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

Physical Review A

Line shape and strength of two-photon absorption in an atomic vapor with a resonant or nearly resonant intermediate state

John E. Bjorkholm, P. F. Liao

Published Aug 1, 1976• 149 citations
Publisher

Abstract

The line shape and strength of two-photon absorption in an atomic vapor are studied both theoretically and experimentally for the case of absorption of unequal-frequency photons. Special attention is given to the situation in which the intermediate state is resonant or nearly resonant. It is shown that for the resonant case, maximum absorption rates and Doppler-free spectra are simultaneously obtained. Either counterpropagating or copropagating beams can be used. With counterpropagating beams the two-photon linewidths are quite insensitive to power broadening of the intermediate state. With copropagating beams the two-photon spectra can also reveal the intermediate-state structure with a resolution determined mainly by the intermediate-state lifetime (nearly as well as can be done using any spectroscopic technique). The theoretical analysis provides a closed-form solution for the line shape and strength of the two-photon spectrum. In general the line shape is composed of two features. One is Doppler broadened and predominates when the intermediate state is nonresonant. The second feature is Doppler free, and it predominates with a resonant intermediate state. Detailed comparisons of experimental measurements of the line shape and strength of two-photon absorption in Na vapor are made with the theory and found to be in excellent agreement. Signal strengths for the onresonance case are 6 \ifmmode\times\else\texttimes\fi{} ${10}^{9}$ larger than the case of equal-frequency photons with no loss in resolution.

DOI
10.1103/physreva.14.751

Related papers

Line Shape of the Sub-Doppler Resonance in Alkali-Metal Atomic Vapors in the Field of Counterpropagating Bichromatic Laser Beams

А. М. Михайлов, Rodolphe Boudot, Denis V. Brazhnikov

Abstract High-contrast sub-Doppler resonances observed in alkali-metal atomic vapors in the field of counterpropagating bichromatic laser beams are perspective in quantum metrology for designing a miniature optical frequency standard. Until now, these nonlinear resonances have been investigated only experimentally or using numerical calculations. In our opinion, the development of a simplified theoretical model of the observed resonances, which would provide explicit compact analytic expressions describing the line shape of the resonance, would be extremely important for further evolution of the theory. In this study, we perform such theoretical analysis based on the three-level Λ scheme of the atom. We investigate two regimes, viz., the regime of a low-intensity standing wave with close intensities of counterpropagating beams (I1 ≈ I2) and the regime of a probe wave, in which one of the beams has a noticeably lower intensity than that of the oppositely propagating beam (I2 ≪ I1). The resulting analytic expressions make it possible to determine qualitative differences between these regimes and to separate explicitly the contributions from different nonlinear effects to the light field absorption, including the terms responsible for the formation of a high-contrast sub-Doppler peak. The expressions derived here are in qualitative agreement with experimental data obtained earlier.

Journal of Experimental and Theoretical Physics•Dec 1, 2021•7 citations

Theory of one-photon high-resolution absorption optical spectroscopy

J. I. Cotrim Vasconcellos

We consider in this paper the Doppler-broadened absorption by two-level molecules of a gas from a weak traveling electromagnetic plane wave in the presence of an oppositely traveling strong plane wave at the same frequency. Here the absorption spectrum exhibits a dip that broadens and deepens as the gas is increasingly saturated by the strong wave. This saturation effect has been employed in the recent experiments on the fine structure of atomic hydrogen performed by H\"ansch, Shahin, and Schawlow (HSS). The form, linewidth, and strength of saturation dips in the fine-structure lines are studied for experimental parameters appropriate to the hydrogen experiment. In addition, saturation line-shape curves are calculated for experimental situations in which the strengths of the stronger field give rise to stronger or weaker saturation of the gas medium and varying degrees of Doppler broadening exist. The calculation of shape of the saturation dip and absorption curves for a Doppler-broadened gas of two-level atoms is made exactly; in effect, the strong field is treated as arbitrarily strong by avoiding a perturbation-theory treatment in favor of the exact solutions for a driven two-level system. The general behavior found is in accord with intuition and experimental observations by HSS. There is an optimum saturation power which gives a prominent dip and beyond which the dip suffers "power broadening."

