Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP.
- Barnum TJ Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
- Herburger H Laboratorium für Physikalische Chemie, ETH Zürich, Vladimir-Prelog-Weg 2, 8093 Zürich, Switzerland.
- Grimes DD Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
- Jiang J Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
- Field RW Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
- 2020-09-03
Published in:
- The Journal of chemical physics. - 2020
English
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.
- Language
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- English
- Open access status
- green
- Identifiers
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- DOI 10.1063/5.0017790
- PMID 32872887
- Persistent URL
- https://sonar.ch/global/documents/139913
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