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Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP
T J Barnum1, H Herburger2, D D Grimes1
1Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
The Journal of Chemical Physics
|September 3, 2020
Summary
Researchers selectively excite high-orbital angular momentum (ℓ) Rydberg states in atoms. This method minimizes decay, extending state lifetimes and enabling study of complex molecular Rydberg states.
Area of Science:
- Atomic and Molecular Physics
- Quantum Chemistry
Background:
- Studying molecular Rydberg states is difficult due to rapid non-radiative decay pathways like predissociation.
- Exciting Rydberg states with high orbital angular momentum (ℓ ≳ 3) can minimize decay and prolong state lifetimes.
Purpose of the Study:
- To demonstrate a method for selectively populating high-ℓ Rydberg states.
- To investigate the potential of this method for studying molecular Rydberg states.
Main Methods:
- Utilized stimulated Raman adiabatic passage (STIRAP) to transfer population.
- Employed optical and millimeter-wave fields to couple initial, intermediate (nd), and final (nf) Rydberg states.
- Performed numerical simulations to analyze population transfer dynamics.
Main Results:
- Successfully transferred population to an nf Rydberg state of the calcium atom.
- Numerical simulations accurately reproduced experimental observations of population transfer.
- The method shows promise for populating high-ℓ Rydberg states.
Conclusions:
- Selective excitation of high-ℓ Rydberg states is achievable using STIRAP.
- This technique offers a viable route to stabilize and study molecular Rydberg states.
- The approach has broad implications for quantum chemistry and atomic physics research.
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