Physical Review A•Jan 1, 1977•10 citations

Three-photon frequency shift on non-collinear excitation

Richard M. Friedberg, Sven R. Hartmann, Jamal T. Manassah

The authors calculate the three-photon resonance absorption shift obtained with two non-collinear excitation beams of arbitrary orientation incident on an ensemble of collisionally broadened two-level atoms excited close to one-third of the resonance frequency. For counterpropagating beams the absorption resonance is narrow and shifted by the order of the linewidth to the violet. As the beams are angled away from the counterpropagating condition the shift increases, and if the angle approaches copropagation the shift becomes very large. When the shift exceeds the single-photon absorption linewidth by more than L/ lambda , the shifted line weakens and disappears, but a separate unshifted peak persists at copropagation. The third-harmonic generation response is more complicated. Except in the region where the beams are almost copropagating the shift in third-harmonic generation response follows the shift in the absorption response. In contrast to the absorption response the third-harmonic generation response increases as the excitation beams approach copropagation, then peaks, then diminishes, broadens and forms a complicated structure whose character is determined by phase matching.

Journal of Physics B Atomic Molecular and Optical Physics•Jul 14, 1989•26 citations

Fundamental linewidth limit of electromagnetically induced transparency in a thermal Rydberg ladder

Anonymous, Nikunjkumar Prajapati, Alexandra B. Artusio‐Glimpse +2 more

Spectroscopy of Rydberg states has become a popular platform for quantum sensing, with the most common readout scheme being two-photon electromagnetically induced transparency (EIT) using counterpropagating laser beams. In this scheme, the energy resolution of the Rydberg state is set by the spectral linewidth of the EIT feature. While selection criteria for the two-photon resonance can narrow the linewidth to the order of the Rydberg state decay rate for a single atom, the Doppler shift from thermal velocity of the atoms broadens the ensemble linewidth to the order of the decay rate of the intermediate state. Here, we derive an analytic expression for the Doppler residual line shape in the low-power limit and corroborate the results with experiment. For Rb, we find the full-width-at-half-maximum linewidth limit to be 1.84 MHz when scanning the coupling laser and measure an experimental linewidth of 2.04 MHz. These linewidths are around a factor of 2 narrower than previous theoretical estimates as well as previously reported measured linewidths. With this, we demonstrate the most precise two-photon energy resolution of a Rydberg state in thermal vapor to date. We then map out broadening mechanisms near this limit.

arXiv:2603.04596•Physical Review Research•Aug 26, 2026•0 citations

Doppler-free multiphotonic spectroscopy

G. Grynberg, Bernard Cagnac

The review describes atomic transitions where two or more photons are simultaneously absorbed by an atom or a molecule (without any intermediate resonant level). The authors show theoretically and experimentally the possibilities of these transitions for numerous high-resolution spectroscopic studies. The Doppler broadening is suppressed in two-photon transitions if the atoms are irradiated by two laser waves travelling in opposite directions, because the Doppler shift in one wave cancels that in the other. A generalization is made for multiphotonic transitions. A typical experimental set-up with a CW dye laser is described in detail, but the possibilities of other light sources are also discussed.

Reports on Progress in Physics•Jul 1, 1977•201 citations

Line shape, frequency shift, Rabi splitting, and two-photon resonances in four-level double-resonance spectroscopy with closely spaced intermediate levels

