REEXAMINATION OF CHIRPED PULSE CONTROL OF WAVE-PACKET MOTION IN NAI

Recent experimental and theoretical studies of femtosecond pump-probe pulse excitation of NaI have led to information concerning bound-state wave packet motion, the control of wave packet localization, and the control of the branching between photodissociation products. This pape r reports calculations that (i) resolve the discrepancy between the ex periments that employ 50-60 fs pulses and those that employ 150-175 fs pulses; the former experiments show that the wave packet motion chang es from simple periodic to multiple periodic and back to simple period ic in a time span of 40 ps, while the latter experiments clo not show this change in wave packet dynamics; (ii) examine the relationship bet ween pulse width and photodissociation yield; and (iii) determine the optimal nonlinear chirped pump pulse that best localizes the excited-s tate wave packet with prescribed position and momentum chosen to enhan ce the photodissociation yield.