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

The Journal of Chemical Physics

Kinetics and spectroscopy of near-resonant optical pumping in intense fields

Frederick H. Mies, Y. Ben Aryeh

Published Jan 1, 1981• 8 citations
Publisher

Abstract

The resonant Raman scattering in a three level system produces an optical pumping of molecules from the initial to the final states which are radiatively coupled to the intermediate resonant state. We consider the pumping that is produced by an intense, pulsed, monochromatic radiation field that is near-resonant with the initial resonance frequency. The Heitler–Ma damping theory is solved exactly for the case when the resonance fluorescence is weak compared to the Raman scattering, or any other processes which might cause irreversible decay of the resonant state. In particular, we examine the usefulness of dressed states to describe the intense field limit. The spectral line shape for the Raman scattering is obtained. The transient behavior following the onset of the laser pulse is examined and a careful analysis of the pumping rate and its relationship to both weak and strong field theories is presented.

DOI
10.1063/1.440806

Related papers

Resonance fluorescence and resonance Raman lineshapes in strong radiation fields

Yitzhak Rabin, A. Ben‐Reuven

Lineshapes of three-level resonance Raman scattering and two-level resonance fluorescence, homogeneously broadened by collisions, in the presence of arbitrarily strong coherent radiation, are studied by means of a tetradic (density-matrix) scattering theory. In the case of medium coupling strength V L to the radiation field (where T 2 -1 <or=V L << tau c -1 , with T 2 and tau c being the coherence damping and collision times, respectively) the Mollow lineshape (1977) for resonance fluorescence is rederived, with proper T 2 and population cross-relaxation effects included. In particular it is shown that relaxation through intermediate non-resonant levels can considerably alter the lineshape in resonance fluorescence. In the case of strong coupling (V L >or approximately= tau c -1 ) the collision rates are modified by the applied field (optical collisions). It is shown that, whereas in self attenuation spectra optical collision rates can be obtained only from line intensity or line wing measurements, in resonance scattering these rates are directly obtained from linewidth measurements.

Journal of Physics B Atomic and Molecular Physics•May 28, 1980•25 citations

Stimulated collision-induced resonance Raman scattering

V.M. Arutunyan, N. Sh. Badanyan, N. V. Shakhnazaryan

The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.

Journal of Physics B Atomic and Molecular Physics•Oct 14, 1985•0 citations

Time and spectral resolution in resonance scattering and resonance fluorescence

E. Courtens, A. Szöke

The theory of resonance Raman effect, resonantly enhanced two-photon absorption, and resonance fluorescence---valid also for strong fields---is treated in a unified and simplified way. Dressed states, Bloch equations, and perturbation theory are used to calculate line positions, and integrated intensities both for steady state and transient excitation. The case of adiabatic following is solved explicitly; it occurs when an off-resonance incident pulse is turned on and off slowly. It leads to the identification of Raman scattering, two-photon absorption, and Rayleigh scattering with an adiabatic process while fluorescence and consecutive two-photon absorption with nonadiabaticity. Time-dependent spectra are defined in a rigorous way. Our formulas agree in the various limits with those that appear in the literature.

Physical Review A•Apr 1, 1977•196 citations

Resonance fluorescence and Raman scattering pumped by an adiabatic pulse

Б. В. Крыжановский, A. O. Melikyan

The approximation of nonoverlapping lines is used to calculate spectra of resonance fluorescence and Raman scattering when two- and three-level atoms are pumped by a smooth pulse of duration comparable with the excited-state lifetime. The difference between the quasienergy terms, that determines the satellite frequency, depends on time and has the same value twice, at the pulse leading and trailing edges, so that interference may occur between the radiation produced in the appropriate parts of the pulse. However, the interference pattern is blurred since radiative broadening destroys the coherence. Relationships are obtained between the parameters for which interference may be observed. An analysis is made of the change to short pulses when allowance can be made for the scattered field using the first order of perturbation theory.