Swapan Kumar Mandal, Pradip Narayan Ghosh

The interaction of a four-level atomic system with two electromagnetic radiations has been studied. The two intermediate levels are closely spaced such that a single radiation frequency can induce transitions from the ground state to both of them. In a cascade-type double resonance, the pump electric-field amplitude is much stronger than the amplitude of the signal field, which can induce transitions from both of the intermediate levels to the upper state. The 15 optical Bloch equations obtained from the Liouville equations are solved analytically to obtain the Doppler-free signal line shape. The computed signals, exhibiting two Lorentzian line profiles, are presented for different pump frequencies. In addition to these one-photon transitions, we obtain a weak two-photon resonance peak. The two-photon resonance becomes weaker when the detuning of the pump frequency from a resonance frequency is increased. When the pump frequency ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$ is intermediate between the pump resonance frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, the two-photon resonance is very weak and almost vanishes when ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$=(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$)/2. When the pump frequency is on resonance with one of the transition frequencies, the Rabi splitting of the signal shows asymmetry because of the presence of a close-lying transition which is pumped off resonance. The intensity-dependent shifts of the transitions are such that they repel each other more and more as the intensity of the pump field is increased. These shifts arise from the nonresonant interaction between the atom and the field.

Physical Review A•Jun 1, 1993•18 citations
The line shape and strength of two-photon absorption in an atomic vapor are studied both theoretically and experimentally for the case of absorption of unequal-frequency photons. Special attention is given to the situation in which the intermediate state is resonant or nearly resonant. It is shown that for the resonant case, maximum absorption rates and Doppler-free spectra are simultaneously obtained. Either counterpropagating or copropagating beams can be used. With counterpropagating beams the two-photon linewidths are quite insensitive to power broadening of the intermediate state. With copropagating beams the two-photon spectra can also reveal the intermediate-state structure with a resolution determined mainly by the intermediate-state lifetime (nearly as well as can be done using any spectroscopic technique). The theoretical analysis provides a closed-form solution for the line shape and strength of the two-photon spectrum. In general the line shape is composed of two features. One is Doppler broadened and predominates when the intermediate state is nonresonant. The second feature is Doppler free, and it predominates with a resonant intermediate state. Detailed comparisons of experimental measurements of the line shape and strength of two-photon absorption in Na vapor are made with the theory and found to be in excellent agreement. Signal strengths for the onresonance case are 6 \ifmmode\times\else\texttimes\fi{} 109{10}^{9}109 larger than the case of equal-frequency photons with no loss in resolution.
Abstract High-contrast sub-Doppler resonances observed in alkali-metal atomic vapors in the field of counterpropagating bichromatic laser beams are perspective in quantum metrology for designing a miniature optical frequency standard. Until now, these nonlinear resonances have been investigated only experimentally or using numerical calculations. In our opinion, the development of a simplified theoretical model of the observed resonances, which would provide explicit compact analytic expressions describing the line shape of the resonance, would be extremely important for further evolution of the theory. In this study, we perform such theoretical analysis based on the three-level Λ scheme of the atom. We investigate two regimes, viz., the regime of a low-intensity standing wave with close intensities of counterpropagating beams (I1 ≈ I2) and the regime of a probe wave, in which one of the beams has a noticeably lower intensity than that of the oppositely propagating beam (I2 ≪ I1). The resulting analytic expressions make it possible to determine qualitative differences between these regimes and to separate explicitly the contributions from different nonlinear effects to the light field absorption, including the terms responsible for the formation of a high-contrast sub-Doppler peak. The expressions derived here are in qualitative agreement with experimental data obtained earlier.
We consider in this paper the Doppler-broadened absorption by two-level molecules of a gas from a weak traveling electromagnetic plane wave in the presence of an oppositely traveling strong plane wave at the same frequency. Here the absorption spectrum exhibits a dip that broadens and deepens as the gas is increasingly saturated by the strong wave. This saturation effect has been employed in the recent experiments on the fine structure of atomic hydrogen performed by H\"ansch, Shahin, and Schawlow (HSS). The form, linewidth, and strength of saturation dips in the fine-structure lines are studied for experimental parameters appropriate to the hydrogen experiment. In addition, saturation line-shape curves are calculated for experimental situations in which the strengths of the stronger field give rise to stronger or weaker saturation of the gas medium and varying degrees of Doppler broadening exist. The calculation of shape of the saturation dip and absorption curves for a Doppler-broadened gas of two-level atoms is made exactly; in effect, the strong field is treated as arbitrarily strong by avoiding a perturbation-theory treatment in favor of the exact solutions for a driven two-level system. The general behavior found is in accord with intuition and experimental observations by HSS. There is an optimum saturation power which gives a prominent dip and beyond which the dip suffers "power broadening."
