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arXiv:2506.05177 · Physical Review A

Adiabatic dynamics in a V-type quantum system by oppositely chirped counterrotating circularly polarized laser pulses

D. Köhnke, Tim Bayer, M. Wollenhaupt

Published Jul 15, 2025• 0 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/78w7-wc89

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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.
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The chirped-pulse interaction in the adiabatic coupling regime induces cyclic permutations of the energy states of a three-level system in the VVV-type configuration, which process is known as the three-level chirped rapid adiabatic passage (RAP). Here we show that a spectral hole in a chirped pulse can turn on or off the level mixing at adiabatic crossing points of this process, reducing the system to an effective two-level system. The given hybrid adiabatic-nonadiabatic transition enables selective excitation of the three-level system, controlled by the laser intensity and spectral position of the hole, as well as the sign of the chirp parameter. Experiments performed with shaped femtosecond laser pulses and the three lowest energy levels (5S1/25{S}_{1/2}5S1/2​, 5P1/25{P}_{1/2}5P1/2​, and 5P3/25{P}_{3/2}5P3/2​) of atomic rubidium (Rb)(\mathrm{Rb})(Rb) show good agreement with the theoretically analyzed dynamics. The result indicates that our method, when being combined with the ordinary chirped RAP, implements an adiabatic transition between the Raman-coupled excited states. Furthermore, our laser intensity-dependent control may have applications including selective excitations of atoms or ions arranged in space when being used in conjunction with laser beam profile programming.
We present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2 + 1 + 1 resonance enhanced multi-photon ionization (REMPI) proceeds via the strongly driven two-photon transition 4s←←3s, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3 + 1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark shifts and level crossings. In particular, we show that under the experimental conditions the passage through an uncommon three-state 'bow-tie' level crossing allows the preparation of coherent superposition states.
Polarization-tailored bichromatic femtosecond laser fields with cycloidal polarization profiles have emerged as a powerful tool for coherent control of quantum processes. We present an optical scheme to create and manipulate three-dimensional free electron wave packets with arbitrary rotational symmetry by combining advanced supercontinuum pulse shaping with high resolution photoelectron tomography. Here we use carrier-envelope phase-stable polarization-tailored bichromatic (3ω:4ω) counter- and corotating femtosecond laser pulses to generate 7-fold rotational symmetric and asymmetric photoelectron momentum distributions by multiphoton ionization of sodium atoms. To elucidate the physical mechanisms, we investigate the interplay between the symmetry properties of the driving field and the resulting electron wave packets by varying the optical field parameters. Our results show that the symmetry properties of electron wave packets are not fully determined by the field symmetry, but completely described by multipath quantum interference of states with different angular momenta.