Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Bulletin of the American Physical Society

Computational analysis of population transfer via STIRAP in sodium vapor

Matt Tilley, Jerald B. Johnson, Chakree Tanjaroon, Susan Davis Allen

Published Jun 5, 2012• 0 citations
OpenAlex

Abstract

We present a theoretical and computational analysis of STIRAP and SEP population transfer in sodium vapor as measured by fluorescence emission imaged onto a spectrometer. Calculations include 1) a careful analysis of the fraction of measured fluorescence output over all spatial positions in the incident beams and due to experimental geometry, 2) calculations of an unexpectedly strong effect on the STIRAP transfer efficiency with beams detuned between the D1 and D2 Fraunhofer lines, 3) a study of the relative efficiency of STIRAP and SEP on resonance at the D1 and D2 transitions, 4) the effects of varying pulse parameters (such as spatial shape, energy, focus) on transfer efficiencies, and 5) explorations of population transfer in sodium as a function of the pump-Stokes energy landscape. The system states are calculated utilizing a Hamiltonian which includes fine and hyperfine structure (two nine-state and four five-state transitions) of the 3s, 3p and 5s levels in sodium. The findings are compared to experimental results obtained using a picosecond laser system with linewidth very near the transform-limit (±15%).

Related papers

STIRAP on sodium vapor with picosecond pulses: calculations and experiment

Jerald B. Johnson, Chakree Tanjaroon, Jim L. Hicks +1 more

Calculations of STIRAP transfer efficiencies were made on sodium starting from the eight hyperfine states of the 3s (2S1/2) electronic ground state, passing through the eight hyperfine states of the 3p (2P1/2) and/or fourteen of the sixteen hyperfine states of the 3p (2P3/2) to the eight hyperfine states of the 5s (2S1/2) state. Linearly polarized light was used in calculations and experiment leading to six independent sets of coupled states (four sets of five states and two sets of nine states). Calculations were made for laser pulses several picoseconds in length and compared with experiment. Although the linewidth of the laser pulses used in both computation and experiment was a small fraction of the fine structure splitting between the 3p states, both fine-structure states were observed to contribute to the STIRAP transfer efficiency. A rich set of results was found including oscillations similar to the Rabi oscillations observed in two-state systems when the pump and Stokes pulses were tuned to wavelengths between the two 3p states.

Bulletin of the American Physical Society•Jun 16, 2011•0 citations

Picosecond multiphoton STIRAP detection of gas phase species: a test with sodium

Jerald B. Johnson, Susan Davis Allen, Daniel R. Britton +4 more

Laser detection technologies offer obvious benefits for the standoff detection of hazardous or energetic materials where safe detection at a distance is the goal. Of the many optical standoff detection methods available, multiphoton fluorescence techniques have been studied less extensively. Multiphoton fluorescence allows high selectivity relative to the background while preserving the larger signal of laser induced fluorescence (LIF). Using sodium vapor as a test system, we demonstrate that stimulated Raman adiabatic passage (STIRAP) is capable of providing more than a factor of ten improvement in population transfer efficiency to the final state when compared to stimulated emission pumping (SEP). The two sodium transitions used are the 3p (2P1/2) ← 3s (2S1/2) and 5s (2S1/2) ← 3p (2P1/2). The light used to couple the states was produced with two synchronously pumped OPG/OPAs pumped by the 355 nm light from a picosecond tripled Nd:YAG.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Apr 21, 2009•4 citations

Stimulated Raman adiabatic passage in sodium vapor with picosecond laser pulses

Jim L. Hicks, Chakree Tanjaroon, Susan Davis Allen +3 more

Experimental measurements and calculations of stimulated Raman adiabatic passage transfer efficiencies were made on a sodium gas starting from the $3{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}$ electronic ground state, passing through the $3{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{1/2}$ and/or the $3{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}$ to the $5{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}$ state. The lasers used in the experiments had a pulse width of several picoseconds and were close to the Fourier transform limit. Although the linewidth of the laser was much smaller than the spin orbit splitting between the $3\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}$ and $3\phantom{\rule{0.16em}{0ex}}^{2}P_{3/2}$ states, Experiments and calculations reveal that both 3p states play a role in the transfer efficiency when the lasers are tuned to resonance through the $3{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{1/2}$ state, revealing evidence of quantum interference between the competing pathways.

