28 Å, respectively.

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Fig 15 Expand

Fig 16.

Orthogonal views of ball-and-stick model of “dynamic” helix of 12-residue capped oligoalanine with two three-centered hydrogen bonds indicated (red dots).

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Fig 16 Expand

Table 5.

Relative energies of the three helical structures of Ac-Ala-Ala-Ala-NHMe by MP2/6–311(1d,1p) quantum calculations in vacuo.

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Table 5 Expand

Table 6.

Location of the two energy mimima-like positions on the potential energy surfaces of Ac-Ala-Ala-Ala-NHMe based on methodology.

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Table 6 Expand

Table 7.

Calculated dipole moments [65] in Debye using a modified set of parameters for solvation energy (Parse) partial atomic charges [67] for various capped 12-residue oligoalanine helices as well as for crambin and its isolated helix compared with those using AMOEBA multipoles.

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Table 7 Expand

Fig 17.

Potential surfaces for torsional force-fields surfaces surrounding helical conformations for A. AMBER99sb, B. AMOEBABIO09, C. CHARMM22, D. OPLS-AA, and E. OPLS-AAL versus F. QM—MP2/6-311(1d,1p) basis set.

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Fig 17 Expand

Fig 18.

The potential surface near helical torsional angles for Ac-Ala-Ala-Ala-NMe as calculated by QM.

The red line traces the transition between the two energy minima-like conformers without an activation energy barrier.

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Fig 18 Expand

Fig 19.

The whole (top) and expanded (lower) Ramachandran plots of 12-residue oligo-Ala (left sides) and oligo-Aib (right sides) from AMOEBA replica-exchange MD simulation.

The 310-region in Aib is heavily occupied while in alanine it’s almost absent.

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Fig 19 Expand

Fig 20.

The hydrogen-bonding matrix of 12-residue capped oligo-Ala (left) and oligo-Aib (right) from AMOEBA replica-exchange MD simulation.

The acceptor+1(i->i+2) and acceptor+2(i->i+3), indicating 310 helix) in oligo-Aib is more heavily occupied than in oligo-Ala.

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Fig 20 Expand

Fig 21.

Contour plots of oligo-Ala dipole moment.

The dipole moment magnitudes of the classic α-helix, 310-helix and Nemethy-, N-, 3.613/10-helix are marked with circles.

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Fig 21 Expand