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Coherent control of femtosecond two-photon absorption in theintermediate-field regime is analyzed in detail in the powerful frequencydomain using an extended 4th-order perturbative description. The correspondingabsorption is coherently induced by the weak-field non-resonant two-photontransitions as well as by four-photon transitions involving three absorbedphotons and one emitted photons. The interferences between these two groups oftransitions lead to a difference between the intermediate-field and weak-fieldabsorption dynamics. The corresponding interference nature (constructive ordestructive) strongly depends on the detuning direction of the pulse spectrumfrom half the two-photon transition frequency. The model system of the study isatomic sodium, for which both experimental and theoretical results areobtained. The detailed understanding obtained here serves as a basis forcoherent control with rationally-shaped femtosecond pulses in a regime ofsizable absorption yields.

Frequency-Domain Coherent Control of Femtosecond Two-Photon Absorption: Intermediate-Field vs. Weak-Field Regime