Multi-Channel Selective Femtosecond Coherent Control Based on Symmetry Properties

We present and implement a new scheme for extended multi-channel selective femtosecond coherent control based on symmetry properties of the excitation channels. Here, an atomic non-resonant two-photon absorption channel is coherently incorporated in a resonance-mediated (2+1) three-photon absorption channel. By proper pulse shaping, utilizing the invariance of the two-photon absorption to specific phase transformations of the pulse, the three-photon absorption is tuned independently over order-of-magnitude yield range for any possible two-photon absorption yield. Noticeable is a set of two-photon dark pulses inducing widely-tunable three-photon absorption

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

Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.Comment: 25 pages, 5 figure

Enhancement of Intermediate-Field Two-Photon Absorption by Rationally-Shaped Femtosecond Pulses

We extend the powerful frequency-domain analysis of femtosecond two-photon absorption to the intermediate-field regime, which involves both two- and four-photon transitions. Consequently, we find a broad family of shaped pulses that enhance the absorption over the transform-limited pulse. It includes any spectral phase that is anti-symmetric around half the transition frequency. The spectrum is asymmetric around it. The theoretical framework and results for Na are verified experimentally. This work opens the door for rational femtosecond coherent control in a regime of considerable absorption yields