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:
-
[1];
[1];
[1];
[1]
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
- Eidgenoessische Technische Hochschule, Zurich (Switzerland). Lab. für Physikalische Chemie
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (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
- Alternate Identifier(s):
- OSTI ID: 1831790
- Report Number(s):
- LLNL-JRNL-811388
Journal ID: ISSN 0021-9606; 1018144; TRN: US2203701
- 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:
- 74 ATOMIC AND MOLECULAR PHYSICS; 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. https://doi.org/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. https://doi.org/10.1063/5.0017790. https://www.osti.gov/servlets/purl/1668488.
@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 = {Mon Aug 24 00:00:00 EDT 2020},
month = {Mon Aug 24 00:00:00 EDT 2020}
}
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Works referenced in this record:
Coherent laser-millimeter-wave interactions en route to coherent population transfer
journal, October 2017
- Grimes, David D.; Barnum, Timothy J.; Zhou, Yan
- The Journal of Chemical Physics, Vol. 147, Issue 14
Stimulated Raman adiabatic passage among degenerate-level manifolds
journal, November 2004
- Kis, Z.; Karpati, A.; Shore, B. W.
- Physical Review A, Vol. 70, Issue 5
Rydberg-State-Enabled Deceleration and Trapping of Cold Molecules
journal, September 2009
- Hogan, S. D.; Seiler, Ch.; Merkt, F.
- Physical Review Letters, Vol. 103, Issue 12
Population transfer between molecular vibrational levels by stimulated Raman scattering with partially overlapping laser fields. A new concept and experimental results
journal, May 1990
- Gaubatz, U.; Rudecki, P.; Schiemann, S.
- The Journal of Chemical Physics, Vol. 92, Issue 9
Creation of Polar and Nonpolar Ultra-Long-Range Rydberg Molecules
journal, September 2000
- Greene, Chris H.; Dickinson, A. S.; Sadeghpour, H. R.
- Physical Review Letters, Vol. 85, Issue 12
High resolution laser spectroscopy of NO: The A , v =1 state and a series of n f , v =1 Rydberg states
journal, September 1988
- Biernacki, D. Therese; Colson, Steven D.; Eyler, E. E.
- The Journal of Chemical Physics, Vol. 89, Issue 5
Optical phase perturbations in nanosecond pulsed amplification and second-harmonic generation
journal, January 1994
- Gangopadhyay, S.; Melikechi, N.; Eyler, E. E.
- Journal of the Optical Society of America B, Vol. 11, Issue 1
Towards measuring the ionisation and dissociation energies of molecular hydrogen with sub-MHz accuracy
journal, January 2011
- Sprecher, Daniel; Jungen, Christian; Ubachs, Wim
- Faraday Discussions, Vol. 150
The Predissociation Mechanism for2Σ+Rydberg States of CaCl
journal, February 1999
- Clevenger, Jason O.; Harris, Nicole A.; Field, Robert W.
- Journal of Molecular Spectroscopy, Vol. 193, Issue 2
Chirped-pulse millimeter-wave spectroscopy: Spectrum, dynamics, and manipulation of Rydberg–Rydberg transitions
journal, January 2013
- Colombo, Anthony P.; Zhou, Yan; Prozument, Kirill
- The Journal of Chemical Physics, Vol. 138, Issue 1
Demonstration of Three-Dimensional Electrostatic Trapping of State-Selected Rydberg Atoms
journal, January 2008
- Hogan, S. D.; Merkt, F.
- Physical Review Letters, Vol. 100, Issue 4
Very high resolution spectroscopy of high Rydberg states of the argon atom
journal, June 1998
- Merkt, F.; Schmutz, H.
- The Journal of Chemical Physics, Vol. 108, Issue 24
Hot spot detection in a focused 10.6μm laser beam using silver halide films
journal, October 1978
- Mitchel, G.; Grek, B.; Martin, F.
- Journal of Physics D: Applied Physics, Vol. 11, Issue 14
Coherent population transfer of ground-state atoms into Rydberg states
journal, August 2005
- Cubel, T.; Teo, B. K.; Malinovsky, V. S.
