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

arXiv:1110.2221 · Physical Review A

Ultrahigh-resolution spectroscopy with atomic or molecular dark resonances: Exact steady-state line shapes and asymptotic profiles in the adiabatic pulsed regime

T. Zanon-Willette, Emeric de Clercq, E. Arimondo

Published Dec 2, 2011• 42 citations
arXivHTMLPDF

Abstract

Exact and asymptotic line shape expressions are derived from the semiclassical density matrix representation describing a set of closed three-level $\ensuremath{\Lambda}$ atomic or molecular states including decoherences, relaxation rates, and light shifts. An accurate analysis of the exact steady-state dark-resonance profile describing the Autler-Townes doublet, the electromagnetically induced transparency or coherent population trapping resonance, and the Fano-Feshbach line shape leads to the linewidth expression of the two-photon Raman transition and frequency shifts associated to the clock transition. From an adiabatic analysis of the dynamical optical Bloch equations in the weak field limit, a pumping time required to efficiently trap a large number of atoms into a coherent superposition of long-lived states is established. For a highly asymmetrical configuration with different decay channels, a strong two-photon resonance based on a lower states population inversion is established when the driving continuous-wave laser fields are greatly unbalanced. When time separated resonant two-photon pulses are applied in the adiabatic pulsed regime for atomic or molecular clock engineering, where the first pulse is long enough to reach a coherent steady-state preparation and the second pulse is very short to avoid repumping into a new dark state, dark-resonance fringes mixing continuous-wave line shape properties and coherent Ramsey oscillations are created. Those fringes allow interrogation schemes bypassing the power broadening effect. Frequency shifts affecting the central clock fringe computed from asymptotic profiles and related to the Raman decoherence process exhibit nonlinear shapes with the three-level observable used for quantum measurement. We point out that different observables experience different shifts on the lower-state clock transition.

DOI
10.1103/physreva.84.062502

Related papers

Coherent two-photon processes: Transient and steady-state cases

Richard G. Brewer, Erwin Louis Hahn

A class of molecular two-photon processes, occurring under transient or steady-state conditions, is analyzed exactly for certain cases using a density-matrix formalism. Our results are relevant to the recently observed phenomena of transient coherent Raman beats and steady-state two-photon absorption of oppositely directed laser beams. Lowest-order perturbation theories have shown that these processes are insensitive to the Doppler effect, and consequently the linewidth is unaffected by Doppler broadening and by elastic collisions that change molecular velocity. The solutions presented here are of the same form for the Raman and two-photon problems and reveal significant power-dependent frequency shifts and line broadening that correct the ideal Doppler-free solutions. For the transient case, we assume a molecular three-level quantum structure that can be switched in or out of optical resonance with cw laser radiation by means of a pulsed dc Stark field, but the solutions also apply when resonant optical pulses are introduced. During the resonant condition when the Stark pulse is on, the three levels are prepared in coherent superposition, and during the nonresonant condition following the Stark pulse, the laser field(s) stimulates the coherently prepared sample in a transient two-photon process. One of these processes, the Ramanbeat effect, has been observed in forward scattering, but the second one, transient two-photon emission, should be observable in backward scattering. Bloch-like equations are derived for this three-level problem that facilitate an exact pulse solution for state preparation. Following the pulse, transient decay is well-approximated by a perturbation calculation. For the steady-state case, an exact solution is also obtained and is of interest for continuous-wave spectroscopy or for transient experiments requiring an initial preparation of quantum states, prior to Stark switching. These solutions exhibit a power-dependent line broadening and a frequency shift of magnitude $\ensuremath{\sim}\frac{\ensuremath{\Delta}({\ensuremath{\alpha}}^{2}\ensuremath{-}{\ensuremath{\beta}}^{2})}{({\ensuremath{\Delta}}^{2}+\frac{1}{{T}_{2}^{2}})}$, in agreement with our earlier estimate, where $\ensuremath{\alpha}$ and $\ensuremath{\beta}$ are the Rabi flopping frequencies for the two intermediate transitions and $\ensuremath{\Delta}$ is the off-resonance tuning behavior for one of them.

