A concentration study is used to identify the optical absorption of zinc atoms isolated in solid nitrogen. Photoexcitation of the threefold-split, atomic 4p 1P1 singlet absorption band did not produce any emission from either the singlet or triplet states. Hartree–Fock (relativistic effective core potentials) plus variational and multireference perturbational configuration-interaction calculations are performed to analyze this very efficient quenching of excited state atomic zinc by molecular nitrogen. Of the two geometries considered in energy calculations of the approach of Zn(1P1) to N2, the collinear exhibited a slightly greater stabilization than the perpendicular approach. However, the collinear is identified as of no significance in the excited state quenching due to the absence of low energy crossings with the ground state. In contrast, for the perpendicular approach a crossing between the repulsive ground 1A1(1S0) state and the strongly attractive 1B2(1P1) state occurs close to the energy minimum of the 1B2 state. The efficiency of crossing between these states is analyzed in the framework of one-dimensional Landau–Zener (LZ) theory. A hopping probability of 0.07 is obtained for a single crossing, considered important in a rapidly relaxing solid state system, such as present in a low temperature matrix. Crossings found between the repulsive 3B1(3P1) and 3A1(3P1) states with the strongly bound 1B2(1P1) state are expected to play a role in gas phase Zn(1P1) quenching leading to the production of Zn(3PJ) states. LZ calculations indicate a small hopping probability for these crossings, consistent with the small 1P1→3PJ quenching cross sections observed in the gas phase work.