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Title: 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. 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.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
  2. Eidgenoessische Technische Hochschule, Zurich (Switzerland). Lab. für Physikalische Chemie
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1668488
Report Number(s):
LLNL-JRNL-811388
Journal ID: ISSN 0021-9606; 1018144
Grant/Contract Number:  
AC52-07NA27344; CHE-1800410; FA9550-16-1-0117; 1122374
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 153; Journal Issue: 8; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
Rydberg states; coherent control; millimeter wave spectrum; dark states

Citation Formats

Barnum, T. J., Herburger, H., Grimes, D. D., Jiang, J., and Field, R. W. Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP. United States: N. p., 2020. Web. doi:10.1063/5.0017790.
Barnum, T. J., Herburger, H., Grimes, D. D., Jiang, J., & Field, R. W. Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP. United States. doi:10.1063/5.0017790.
Barnum, T. J., Herburger, H., Grimes, D. D., Jiang, J., and Field, R. W. Mon . "Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP". United States. doi:10.1063/5.0017790.
@article{osti_1668488,
title = {Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP},
author = {Barnum, T. J. and Herburger, H. and Grimes, D. D. and Jiang, J. and Field, R. W.},
abstractNote = {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.},
doi = {10.1063/5.0017790},
journal = {Journal of Chemical Physics},
number = 8,
volume = 153,
place = {United States},
year = {2020},
month = {8}
}

Journal Article:
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