Physical Review A•May 1, 1975•341 citations

Light-shift comparison of electromagnetically induced transparency and coherent population trapping in continuous-wave and Ramsey spectroscopies

Xiaoyan Liu, Xu Zhao, Zhen Xu +1 more

In the atomic frequency standard, the light shift inevitably affects the long-term stability of the atomic clock. In this work, we accurately calculated the light shifts of electromagnetically induced transparency (EIT) and coherent population trapping (CPT) clocks operating under continuum and pulse sequence regimes by numerically solving the Liouville density matrix equation, including all the relaxation terms of a three-level system. The results show that the light shifts under pulse excitation are smaller than those under continuous excitation and the light shifts of the CPT process are much smaller than those of the EIT process under both excitations. It is also found that the light shifts in the continuous excitation increase and those in the pulse excitation decrease with an increase in the Rabi frequency. The light shifts will increase with an increase of the relaxations of the ground states for both the processes under both regimes. Compared to all process atomic clocks, the light shift of pulse-excited atomic clocks is the smallest, which will be suitable for many applications.

Journal of the Optical Society of America B•Mar 2, 2021•2 citations

Two-step pulse observation for Raman–Ramsey coherent population trapping atomic clocks

Yuichiro Yano, Shigeyoshi Goka, Masatoshi Kajita

We propose a two-step pulse observation method to enhance the frequency stability of coherent population trapping (CPT) atomic clocks. The proposed method is a Raman–Ramsey scheme with low light intensity at resonance observation and provides a Ramsey-CPT resonance with both reduced frequency sensitivity to the light intensity and a high signal-to-noise ratio by reducing the repumping into a steady dark state. The resonance characteristics were calculated using density matrix analysis of a Λ-type three-level system that was modeled on the 133 Cs D 1 line, and the characteristics were also measured using a vertical-cavity surface-emitting laser and a Cs vapor cell.

arXiv:1411.3779•Applied Physics Express•Dec 11, 2014•8 citations

Composite laser-pulses spectroscopy for high-accuracy optical clocks: a review of recent progress and perspectives

T. Zanon-Willette, R. Lefèvre, Rémi Metzdorff +7 more

Probing an atomic resonance without disturbing it is an ubiquitous issue in physics. This problem is critical in high-accuracy spectroscopy or for the next generation of atomic optical clocks. Ultra-high resolution frequency metrology requires sophisticated interrogation schemes and robust protocols handling pulse length errors and residual frequency detuning offsets. This review reports recent progress and perspective in such schemes, using sequences of composite laser-pulses tailored in pulse duration, frequency and phase, inspired by NMR techniques and quantum information processing. After a short presentation of Rabi technique and NMR-like composite pulses allowing efficient compensation of electromagnetic field perturbations to achieve robust population transfers, composite laser-pulses are investigated within Ramsey's method of separated oscillating fields in order to generate non-linear compensation of probe-induced frequency shifts. Laser-pulses protocols such as hyper-Ramsey, modified hyper-Ramsey, generalized hyper-Ramsey and hybrid schemes as auto-balanced Ramsey spectroscopy are reviewed. These techniques provide excellent protection against both probe induced light-shift perturbations and laser intensity variations. More sophisticated schemes generating synthetic frequency-shifts are presented. They allow to reduce or completely eliminate imperfect correction of probe-induced frequency-shifts even in presence of decoherence due to the laser line-width. Finally, two universal protocols are presented which provide complete elimination of probe-induced frequency shifts in the general case where both decoherence and relaxation dissipation effects are present by using exact analytic expressions for phase-shifts and the clock frequency detuning. These techniques might be applied to atomic, molecular and nuclear frequency metrology, Ramsey-type mass spectrometry as well as precision spectroscopy.

arXiv:1806.04639•Reports on Progress in Physics•Jun 4, 2018•54 citations

Quantum engineering of atomic phase shifts in optical clocks

T. Zanon-Willette, Sylvain Almonacil, Emeric de Clercq +2 more

Quantum engineering of time-separated Raman laser pulses in three-level systems is presented to produce an ultranarrow optical transition in bosonic alkali-earth clocks free from light shifts and with a significantly reduced sensitivity to laser parameter fluctuations. Based on a quantum artificial complex wave-function analytical model and supported by a full density-matrix simulation including a possible residual effect of spontaneous emission from the intermediate state, atomic phase shifts associated with Ramsey and hyper-Ramsey two-photon spectroscopy in optical clocks are derived. Various common-mode Raman frequency detunings are found in which the frequency shifts from off-resonant states are canceled, while their uncertainties at the ${10}^{\ensuremath{-}18}$ level of accuracy are strongly reduced.

