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The general considerations for two-step photoionization of atoms and photodissociation of molecules using tunable laser sources are discussed. Experimental results are given for the (1) photoionization of rubidium vapor using a ruby-laser-pumped dye laser and a doubled ruby laser radiation, and (2) photodissociation of HCl using the Raman-shifted output and the fourth harmonic output of a tunable Nd-glass laser. The possibilities for other laser systems are also discussed.