Femtosecond ultraviolet laser-induced desorption of NO from NiO(100)/Ni(100)

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Abstract
We have studied the ultraviolet laser-induced desorption of NO molecules from an epitaxial film of NiO(100) on Ni(100) for pulse durations of 550 fs and at a photon energy of 3.95 eV. For applied laser intensities up to 450 MW/cm2, the highest intensities employed in this work, a linear dependence of the desorption yield on the laser intensity is observed. A desorption cross section of (1.9±0.3)⋅10−17 cm2 is then derived. The molecules are detected with rovibrational state selectivity by (1+1)-REMPI via the A 2Σ+(v′=0,1,2,3)←X 2Π(v″=0,1,2,3) γ-band transitions. The rotational population distributions are nonthermal, with rotational temperatures of about 290 K at low and of about 770 K at high rotational energies. The relative populations in the 2Π1/2 and 2Π3/2 fine-structure states and of the Λ-doublet states are examined for the given set of (v″,J″) quantum numbers. The vibrational states v″>0 are significantly populated approaching vibrational temperatures of 3800 K. Velocity distributions of the desorbed molecules are measured for individual rovibrational states. Bimodal distributions with a distinct rotational-translational coupling are observed. Further, molecules desorbing in the excited fine-structure state 2Π3/2 show a higher velocity than those desorbing in 2Π1/2 The results are compared with earlier ones obtained for the same system with nanosecond desorption pulses at hν=6.4 eV.