The authors calculate the three-photon resonance absorption shift obtained with two non-collinear excitation beams of arbitrary orientation incident on an ensemble of collisionally broadened two-level atoms excited close to one-third of the resonance frequency. For counterpropagating beams the absorption resonance is narrow and shifted by the order of the linewidth to the violet. As the beams are angled away from the counterpropagating condition the shift increases, and if the angle approaches copropagation the shift becomes very large. When the shift exceeds the single-photon absorption linewidth by more than L/ lambda , the shifted line weakens and disappears, but a separate unshifted peak persists at copropagation. The third-harmonic generation response is more complicated. Except in the region where the beams are almost copropagating the shift in third-harmonic generation response follows the shift in the absorption response. In contrast to the absorption response the third-harmonic generation response increases as the excitation beams approach copropagation, then peaks, then diminishes, broadens and forms a complicated structure whose character is determined by phase matching.
Spectroscopy of Rydberg states has become a popular platform for quantum sensing, with the most common readout scheme being two-photon electromagnetically induced transparency (EIT) using counterpropagating laser beams. In this scheme, the energy resolution of the Rydberg state is set by the spectral linewidth of the EIT feature. While selection criteria for the two-photon resonance can narrow the linewidth to the order of the Rydberg state decay rate for a single atom, the Doppler shift from thermal velocity of the atoms broadens the ensemble linewidth to the order of the decay rate of the intermediate state. Here, we derive an analytic expression for the Doppler residual line shape in the low-power limit and corroborate the results with experiment. For Rb, we find the full-width-at-half-maximum linewidth limit to be 1.84 MHz when scanning the coupling laser and measure an experimental linewidth of 2.04 MHz. These linewidths are around a factor of 2 narrower than previous theoretical estimates as well as previously reported measured linewidths. With this, we demonstrate the most precise two-photon energy resolution of a Rydberg state in thermal vapor to date. We then map out broadening mechanisms near this limit.
The review describes atomic transitions where two or more photons are simultaneously absorbed by an atom or a molecule (without any intermediate resonant level). The authors show theoretically and experimentally the possibilities of these transitions for numerous high-resolution spectroscopic studies. The Doppler broadening is suppressed in two-photon transitions if the atoms are irradiated by two laser waves travelling in opposite directions, because the Doppler shift in one wave cancels that in the other. A generalization is made for multiphotonic transitions. A typical experimental set-up with a CW dye laser is described in detail, but the possibilities of other light sources are also discussed.
The interaction of a four-level atomic system with two electromagnetic radiations has been studied. The two intermediate levels are closely spaced such that a single radiation frequency can induce transitions from the ground state to both of them. In a cascade-type double resonance, the pump electric-field amplitude is much stronger than the amplitude of the signal field, which can induce transitions from both of the intermediate levels to the upper state. The 15 optical Bloch equations obtained from the Liouville equations are solved analytically to obtain the Doppler-free signal line shape. The computed signals, exhibiting two Lorentzian line profiles, are presented for different pump frequencies. In addition to these one-photon transitions, we obtain a weak two-photon resonance peak. The two-photon resonance becomes weaker when the detuning of the pump frequency from a resonance frequency is increased. When the pump frequency ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$ is intermediate between the pump resonance frequencies ${\mathrm{\ensuremath{\omega}}}_{1}$ and ${\mathrm{\ensuremath{\omega}}}_{2}$, the two-photon resonance is very weak and almost vanishes when ${\mathrm{\ensuremath{\Omega}}}_{\mathit{p}}$=(${\mathrm{\ensuremath{\omega}}}_{1}$+${\mathrm{\ensuremath{\omega}}}_{2}$)/2. When the pump frequency is on resonance with one of the transition frequencies, the Rabi splitting of the signal shows asymmetry because of the presence of a close-lying transition which is pumped off resonance. The intensity-dependent shifts of the transitions are such that they repel each other more and more as the intensity of the pump field is increased. These shifts arise from the nonresonant interaction between the atom and the field.