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Theoretical studies of Resonance Enhance Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor

N. M. Lawandy

Published Jan 1, 1986• 0 citations
OpenAlex

Abstract

It is well known that the presence of a real atomic level which is nearly resonant with the pump field can greatly enhance the Raman emission cross section. In order to accurately calculate the Raman gain in systems where resonance enhancement plays a dominant role, expressions for the pump and signal susceptibilities must be derived. These expressions should be valid for arbitrary field strengths in order to allow for pump and signal saturation. In addition, the theory should allow for arbitrary longitudinal and transverse relaxation rates. This latter point is extremely vital for three level atomic systems such as the alkali earth metals since they do not have population reservoirs and can have widely varying spontaneous lifetimes on the three pertinent transitions. Moreover, the dephasing rates are strong functions of electron states and are therefore also different for the three coupled pairs of levels. These considerations are not as important when molecular systems are concerned since the large reservoir of rotational states serve to produce essentially equal longitudinal recovery rates for the population of the three levels. The three level system with three arbitrary longitudinal and transverse relaxation rates was solved. There is no need for setting either pair of rates equal and the expressions are valid for arbitrarily strong fields.

Related papers

Theoretical studies of Resonance Enhanced Stimulated Raman Scattering (RESRS) of frequency doubled Alexandrite laser wavelengths in cesium vapor

N. M. Lawandy

This work focused on understanding the effects of arbitrary transverse and longitudinal relaxation rates on the susceptibilities of coherently driven three-level systems. The approximation of a single relaxation rate often made in previous work is strongly invalidated by the variation in the spontaneous emission lifetime between various atomic level pairs in systems such as cesium. It is of great importance to the problem of nonlinear infrared generation to determine the dependence of both real and imaginary susceptibility on relaxation rates. The imaginary susceptibility on the pump transition determines the absorption of pump photons and the imaginary susceptibility on the laser transition determines the spectral dependence of the gain. This is of particular importance for pure Raman emission (i.e., absorption at linecenter of the gain transition) as it determines the tunability characteristics we are aiming to predict. The real susceptibility is important when cavities are used at the signal field as this will determine the loaded resonance of the Raman oscillator. Researchers show that in some cases which result from having different relaxation rates mode splitting may result, allowing more than one frequency to have the same Raman wavelength, possibly resulting in a temporal instability.

•Jan 14, 1986•0 citations

Nonlinear infrared generation in alkali metal vapors: Steady state susceptibilities and dynamic behavior. Effective relaxation rates and preliminary Raman gain predictions for the Cs system

N. M. Lawandy

Effective relaxation rates for atomic cesium pumped by doubled Alexandrite radiation are presented. Laser radiation levels are 8S 1/2 and 9S 1/2; resonance levels 3 = 8P 1/2 and 8P 1/2, respectively. In addition, Raman gain is represented in two graphs which plot chi per atom (10 to the -13 power) at Raman peak versus the infrared wave number per centimeter and the corresponding doubled Alexandrite wave number. One graph covers resonance level 8P, the other 9P; in both cases cesium is pumped with a peak pulse height of 0.5 MW in a 200 micron diameter spot size.

•Dec 18, 1986•0 citations

Effect of the pump absorption on generation of infrared stimulated electronic Raman scattering in alkali-metal vapors

A. I. Agafonov, G. G. Grigoryan, Nikolay V Znamenskiy +5 more

The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.

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Strong amplification of sidebands in a strongly driven three-level atomic system

Constantine Mavroyannis

We have considered the excitation spectra for a three-level atom interacting simultaneously with a strong pump field and a weak signal field. The atom consists of an upper excited state ‖2〉 and two lower states ‖1〉 and ‖3〉 where the transition ‖1〉↔‖3〉 is electric-dipole forbidden from parity considerations. The pump field, whose frequency mode ωb is initially populated, operates near resonance between the states ‖2〉 and ‖3〉, ‖2〉↔‖3〉, while the signal field describes the radiative decays ‖2〉→‖3〉 and ‖2〉→‖1〉, respectively. Using the Green function method, the spectral functions for the signal field have been calculated in the limit of high photon densities of the pump field describing the following processes: (i) one-photon process; the spectra consist of a main peak at the signal frequency ω=ω21 and a pair of sidebands at ω=ω21±Ω−(ω23−ωb)/2, where Ω2=Ω2b/2+(ω23−ωb)2/4 with Ωb and (ω23−ωb) being the Rabi frequency and the detuning of the pump field, respectively. The intensity of the main peak at ω=ω21 is positive indicating signal-field absorption while those of the sidebands are always negative implying amplification (stimulated emission) of the signal field. The sum of the intensities (in absolute value) of the sidebands is twice that of the main peak at resonance while in the off-resonance case it depends on the value of the ratio (ω23−ωb)/2Ω. (ii) Stimulated three-photon process; the spectra consists of a pair of sidebands peaked at ω=ω21−2ωb±Ω−(ω23−ωb)/2 whose intensity is negative indicating amplification. At resonance the sidebands have equal intensities but at finite detuning asymmetry arises enhancing one peak while diminishing the intensity of the other. (iii) Stimulated two-photon process; the stimulated Raman spectra consist of a peak at ω=ω31, which has a delta function distribution, and a pair of strongly amplified sidebands at ω=ω31±Ω+(ω23−ωb)/2. The computed spectra for the three processes are presented graphically for different values of Rabi frequencies and detunings.