arXiv:1407.1381•Physical Review A•Nov 24, 2014•18 citations

Light shifts in a pulsed cold-atom coherent-population-trapping clock

E. Blanshan, Simon Rochester, Elizabeth A. Donley +1 more

Field-grade atomic clocks capable of primary standard performance in compact physics packages would be of significant value in applications ranging from network synchronization to inertial navigation. A coherent-population-trapping clock featuring laser-cooled $^{87}\mathrm{Rb}$ atoms and pulsed Ramsey interrogation is a strong candidate for this technology if the frequency biases can be minimized and controlled. Here we characterize the light shift in a cold-atom coherent-population-trapping clock, explaining observed shifts in terms of phase shifts that arise during the formation of dark-state coherences combined with optical-pumping effects caused by unwanted incoherent light in the interrogation spectrum. Measurements are compared with existing and new theoretical treatments, and a laser configuration is identified that would reduce clock frequency uncertainty from light shifts to a fractional frequency level of $\ensuremath{\Delta}\ensuremath{\nu}/\ensuremath{\nu}=4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ per 100 kHz of laser frequency uncertainty.

Physical Review A•Apr 10, 2015•42 citations
Exact and asymptotic line shape expressions are derived from the semiclassical density matrix representation describing a set of closed three-level \ensuremathΛ\ensuremath{\Lambda}\ensuremathΛ atomic or molecular states including decoherences, relaxation rates, and light shifts. An accurate analysis of the exact steady-state dark-resonance profile describing the Autler-Townes doublet, the electromagnetically induced transparency or coherent population trapping resonance, and the Fano-Feshbach line shape leads to the linewidth expression of the two-photon Raman transition and frequency shifts associated to the clock transition. From an adiabatic analysis of the dynamical optical Bloch equations in the weak field limit, a pumping time required to efficiently trap a large number of atoms into a coherent superposition of long-lived states is established. For a highly asymmetrical configuration with different decay channels, a strong two-photon resonance based on a lower states population inversion is established when the driving continuous-wave laser fields are greatly unbalanced. When time separated resonant two-photon pulses are applied in the adiabatic pulsed regime for atomic or molecular clock engineering, where the first pulse is long enough to reach a coherent steady-state preparation and the second pulse is very short to avoid repumping into a new dark state, dark-resonance fringes mixing continuous-wave line shape properties and coherent Ramsey oscillations are created. Those fringes allow interrogation schemes bypassing the power broadening effect. Frequency shifts affecting the central clock fringe computed from asymptotic profiles and related to the Raman decoherence process exhibit nonlinear shapes with the three-level observable used for quantum measurement. We point out that different observables experience different shifts on the lower-state clock transition.
A class of molecular two-photon processes, occurring under transient or steady-state conditions, is analyzed exactly for certain cases using a density-matrix formalism. Our results are relevant to the recently observed phenomena of transient coherent Raman beats and steady-state two-photon absorption of oppositely directed laser beams. Lowest-order perturbation theories have shown that these processes are insensitive to the Doppler effect, and consequently the linewidth is unaffected by Doppler broadening and by elastic collisions that change molecular velocity. The solutions presented here are of the same form for the Raman and two-photon problems and reveal significant power-dependent frequency shifts and line broadening that correct the ideal Doppler-free solutions. For the transient case, we assume a molecular three-level quantum structure that can be switched in or out of optical resonance with cw laser radiation by means of a pulsed dc Stark field, but the solutions also apply when resonant optical pulses are introduced. During the resonant condition when the Stark pulse is on, the three levels are prepared in coherent superposition, and during the nonresonant condition following the Stark pulse, the laser field(s) stimulates the coherently prepared sample in a transient two-photon process. One of these processes, the Ramanbeat effect, has been observed in forward scattering, but the second one, transient two-photon emission, should be observable in backward scattering. Bloch-like equations are derived for this three-level problem that facilitate an exact pulse solution for state preparation. Following the pulse, transient decay is well-approximated by a perturbation calculation. For the steady-state case, an exact solution is also obtained and is of interest for continuous-wave spectroscopy or for transient experiments requiring an initial preparation of quantum states, prior to Stark switching. These solutions exhibit a power-dependent line broadening and a frequency shift of magnitude $\ensuremath{\sim}\frac{\ensuremath{\Delta}({\ensuremath{\alpha}}^{2}\ensuremath{-}{\ensuremath{\beta}}^{2})}{({\ensuremath{\Delta}}^{2}+\frac{1}{{T}_{2}^{2}})}$, in agreement with our earlier estimate, where $\ensuremath{\alpha}$ and $\ensuremath{\beta}$ are the Rabi flopping frequencies for the two intermediate transitions and $\ensuremath{\Delta}$ is the off-resonance tuning behavior for one of them.
