Ultrafast photodissociation dynamics from the B(Σ) state of CS are studied by time-resolved photoelectron imaging using the fourth (4ω, 198 nm) and sixth (6ω, 133 nm) harmonics of a femtosecond Ti:sapphire laser. The B state of CS was prepared with the 4ω pulses, and subsequent dynamics were probed using the 6ω vacuum ultraviolet (VUV) pulses. The VUV pulses enabled real-time detection of S(D) photofragments, produced via CS(B(Σ)) → CS(X Σ) + S(D). The photoionization signal of dissociating CS(B(Σ)) molecules starts to decrease at about 100 fs, while the S(D) fragments appear with a finite (ca. 400 fs) delay time after the pump pulse. Also discussed is the configuration interaction of the B(Σ) state based on relative photoionization cross-sections to different cationic states.
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