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

Barnum, T. J.; Herburger, H.; Grimes, D. D.; Jiang, J.; Field, R. W.

doi:10.1063/5.0017790

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

Journal Article · Mon Aug 24 00:00:00 EDT 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0017790· OSTI ID:1668488

^[1]; Herburger, H. ^[2]; ^[1]; ^[1]; ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
Eidgenoessische Technische Hochschule, Zurich (Switzerland). Lab. für Physikalische Chemie

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. Here, 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR); USDOE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1668488

Alternate ID(s):: OSTI ID: 1831790

Report Number(s):: LLNL-JRNL--811388; 1018144

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 8 Vol. 153; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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