In the atomic frequency standard, the light shift inevitably affects the long-term stability of the atomic clock. In this work, we accurately calculated the light shifts of electromagnetically induced transparency (EIT) and coherent population trapping (CPT) clocks operating under continuum and pulse sequence regimes by numerically solving the Liouville density matrix equation, including all the relaxation terms of a three-level system. The results show that the light shifts under pulse excitation are smaller than those under continuous excitation and the light shifts of the CPT process are much smaller than those of the EIT process under both excitations. It is also found that the light shifts in the continuous excitation increase and those in the pulse excitation decrease with an increase in the Rabi frequency. The light shifts will increase with an increase of the relaxations of the ground states for both the processes under both regimes. Compared to all process atomic clocks, the light shift of pulse-excited atomic clocks is the smallest, which will be suitable for many applications.
We propose a two-step pulse observation method to enhance the frequency stability of coherent population trapping (CPT) atomic clocks. The proposed method is a Raman–Ramsey scheme with low light intensity at resonance observation and provides a Ramsey-CPT resonance with both reduced frequency sensitivity to the light intensity and a high signal-to-noise ratio by reducing the repumping into a steady dark state. The resonance characteristics were calculated using density matrix analysis of a Λ-type three-level system that was modeled on the 133 Cs D 1 line, and the characteristics were also measured using a vertical-cavity surface-emitting laser and a Cs vapor cell.
Probing an atomic resonance without disturbing it is an ubiquitous issue in physics. This problem is critical in high-accuracy spectroscopy or for the next generation of atomic optical clocks. Ultra-high resolution frequency metrology requires sophisticated interrogation schemes and robust protocols handling pulse length errors and residual frequency detuning offsets. This review reports recent progress and perspective in such schemes, using sequences of composite laser-pulses tailored in pulse duration, frequency and phase, inspired by NMR techniques and quantum information processing. After a short presentation of Rabi technique and NMR-like composite pulses allowing efficient compensation of electromagnetic field perturbations to achieve robust population transfers, composite laser-pulses are investigated within Ramsey's method of separated oscillating fields in order to generate non-linear compensation of probe-induced frequency shifts. Laser-pulses protocols such as hyper-Ramsey, modified hyper-Ramsey, generalized hyper-Ramsey and hybrid schemes as auto-balanced Ramsey spectroscopy are reviewed. These techniques provide excellent protection against both probe induced light-shift perturbations and laser intensity variations. More sophisticated schemes generating synthetic frequency-shifts are presented. They allow to reduce or completely eliminate imperfect correction of probe-induced frequency-shifts even in presence of decoherence due to the laser line-width. Finally, two universal protocols are presented which provide complete elimination of probe-induced frequency shifts in the general case where both decoherence and relaxation dissipation effects are present by using exact analytic expressions for phase-shifts and the clock frequency detuning. These techniques might be applied to atomic, molecular and nuclear frequency metrology, Ramsey-type mass spectrometry as well as precision spectroscopy.
Quantum engineering of time-separated Raman laser pulses in three-level systems is presented to produce an ultranarrow optical transition in bosonic alkali-earth clocks free from light shifts and with a significantly reduced sensitivity to laser parameter fluctuations. Based on a quantum artificial complex wave-function analytical model and supported by a full density-matrix simulation including a possible residual effect of spontaneous emission from the intermediate state, atomic phase shifts associated with Ramsey and hyper-Ramsey two-photon spectroscopy in optical clocks are derived. Various common-mode Raman frequency detunings are found in which the frequency shifts from off-resonant states are canceled, while their uncertainties at the ${10}^{\ensuremath{-}18}$ level of accuracy are strongly reduced.
Field-grade atomic clocks capable of primary standard performance in compact physics packages would be of significant value in applications ranging from network synchronization to inertial navigation. A coherent-population-trapping clock featuring laser-cooled 87Rb^{87}\mathrm{Rb}87Rb atoms and pulsed Ramsey interrogation is a strong candidate for this technology if the frequency biases can be minimized and controlled. Here we characterize the light shift in a cold-atom coherent-population-trapping clock, explaining observed shifts in terms of phase shifts that arise during the formation of dark-state coherences combined with optical-pumping effects caused by unwanted incoherent light in the interrogation spectrum. Measurements are compared with existing and new theoretical treatments, and a laser configuration is identified that would reduce clock frequency uncertainty from light shifts to a fractional frequency level of $\ensuremath{\Delta}\ensuremath{\nu}/\ensuremath{\nu}=4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ per 100 kHz of laser frequency uncertainty.