Nonadiabatic wave packet dynamics: experiment and theory in IBr

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Journal titleThe Journal Of Chemical Physics
Pages24652473; # of pages: 9
Subjectexcited states; iodine compounds; photoionisation; time resolved spectra; two-photon spectra
AbstractWe present an experimental and a theoretical study of nonadiabatic wave packet dynamics in the intermediate coupling regime as exhibited by the IBr molecule. Using a femtosecond pump舑probe molecular beam technique, we generated a wave packet which evolves on the electronically excited B 3 Pi0+/Y(0+) coupled states. The wave packet dynamics was detected by a time-delayed probe pulse which induced two photon ionization to the ground state of the IBr + ion. The study consisted of a systematic variation of the pump laser wavelength from the crossing point of the two coupled states to the dissociation limit of the bound diabatic state. The theoretical study is based on the convolution of the products of the energy resolved X 1 Sigma+ --> B 3 Pi0+/Y(0+) bound舑free dipole matrix elements and the free舑bound two-photon ionization amplitudes (calculated exactly using the artificial channel method) with the profiles of the pump and probe pulses. The theoretical calculations reproduce the general decay, recurrence, and revivals observed experimentally. The importance of treating nonadiabatic dynamics beyond the Landau舑Zener approximation, as well as the utility of femtosecond pump舑probe techniques in probing simultaneously short and long lived resonances is demonstrated.
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PublisherAIP Publishing
AffiliationNational Research Council Canada; Security and Disruptive Technologies
Peer reviewedYes
NPARC number12338155
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Record identifiere322de35-f7b4-4a0f-be3e-b3a677938aa1
Record created2009-09-10
Record modified2017-03-23
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