arXiv:1510.04334•Physical Review A•Aug 1, 2017•1 citation

STIRAP on sodium gas as a function of argon buffer gas pressure

Jerald B. Johnson, Susan Davis Allen, Jim L. Hicks +1 more

The standoff detection of energetic materials via laser-induced fluorescence of vapors has received relatively little attention due to spectrally broad fluorescence emission from aerosols and unwanted background molecules. This unwanted broad emission can obscure fluorescence from the molecule of interest. When multiphoton excitation is used, the problem can be avoided by blue-shifting the emission from the target molecule relative to the unwanted broad emission. As a precursor to the detection of explosives, we demonstrate coherent multiphoton excitation via stimulated Raman adiabatic passage (STIRAP) on sodium vapor in an argon buffer gas as a function of argon pressure. Results indicate that STIRAP can be performed in a buffer gas at atmospheric pressure with a minimal eduction in STIRAP efficiency. The 15 ps long light pulses used for the pump and Stokes pulses were produced by two synchronously pumped OPO/OPAs tuned to the 3p (2P1/2) ← 3s (2S1/2) transition for the pump pulse and the 5s (2S1/2) ← 3p (2P1/2) for the Stokes pulse.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Apr 23, 2010•3 citations

Population transfer by stimulated Raman scattering with delayed pulses: Analytical results for multilevel systems

George W. Coulston, Klaas Bergmann

Stimulated Raman scattering involving adiabatic passage (STIRAP) is a proven technique for population transfer in three-level systems with strong oscillator strengths. We show that the STIRAP process should also yield high transfer efficiencies when the densities of states near the intermediate and final levels are high, provided certain criteria for the experimentally controllable parameters are met. We also show that high transfer efficiencies may even be possible when the pump and Stokes lasers can access levels outside of the three-level system. The criteria are derived with an approach that emphasizes the adiabatic nature of the transfer process in an eigenvector of the interaction Hamiltonian that resembles a trapped state. The results are compared to density matrix calculations.

The Journal of Chemical Physics•Mar 1, 1992•126 citations

Population transfer by stimulated Raman scattering with delayed pulses and by the stimulated-emission pumping method: a comparative study

Guo‐Zhong He, Axel Kuhn, S. Schiemann +1 more

The characteristics of the stimulated-emission pumping (SEP) method and the technique of stimulated Raman scattering by delayed pulses (STIRAP) are compared, based on numerical results from density matrix calculations. The latter technique requires the use of nearly transform-limited pulses, whereas the former method is successfully implemented with broadband lasers. Damping coefficients γ are introduced to model the consequences of phase fluctuations of the radiation. It is shown that the various techniques can be classified in terms of the delay D of the Stokes laser relative to the pump laser and the damping rate γ. The delay D/ΔτL ≈ −1 and γ = 0 corresponds to the STIRAP mode of operation, whereas the SEP method requires that D/ΔτL ≥ 0 and γΔτL ≫ 1, where ΔτL is the width of the laser pulse.

