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Journal of the Optical Society of America B

Multiphoton Excitation by Adiabatic Following

F. T. Hioe, Joseph H. Eberly

Published Jan 1, 1984• 0 citations
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Pulsed multiphoton excitation of atoms

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•Jan 1, 1985•0 citations
We study the dynamics of multiphoton-absorption chirped adiabatic passage (CHIRAP) in atoms, and show that the dynamics of the excited-state fine-structure transitions can be nonadiabatic even though the optical transfer to the highly excited electronic states is fully adiabatic. Hence, care must be taken to ensure that the dynamics is selective if multiphoton-absorption CHIRAP is to be used as a pump- ing mechanism to populate very-high-lying states that can serve as the pumping levels for uv lasers. We investigate the dynamics as a function of chirp rate and field intensity in the 5s 2^{2}2S1/2{\mathit{S}}_{1/2}S1/2​\ensuremath{\rightarrow}5p 2^{2}2P3/2{\mathit{P}}_{3/2}P3/2​\ensuremath{\rightarrow}5d 2^{2}2D3/2{\mathit{D}}_{3/2}D3/2​,5d 2^{2}2D5/2{\mathit{D}}_{5/2}D5/2​ rubidium system, and show that selectivity can be maintained despite the near degeneracy of the 2^{2}2D manifold.
Shaped free electron vortices (SEVs) have recently been studied using atomic ( 1 + 2 ) resonance-enhanced multiphoton ionization (REMPI) by oppositely chirped counterrotating circularly polarized (OC-CRCP) femtosecond laser pulses. By transitioning from the perturbative to the nonperturbative REMPI regime, we identify an adiabatic excitation mechanism in a resonant V-type three-level system, termed V-RAP due to its similarities to rapid adiabatic passage (RAP). Experimentally, we observe a pronounced change in the shape of the measured three-dimensional (3D) photoelectron momentum distribution (PMD), which we trace back to this mechanism via analytical calculations and numerical simulations of the bound state and ionization dynamics. In V-RAP, the atom adiabatically follows the OC-CRCP field, with the two excited states driven in antiphase, leading to an adiabatic cancellation of specific ionization pathways and explaining the observed changes in the PMD. In the experiment, we combine supercontinuum polarization pulse shaping to generate OC-CRCP femtosecond laser pulses with velocity map imaging-based photoelectron tomography to reconstruct the 3D PMD. The reconstructed PMDs are decomposed by 3D Fourier analysis into SEVs of different rotational symmetry, revealing a significant enhancement of the c 6 -symmetric contribution, which is the signature of the V-RAP.
We develop a multiphoton adiabatic passage to realize a highly efficient Rydberg excitation in a four-level ladder-type atomic system. The adiabatic passage is based on the existence of a novel quasidark state in the cascade excitation system where the frequencies of the lasers are appropriately chirped with time. We also investigate the influence of the interatomic Rydberg interaction on the passage and extend its application to the preparation of antiblockade Rydberg atom pairs in the Rydberg blockade regime.