Quantum transition probabilities due to overlapping electromagnetic pulses: Persistent differences between Dirac's form and nonadiabatic perturbation theory.

The probability of transition to an excited state of a quantum system in a time-dependent electromagnetic field determines the energy uptake from the field. The standard expression for the transition probability has been given by Dirac. Landau and Lifshitz suggested, instead, that the adiabatic effects of a perturbation should be excluded from the transition probability, leaving an expression in terms of the nonadiabatic response. In our previous work, we have found that these two approaches yield different results while a perturbing field is acting on the system. Here, we prove, for the first time, that differences between the two approaches may persist after the perturbing fields have been completely turned off. We have designed a pair of overlapping pulses in order to establish the possibility of lasting differences, in a case with dephasing. Our work goes beyond the analysis presented by Landau and Lifshitz, since they considered only linear response and required that a constant perturbation must remain as t → ∞. First, a "plateau" pulse populates an excited rotational state and produces coherences between the ground and excited states. Then, an infrared pulse acts while the electric field of the first pulse is constant, but after dephasing has occurred. The nonadiabatic perturbation theory permits dephasing, but dephasing of the perturbed part of the wave function cannot occur within Dirac's method. When the frequencies in both pulses are on resonance, the lasting differences in the calculated transition probabilities may exceed 35%. The predicted differences are larger for off-resonant perturbations.