Quadrupole Coupling in Purines and Pyrimidines by Hartree-Fock Lattice Calculations of Electric Field Gradients*

We present ab initio Hartree-Fock lattice calculations on adenine, guanine and hypoxanthine, and some pyrimidines, including cytosine and uracil derivatives. The electric field gradients at the nitrogen centres are related to NQR experimental determinations of nuclear quadrupole coupling constants. The calculations were performed as lattice calculations in the unit cell environment, with 6-31G or double zeta basis sets at the SCF level. The present analysis strongly suggests that at N3 in cytosine, N3 in guanine are both positive, and approximately tangential to the ring at that centre. In contrast, N7 in guanine is like most other azine-type N centres, with a largely radial direction for The 3-protonated cytosine ring has x as the local 7r-direction.