Characterization of the 3dδ Rydberg state of MgAr+ using a quantum-control optical scheme
Open access
Date
2021-10Type
- Journal Article
Abstract
We report a spectroscopic investigation of the 3dδΩ (Ω=32,52) Rydberg states of the MgAr+ 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(3s21S) + Ar+(3p52P) 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 3dδΩ states from experimental data. They are very similar to the one of the X2+1Σ+ 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. Show more
Permanent link
https://doi.org/10.3929/ethz-b-000513781Publication status
publishedExternal links
Journal / series
Physical Review AVolume
Pages / Article No.
Publisher
American Physical SocietyOrganisational unit
03449 - Merkt, Frédéric / Merkt, Frédéric
Funding
200478 - Precision measurements with cold molecules: Rydberg states, ions and photoionization (SNF)
743121 - Cold Ion Chemistry - Experiments within a Rydberg Orbit (EC)
More
Show all metadata