Abstract
A direct relationship between the N valence shell charge topology reflected in its Laplacian and the components of the electric field gradient (EFG) at the N nucleus in nitriles was found. The largest diagonal component of the N EFG tensor was showed to be determined by the combined effect of the bonded and nonbonded maxima of the Laplacian of the valence shell of the N atom along the C–N direction. In nonlinear nitriles, the asymmetry of the N field gradient around the C–N direction was showed to be determined by the difference in the values of the maxima of the Laplacian of the valence shell obtained in two mutually perpendicular planes that are also normal to the C–N direction and contained the N nucleus.

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