A combined experimental and theoretical study of the vibrational wave packe
t dynamics for the NaK molecule in the A (1)Sigma(+) state is presented. Th
e experiment utilises a 790 nm one-colour femtosecond pump-probe scheme wit
h detection of a previously nor reported dissociation pathway of the 3 (1)P
i(+) state, leading to the Na(3p) + K(4s) product channel. The dissociation
is suggested to proceed via either collisionally mediated processes or a m
olecular cascading process via the 4 (1)Sigma(+) state, which crosses sever
al states correlating to the Na(3p) + K(4s) limit. Time-dependent quantum m
echanical calculations are used for studying the dynamics in detail. Simula
tions are performed both for 790 nm and for 766 nm, to relate also to earli
er studies. The previous interpretations of the probe processes are revised
. Inclusion of vibrational and rotational temperature effects are shown to
be crucial for explaining the shape of the signal and the vibrational perio
d, and leads to excellent agreement with the experiments. (C) 1999 Elsevier
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