We report electron and Na + ion emission from single-crystal sodium nitrate (∼ 10 eV band gap) upon exposure to IR (1064 nm, 1.16 eV) laser radiation. The fluence dependence of both the ion and the electron yield is highly nonlinear, and the kinetic energies of the emitted ions can reach values up to 5 eV. The fluence dependence and the ion energy distributions can be understood by a previously presented model involving multiple photon charge transfer plus electrostatic ejection of adions siting atop electron traps. Further evidence for the role of defects in the observed ion emission are provided by two-beam experiments; one beam (UV laser) is used to generate defects and the second beam (IR laser) is used to photodesorb the ions. Such experiments demonstrate that exposure of the sodium nitrate surfaces to UV laser radiation significantly increases the ion emission due to IR laser radiation. PACS: 79.20.Ds; 61.82.Ms; 61.80.Ba Sodium nitrate (NaNO 3 ) is a major component of the highlevel nuclear wastes in underground storage tanks associated with US plutonium production during the cold war. Full description of the properties of NaNO 3 is essential to safely and correctly analyze and handle such wastes. Laser-induced desorption and ablation techniques are currently being developed for the analysis, control and processing of mixed nuclear wastes [1]. However, reliable quantitative analysis requires an understanding of the photodecomposition and desorption mechanisms, since they can affect the sample composition and resulting signals. For this purpose a number of studies have been recently performed that used laser fluences well below the ablation threshold, so that changes in the surface composition and morphology, as well as the interactions among the emitted species can be kept to a minimum [2][3][4][5][6][7][8][9][10][11].Although the major absorption bands of NaNO 3 have been observed at ∼ 6.4 eV, ∼ 10.5 eV, and ∼ 12.1 eV [12], it has been shown in previous work that exposure of NaNO 3 surfaces to 248-nm (5-eV) excimer laser radiation results in both neutral and ion emission [2,7,13]. Furthermore, the important role of defects during the emission process has been demonstrated by comparing the emission from as-cleaved, abraded and electron irradiated surfaces. Both the fluence dependence and the kinetic energy of the emitted species strongly depend on the surface treatment, and therefore defect density, with treated surfaces exhibiting dramatically higher ion yields [7,14].Because sodium nitrate is a wide-band-gap molecularionic crystal, one might not expect emission of several-eV positive ions from NaNO 3 surfaces upon irradiation with low-energy photons (hν = 1.16 eV). Surprisingly, we do observe Na + emission accompanying nanosecond laser pulses at 1064 nm with fluences below the single-pulse damage threshold from single-crystal NaNO 3 surfaces. The fluence dependence of the ion yield is highly nonlinear and the emitted ions exhibit kinetic energies up to 5 eV. In addition to positive ions, emission of photo...