The comparison between experimental values of the electric field gradient in neptunyl and uranyl complexes allows the derivation of a simple expression for the inner Sternheimer factor in Np. Its evaluation using relativistic expressions for the hyperfine interactions gives the result JR 5/ =0.35±0.1. An early theoretical estimate is in poor agreement with this number.The Hamiltonian describing the nuclear quadrupole interaction in the presence of an axially symmetric electric field gradient (efg) has the form 3C Q =[e 2^( ?(3?/-/ 2 )]/4/(2/-l).(1)Here Q is the nuclear quadrupole moment, eq z is the principal component of the efg tensor evaluated at the nucleus, and I* and I 2 are the nuclear angular momentum operators. If Q is known, 1 a measurement of the quadrupole interaction makes it possible to obtain the value of eq z . In general eq z is the sum of several contributions having values that depend on the physical and chemical nature of the solid. In the case of a covalent complex of an actinide we can write + B(i~i?" J k / A !ffl i %J.(2) tnlm The first term of Eq.(2) is given in analogy to rare-earth compounds, 2 and e(q 5f ) T represents the thermal expectation value of the efg produced by the 5f valence electrons which do not participate in bonding. As originally pointed out by Sternheimer, the inner electrons modify the efg, 3 and this effect is described by the introduction of a shielding factor (l-i? 5/ ). In the second term, eq Utt is the efg from the lattice charges external to the ion. The corresponding Sternheimer factor y^ is large and negative for the actinides (ca. -150), 4 however the lattice term is in general small compared to the other contributions. The last term in Eq.(2) gives the efg from bonding orbitals of the type nlm and the R nl are again Sternheimer factors. Since the 5/ electrons often participate in the bonding of actinide compounds, this term can be of major importance. This is a behavior quite different from the rare earths.For the purpose of this paper we will combine the last two terms of Eq. (2) and write eq z =e(q 5f ) T (l-R 5f ) + eq'.In order to extract the value of R 5f from a measurement of eq z , one needs to know e(q Bf ) T and eq'. The first term e(q 5f ) T can be calculated in 1085