- Physical Review A, Vol. 72, Issue 2
Resonance between electronic and rotational motions in Rydberg states of CaF
journal, June 2007
- Kay, Jeffrey J.; Altunata, Serhan N.; Coy, Stephen L.
- Molecular Physics, Vol. 105, Issue 11-12
A High Phase-Space-Density Gas of Polar Molecules
journal, October 2008
- Ni, K. -K.; Ospelkaus, S.; de Miranda, M. H. G.
- Science, Vol. 322, Issue 5899
Coherent population transfer in NO with pulsed lasers: the consequences of hyperfine structure, doppler broadening aaand electromagnetically induced absorption
journal, January 1998
- Kuhn, A.; Steuerwald, S.; Bergmann, K.
- The European Physical Journal D - Atomic, Molecular and Optical Physics, Vol. 1, Issue 1
Direct detection of Rydberg–Rydberg millimeter-wave transitions in a buffer gas cooled molecular beam
journal, November 2015
- Zhou, Yan; Grimes, David D.; Barnum, Timothy J.
- Chemical Physics Letters, Vol. 640
Adiabatic population transfer in the three-level Λ-system: two-photon lineshape
journal, August 1997
- Romanenko, V. I.; Yatsenko, L. P.
- Optics Communications, Vol. 140, Issue 4-6
Landau-Zener transitions and population transfer in a three-level system driven by two delayed laser pulses
journal, July 1994
- Danileiko, M. V.; Romanenko, V. I.; Yatsenko, L. P.
- Optics Communications, Vol. 109, Issue 5-6
Stimulated Raman adiabatic passage preparation of a coherent superposition of ThO states for an improved electron electric-dipole-moment measurement
journal, May 2016
- Panda, C. D.; O'Leary, B. R.; West, A. D.
- Physical Review A, Vol. 93, Issue 5
Coherent population transfer and dark resonances in SO 2
journal, May 1996
- Halfmann, T.; Bergmann, K.
- The Journal of Chemical Physics, Vol. 104, Issue 18
Rotational structure and dissociation of the Rydberg states of CO investigated by ion‐dip spectroscopy
journal, August 1995
- Komatsu, Masaaki; Ebata, Takayuki; Maeyama, Toshihiko
- The Journal of Chemical Physics, Vol. 103, Issue 7
Rotationally resolved photoelectron spectra from vibrational autoionization of NO Rydberg levels
journal, February 1997
- Park, Hongkun; Zare, Richard N.
- The Journal of Chemical Physics, Vol. 106, Issue 6
Analysis of vibrational autoionization of CaF Rydberg states
journal, April 2019
- Jiang, Jun; Barnum, Timothy J.; Coy, Stephen L.
- The Journal of Chemical Physics, Vol. 150, Issue 15
Three‐color triple resonance spectroscopy of highly excited ng Rydberg states of NO: Decay dynamics of high‐ l Rydberg states
journal, October 1995
- Fujii, Asuka; Morita, Norio
- The Journal of Chemical Physics, Vol. 103, Issue 14
Determination of dipole and quadrupole polarizabilities of by fine-structure measurements in high- Rydberg states of magnesium
journal, May 2008
- Snow, E. L.; Lundeen, S. R.
- Physical Review A, Vol. 77, Issue 5
Lifetimes of Rydberg states in zero‐electron‐kinetic‐energy experiments. I. Electric field induced and collisional enhancement of NO predissociation lifetimes
journal, June 1995
- Vrakking, Marc J. J.; Lee, Yuan T.
- The Journal of Chemical Physics, Vol. 102, Issue 22
Direct Observation of Rydberg-Rydberg Transitions via Cpmmw Spectroscopy
conference, June 2014
- Zhou, Yan; Field, Robert; Barnum, Timothy
- Proceedings of the 69th International Symposium on Molecular Spectroscopy
An arbitrary waveform generator based chirped pulse Fourier transform spectrometer operating from 260 to 295GHz
journal, October 2012
- Steber, Amanda L.; Harris, Brent J.; Neill, Justin L.
- Journal of Molecular Spectroscopy, Vol. 280