Soviet Journal of Quantum Electronics•Jan 31, 1984•1 citation

Raman processes

Bruce W. Shore

The traditional Raman process alluded to in Chap. 13 is a three-state sequence of transitions in which radiative excitation (induced by a pump field) is followed by spontaneous emission that produces a final state differing from the initial state [Her50b] [Sho90, § 17.5]. When the final state of the sequence is more energetic than the initial state the resulting emission line (to the red of the pump wavelength) is known as a Stokes spectral line. The difference between the pump frequency and the Stokes frequency, the Raman frequency , defines the excitation energy of the final state relative to the initial state. When, instead, the final state has lower energy than the initial state, as can occur when the initial quantum state is already excited, then the emission is an anti-Stokes line, at a bluer wavelength than the pump field. The overall Raman scattering is a two-photon process. Typically Raman spectroscopy deals with molecules; the two-photon transitions are then between vibrational-rotational states, through electronically excited intermediate states, that are characterized in part by vibrational quantum number v and rotational angular momentum quantum numbers J, M . From any given excited electronic state there are many fluorescing transitions, corresponding to various vibrational and rotational quantum numbers of the final state. The wavelengths of the various Stokes and anti-Stokes lines (i.e. the Raman frequencies) characterize the particular molecular species, and so they have provided a valuable diagnostic tool for spectroscopists.

Cambridge University Press eBooks•Sep 29, 2011•0 citations

Cooperative behavior among three-level systems: Transient effects of coherent optical pumping

C. M. Bowden, Chi C. Sung

The dynamical evolution of an excited-state population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the excited states by an externally applied ($c$-number) coherent pump. The intermediate and ground states are taken as nonradiatively coupled whereas the excited-to-intermediate-state transition is coupled to the radiation field which is treated quantum mechanically. It is found that stimulated Raman processes can significantly influence the dynamical evolution of population inversion and macroscopic polarization by producing coherence effects among the populations. We examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration. It is shown, using the mean-field approximation, that for uniform pumping and conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective radiation time ${\ensuremath{\tau}}_{R}$, and the pump pulse duration ${\ensuremath{\tau}}_{P}$ satisfy the inequalities, ${\ensuremath{\omega}}_{R}>\frac{1}{{\ensuremath{\tau}}_{R}}>\ensuremath{\gamma}$ and ${\ensuremath{\tau}}_{P}\ensuremath{\gtrsim}{\ensuremath{\tau}}_{R}$ ($\ensuremath{\gamma}$ is a characteristic internal dephasing rate for the molecules), the system is left in a state with classical transverse polarization when the pump pulse terminates. The system can evolve collectively from such a state only as superradiant (classical) evolution. For superfluorescent evolution which requires a state of preparation of complete inversion (zero transverse polarization), it is shown that the pump pulse must be effectively of area $\ensuremath{\pi}$ and that ${\ensuremath{\tau}}_{P}<{\ensuremath{\tau}}_{R}$. Our results show that when the former conditions are satisfied the delay time ${\ensuremath{\tau}}_{D}$ for collective free pulse evolution is a function of both ${\ensuremath{\tau}}_{P}$ and ${\ensuremath{\tau}}_{R}$. It is shown further that the pump pulse shape as well as temporal duration significantly affect the final state of preparation. The results of this work are interpreted in connection with recent reported results of experiments in superfluorescence and superradiance.

