Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP
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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Aug 24, 2020
- Source ID
- 10.1063/5.0017790
Entities
People
- David D Grimes
- H. Herburger
- Jun Jiang
- Robert W. Field
- Timothy James Barnum
Organizations
- Air Force Office of Scientific Research
- Division of Chemistry
- ETH Zurich
- Massachusetts Institute of Technology