Characterization of the 3dδ Rydberg state of MgAr⁺ using a quantum-control optical scheme
(2021) Physical Review A — Vol. 104, n° 4, p. 42811 (2021)
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- Authors
Wehrli, D. 
Berglitsch, T. Merkt, F.
- Abstract
- We report a spectroscopic investigation of the 3dδ_ (_ = 3 2 , 5 2 ) Rydberg states of theMgAr+ molecular cation. Vibrational levels of the 3dδ3/2 spin-orbit component with v _ 15 were observed to directly predissociate into charge-transfer continua correlating to the Mg(3s2 1S) + Ar+(3p5 2P) dissociation limit, making it possible to record their spectra by isolated-core multiphoton Rydberg dissociation spectroscopy. Vibrational states below v = 15, which do not predissociate, were characterized with partial rotational resolution using a multiphoton excitation and dissociation quantum-control scheme that radiatively couples the 3dδ vibronic states to predissociative levels of the 3dπ state. An effective Hamiltonian approach was used to theoretically investigate this scheme, including the origin of the control over the spectral lineshapes provided by the laser detuning. This approach provided results in quantitative agreement with the measured spectra. Potential-energy functions were derived for the 3dδ_ states from experimental data. They are very similar to the one of the X2+ 1_ + ground state of the MgAr2+ doubly charged ion, highlighting the Rydberg character of the 3dδ state. Whereas homogeneous charge-transfer interactions play a major role in the dynamics of the Rydberg states of molecular ions, the present study shows that heterogeneous interactions leave these states essentially unaffected.
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Génévriez, M., Wehrli, D., Berglitsch, T., & Merkt, F. (2021). Characterization of the 3dδ Rydberg state of MgAr⁺ using a quantum-control optical scheme. Physical Review A, 104(4), 42811. https://doi.org/10.1103/physreva.104.042811 (Original work published 2021)