Physical Review A•Oct 1, 1978•58 citations
The resonant Raman scattering in a three level system produces an optical pumping of molecules from the initial to the final states which are radiatively coupled to the intermediate resonant state. We consider the pumping that is produced by an intense, pulsed, monochromatic radiation field that is near-resonant with the initial resonance frequency. The Heitler–Ma damping theory is solved exactly for the case when the resonance fluorescence is weak compared to the Raman scattering, or any other processes which might cause irreversible decay of the resonant state. In particular, we examine the usefulness of dressed states to describe the intense field limit. The spectral line shape for the Raman scattering is obtained. The transient behavior following the onset of the laser pulse is examined and a careful analysis of the pumping rate and its relationship to both weak and strong field theories is presented.
Lineshapes of three-level resonance Raman scattering and two-level resonance fluorescence, homogeneously broadened by collisions, in the presence of arbitrarily strong coherent radiation, are studied by means of a tetradic (density-matrix) scattering theory. In the case of medium coupling strength V L to the radiation field (where T 2 -1 <or=V L << tau c -1 , with T 2 and tau c being the coherence damping and collision times, respectively) the Mollow lineshape (1977) for resonance fluorescence is rederived, with proper T 2 and population cross-relaxation effects included. In particular it is shown that relaxation through intermediate non-resonant levels can considerably alter the lineshape in resonance fluorescence. In the case of strong coupling (V L >or approximately= tau c -1 ) the collision rates are modified by the applied field (optical collisions). It is shown that, whereas in self attenuation spectra optical collision rates can be obtained only from line intensity or line wing measurements, in resonance scattering these rates are directly obtained from linewidth measurements.
The passage of strong monochromatic laser radiation through a resonance medium consisting of three-level atoms is investigated. It is shown that if collisions are taken into account in the scattered waves the resonances at combination frequencies occur to first order in the laser field intensity. A numerical analysis of the dependence of the stimulated electronic Raman scattering (SERS) components' gain factors on the pump frequency is carried out. The dispersion curves of the SERS components' gain (absorption) factors for fixed values of pump frequency and intensity are plotted.
The theory of resonance Raman effect, resonantly enhanced two-photon absorption, and resonance fluorescence---valid also for strong fields---is treated in a unified and simplified way. Dressed states, Bloch equations, and perturbation theory are used to calculate line positions, and integrated intensities both for steady state and transient excitation. The case of adiabatic following is solved explicitly; it occurs when an off-resonance incident pulse is turned on and off slowly. It leads to the identification of Raman scattering, two-photon absorption, and Rayleigh scattering with an adiabatic process while fluorescence and consecutive two-photon absorption with nonadiabaticity. Time-dependent spectra are defined in a rigorous way. Our formulas agree in the various limits with those that appear in the literature.
The approximation of nonoverlapping lines is used to calculate spectra of resonance fluorescence and Raman scattering when two- and three-level atoms are pumped by a smooth pulse of duration comparable with the excited-state lifetime. The difference between the quasienergy terms, that determines the satellite frequency, depends on time and has the same value twice, at the pulse leading and trailing edges, so that interference may occur between the radiation produced in the appropriate parts of the pulse. However, the interference pattern is blurred since radiative broadening destroys the coherence. Relationships are obtained between the parameters for which interference may be observed. An analysis is made of the change to short pulses when allowance can be made for the scattered field using the first order of perturbation theory.
The traditional Raman process alluded to in Chap. 13 is a three-state sequence of transitions in which radiative excitation (induced by a pump field) is followed by spontaneous emission that produces a final state differing from the initial state [Her50b] [Sho90, § 17.5]. When the final state of the sequence is more energetic than the initial state the resulting emission line (to the red of the pump wavelength) is known as a Stokes spectral line. The difference between the pump frequency and the Stokes frequency, the Raman frequency , defines the excitation energy of the final state relative to the initial state. When, instead, the final state has lower energy than the initial state, as can occur when the initial quantum state is already excited, then the emission is an anti-Stokes line, at a bluer wavelength than the pump field. The overall Raman scattering is a two-photon process. Typically Raman spectroscopy deals with molecules; the two-photon transitions are then between vibrational-rotational states, through electronically excited intermediate states, that are characterized in part by vibrational quantum number v and rotational angular momentum quantum numbers J, M . From any given excited electronic state there are many fluorescing transitions, corresponding to various vibrational and rotational quantum numbers of the final state. The wavelengths of the various Stokes and anti-Stokes lines (i.e. the Raman frequencies) characterize the particular molecular species, and so they have provided a valuable diagnostic tool for spectroscopists.
The dynamical evolution of an excited-state population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the excited states by an externally applied (ccc-number) coherent pump. The intermediate and ground states are taken as nonradiatively coupled whereas the excited-to-intermediate-state transition is coupled to the radiation field which is treated quantum mechanically. It is found that stimulated Raman processes can significantly influence the dynamical evolution of population inversion and macroscopic polarization by producing coherence effects among the populations. We examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration. It is shown, using the mean-field approximation, that for uniform pumping and conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective radiation time ${\ensuremath{\tau}}_{R}$, and the pump pulse duration ${\ensuremath{\tau}}_{P}$ satisfy the inequalities, ${\ensuremath{\omega}}_{R}>\frac{1}{{\ensuremath{\tau}}_{R}}>\ensuremath{\gamma}$ and ${\ensuremath{\tau}}_{P}\ensuremath{\gtrsim}{\ensuremath{\tau}}_{R}$ ($\ensuremath{\gamma}$ is a characteristic internal dephasing rate for the molecules), the system is left in a state with classical transverse polarization when the pump pulse terminates. The system can evolve collectively from such a state only as superradiant (classical) evolution. For superfluorescent evolution which requires a state of preparation of complete inversion (zero transverse polarization), it is shown that the pump pulse must be effectively of area $\ensuremath{\pi}$ and that ${\ensuremath{\tau}}_{P}<{\ensuremath{\tau}}_{R}$. Our results show that when the former conditions are satisfied the delay time ${\ensuremath{\tau}}_{D}$ for collective free pulse evolution is a function of both ${\ensuremath{\tau}}_{P}$ and ${\ensuremath{\tau}}_{R}$. It is shown further that the pump pulse shape as well as temporal duration significantly affect the final state of preparation. The results of this work are interpreted in connection with recent reported results of experiments in superfluorescence and superradiance.