Abstract

The three-dimensional time-dependent quantum wave packet dynamics $(J=0)$ using a Hamiltonian for a triatomic molecule in Radau coordinates is employed to study laser pulse excitation of the OClO molecule. The fast Fourier transform (FFT) and the split operator methods are applied to propagate the wave packet. The vibronic excitations $A\phantom{\rule{0.2em}{0ex}}^{2}A_{2}({\ensuremath{\nu}}_{1},{\ensuremath{\nu}}_{2},{\ensuremath{\nu}}_{3})\ensuremath{\leftarrow}X\phantom{\rule{0.2em}{0ex}}^{2}B_{1}(0,0,0)$ of the triatomic molecule OClO using femtosecond laser pulses of varying intensities are investigated. With an ultrashort laser pulse of certain FWHM (full width at half maximum), the vibrational level can be selectively excited. The changes in the vibrational population distributions caused by simple variation of the pulse are remarkable.

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