32 research outputs found
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