Continuum resonance Raman scattering in iodine: Time‐dependent calculations, scattering delay times and demonstration of fundamental principles

Abstract

Continuum resonance Raman spectra of ' * ' I 2 were numerically simulated using timedependent quantum theory. The calculated spectra were compared with results obtained from traditional time-indepeadent calculations, based on the Kramers-HeisenbereDmc relationship, and experimental data obtained earlier by Strempel and Kiefer. A symmetry principle for corresponding Stokes and antiStokes Raman spectra is also'demonstrated and the corm sponding spectra for this principle were simulated applying both timedependent and timeindependent theory. Further aspects such as the reflection principle and scattering delay times are discussed and compared with results obtained for 79Br2.

Continuum resonance Raman scattering in isotopically pure127I35Cl

“…In addition we have derived information on the time evolution of the scattering process and scattering delay times were given by means of time dependent calculations. The values of the scattering delay times are similar (a few fs) to those for 12 [47] and Br 2 [35]. …”

“…In table 2 the continuum resonance Raman delay times for the fundamental, hot band and overtone transitions are given. As can be recognized the scattering delay times are in the same range as those for the halogen molecules 12 and Br2 (for comparison see [35] and [47]). It is of interest to demonstrate how the intensities of the various vibrational transitions develop in time while the wavepackets propagate on the excited state potential functions.…”

“…In another recent theoretical study [47] we have applied the time dependent approach to continuum resonance Raman scattering in iodine and have derived scattering delay times "r for the fundamental transition, hot bands and overtones. We found values for ~-in the range between 10fs and 25fs depending on the particular vibrational transition.…”

On the limitations of adiabatic population transfer between molecular electronic states induced by intense femtosecond laser pulses

“…Motivated by recent experiments on gaseous I 2 molecules, 8 we here study the ͉B͘ ← ͉X͘ transition in the iodine molecule 9-11 which is extremely well characterized by linear 12 and resonance Raman spectroscopy. 13 As an isolated system, it has also been used to, e.g., establish femtosecond fluorescence spectroscopy, 14 Femtosecond time-resolved four-wave mixing experiments on I 2 were first performed at the University of Würzburg, [19][20][21][22] and later at other places. [23][24][25] In Fig.…”