Journal of the Optical Society of America B•Sep 1, 1990•60 citations
We present a theoretical and computational analysis of STIRAP and SEP population transfer in sodium vapor as measured by fluorescence emission imaged onto a spectrometer. Calculations include 1) a careful analysis of the fraction of measured fluorescence output over all spatial positions in the incident beams and due to experimental geometry, 2) calculations of an unexpectedly strong effect on the STIRAP transfer efficiency with beams detuned between the D1 and D2 Fraunhofer lines, 3) a study of the relative efficiency of STIRAP and SEP on resonance at the D1 and D2 transitions, 4) the effects of varying pulse parameters (such as spatial shape, energy, focus) on transfer efficiencies, and 5) explorations of population transfer in sodium as a function of the pump-Stokes energy landscape. The system states are calculated utilizing a Hamiltonian which includes fine and hyperfine structure (two nine-state and four five-state transitions) of the 3s, 3p and 5s levels in sodium. The findings are compared to experimental results obtained using a picosecond laser system with linewidth very near the transform-limit (±15%).
Calculations of STIRAP transfer efficiencies were made on sodium starting from the eight hyperfine states of the 3s (2S1/2) electronic ground state, passing through the eight hyperfine states of the 3p (2P1/2) and/or fourteen of the sixteen hyperfine states of the 3p (2P3/2) to the eight hyperfine states of the 5s (2S1/2) state. Linearly polarized light was used in calculations and experiment leading to six independent sets of coupled states (four sets of five states and two sets of nine states). Calculations were made for laser pulses several picoseconds in length and compared with experiment. Although the linewidth of the laser pulses used in both computation and experiment was a small fraction of the fine structure splitting between the 3p states, both fine-structure states were observed to contribute to the STIRAP transfer efficiency. A rich set of results was found including oscillations similar to the Rabi oscillations observed in two-state systems when the pump and Stokes pulses were tuned to wavelengths between the two 3p states.
Laser detection technologies offer obvious benefits for the standoff detection of hazardous or energetic materials where safe detection at a distance is the goal. Of the many optical standoff detection methods available, multiphoton fluorescence techniques have been studied less extensively. Multiphoton fluorescence allows high selectivity relative to the background while preserving the larger signal of laser induced fluorescence (LIF). Using sodium vapor as a test system, we demonstrate that stimulated Raman adiabatic passage (STIRAP) is capable of providing more than a factor of ten improvement in population transfer efficiency to the final state when compared to stimulated emission pumping (SEP). The two sodium transitions used are the 3p (2P1/2) ← 3s (2S1/2) and 5s (2S1/2) ← 3p (2P1/2). The light used to couple the states was produced with two synchronously pumped OPG/OPAs pumped by the 355 nm light from a picosecond tripled Nd:YAG.
Experimental measurements and calculations of stimulated Raman adiabatic passage transfer efficiencies were made on a sodium gas starting from the 32S1/23{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}32S1/2​ electronic ground state, passing through the 32P1/23{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{1/2}32P1/2​ and/or the 32P3/23{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{3/2}32P3/2​ to the 52S1/25{\phantom{\rule{0.16em}{0ex}}}^{2}{S}_{1/2}52S1/2​ state. The lasers used in the experiments had a pulse width of several picoseconds and were close to the Fourier transform limit. Although the linewidth of the laser was much smaller than the spin orbit splitting between the 32P1/23\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}32P1/2​ and 32P3/23\phantom{\rule{0.16em}{0ex}}^{2}P_{3/2}32P3/2​ states, Experiments and calculations reveal that both 3p states play a role in the transfer efficiency when the lasers are tuned to resonance through the 32P1/23{\phantom{\rule{0.16em}{0ex}}}^{2}{P}_{1/2}32P1/2​ state, revealing evidence of quantum interference between the competing pathways.
The standoff detection of energetic materials via laser-induced fluorescence of vapors has received relatively little attention due to spectrally broad fluorescence emission from aerosols and unwanted background molecules. This unwanted broad emission can obscure fluorescence from the molecule of interest. When multiphoton excitation is used, the problem can be avoided by blue-shifting the emission from the target molecule relative to the unwanted broad emission. As a precursor to the detection of explosives, we demonstrate coherent multiphoton excitation via stimulated Raman adiabatic passage (STIRAP) on sodium vapor in an argon buffer gas as a function of argon pressure. Results indicate that STIRAP can be performed in a buffer gas at atmospheric pressure with a minimal eduction in STIRAP efficiency. The 15 ps long light pulses used for the pump and Stokes pulses were produced by two synchronously pumped OPO/OPAs tuned to the 3p (2P1/2) ← 3s (2S1/2) transition for the pump pulse and the 5s (2S1/2) ← 3p (2P1/2) for the Stokes pulse.
Stimulated Raman scattering involving adiabatic passage (STIRAP) is a proven technique for population transfer in three-level systems with strong oscillator strengths. We show that the STIRAP process should also yield high transfer efficiencies when the densities of states near the intermediate and final levels are high, provided certain criteria for the experimentally controllable parameters are met. We also show that high transfer efficiencies may even be possible when the pump and Stokes lasers can access levels outside of the three-level system. The criteria are derived with an approach that emphasizes the adiabatic nature of the transfer process in an eigenvector of the interaction Hamiltonian that resembles a trapped state. The results are compared to density matrix calculations.
The characteristics of the stimulated-emission pumping (SEP) method and the technique of stimulated Raman scattering by delayed pulses (STIRAP) are compared, based on numerical results from density matrix calculations. The latter technique requires the use of nearly transform-limited pulses, whereas the former method is successfully implemented with broadband lasers. Damping coefficients γ are introduced to model the consequences of phase fluctuations of the radiation. It is shown that the various techniques can be classified in terms of the delay D of the Stokes laser relative to the pump laser and the damping rate γ. The delay D/ΔτL ≈ −1 and γ = 0 corresponds to the STIRAP mode of operation, whereas the SEP method requires that D/ΔτL ≥ 0 and γΔτL ≫ 1, where ΔτL is the width of the laser pulse.