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Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP

Author(s)
Barnum, Timothy James; Herburger, H.; Grimes, David Darrah; Jiang, Jun; Field, Robert W
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Abstract
Rydberg states of molecules are intrinsically challenging to study due to the presence of fast non-radiative decay pathways, such as predissociation. However, selectively exciting Rydberg states with values of the orbital angular momentum (ℓ) ℓ ≳ 3 is a productive strategy to minimize this rapid decay and to populate molecular Rydberg states with lifetimes that approach those of atoms. In this proof-of-principle demonstration, we transfer population to an nf Rydberg state of the calcium atom by stimulated Raman adiabatic passage, in which an optical and a millimeter-wave field couple the initial and final states via an intermediate nd Rydberg state. Numerical simulations reproduce the observed time and frequency dependences of the population transfer and suggest the utility of this scheme to populate high-ℓ Rydberg states of molecules. ©2020
Date issued
2020-08
URI
https://hdl.handle.net/1721.1/128202
Department
Massachusetts Institute of Technology. Department of Chemistry
Journal
The Journal of chemical physics
Publisher
AIP Publishing
Citation
Barnum, T. J. et al., "Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP." Journal of Chemical Physics 153, 8 (August 2020): 084301 doi. 10.1063/5.0017790 ©2020 Authors
Version: Author's final manuscript
ISSN
1089-7690

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