Role of quadratic and cubic spectral phases in ladder climbing with ultrashort pulses

Two-photon excitation of a quantum ladder system by an ultrashort chirped pulse leads to interferences in the excited-state population, between direct and sequential paths. Experimental results have been obtained in atomic sodium vapor. The presence of several intermediate and final states leads to new phenomena. The interplay between the two sequential paths leads to strongly contrasted oscillations and a large enhancement of the transition probability for precise values of the chirp. A cubic spectral phase modifies significantly the behavior of the quantum interferences and can be used to enhance the two-photon absorption rate.