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Stimulated Raman gain in a Λ-type atomic system with doubly excited transitions

Jason L. Bowie, J. C. Garrison, R. Y. Chiao

Measurements of stimulated Raman gain in rubidium vapor are made and compared with a detailed model. Amplification of a weak probe laser is observed in a \ensuremath{\Lambda}-type three-level system that is driven by a strong cw coupling laser. The intensity of the coupling laser is sufficiently strong that it both optically pumps the atomic levels, causing a population inversion in the ground-state hyperfine levels, and drives the stimulated Raman process producing gain. A theory that models all aspects of the gain mechanism is presented. The model includes all interactions between the external fields and the atomic transitions, including those processes that involve multiple fields interacting with the same transition. Numerical calculations are compared with gain measurements made at several coupling laser intensities and detunings from the $D1$ line in ${}^{85}\mathrm{Rb}.$

Physical Review A•Apr 14, 2000•9 citations

Stimulated Raman spectra of a strong bichromatic field interacting with a three-level atom

Constantine Mavroyannis

We have studied the stimulated Raman spectra arising from the interaction of a three-level atom with two strong electromagnetic fields whose initially populated modes ω a and ω b are in resonance with the two atomic transition frequencies. The Green's function formalism has been used in the limit of high photon densities to calculate the excitation spectra near the frequencies ω = ± ω ab = ± (ω a - ω b ). Expressions are derived for the relative intensities, which describe, apart from the usual Raman peak at the frequency ω = ω ab , four pairs of lorentzian lines peaked at the frequencies ω - ω ab = ± Ω a /√2, ± Ω b /√2, ± Ω and ± 2Ω, respectively, and having spectra widths of the order of 3γ0/4. The parameter Ω is defined as Ω2 = (Ω a 2 + Ω b 2)/2, where Ω a and Ω b are the Rabi frequencies of the two laser fields and γ0 is the spontaneous emission probability. Numerical calculations for selected values of the Rabi frequencies are graphically presented and discussed. Conditions have been established for which Raman gain processes are anticipated to take place.

Molecular Physics•Mar 1, 1983•6 citations
It is well known that the presence of a real atomic level which is nearly resonant with the pump field can greatly enhance the Raman emission cross section. In order to accurately calculate the Raman gain in systems where resonance enhancement plays a dominant role, expressions for the pump and signal susceptibilities must be derived. These expressions should be valid for arbitrary field strengths in order to allow for pump and signal saturation. In addition, the theory should allow for arbitrary longitudinal and transverse relaxation rates. This latter point is extremely vital for three level atomic systems such as the alkali earth metals since they do not have population reservoirs and can have widely varying spontaneous lifetimes on the three pertinent transitions. Moreover, the dephasing rates are strong functions of electron states and are therefore also different for the three coupled pairs of levels. These considerations are not as important when molecular systems are concerned since the large reservoir of rotational states serve to produce essentially equal longitudinal recovery rates for the population of the three levels. The three level system with three arbitrary longitudinal and transverse relaxation rates was solved. There is no need for setting either pair of rates equal and the expressions are valid for arbitrarily strong fields.
This work focused on understanding the effects of arbitrary transverse and longitudinal relaxation rates on the susceptibilities of coherently driven three-level systems. The approximation of a single relaxation rate often made in previous work is strongly invalidated by the variation in the spontaneous emission lifetime between various atomic level pairs in systems such as cesium. It is of great importance to the problem of nonlinear infrared generation to determine the dependence of both real and imaginary susceptibility on relaxation rates. The imaginary susceptibility on the pump transition determines the absorption of pump photons and the imaginary susceptibility on the laser transition determines the spectral dependence of the gain. This is of particular importance for pure Raman emission (i.e., absorption at linecenter of the gain transition) as it determines the tunability characteristics we are aiming to predict. The real susceptibility is important when cavities are used at the signal field as this will determine the loaded resonance of the Raman oscillator. Researchers show that in some cases which result from having different relaxation rates mode splitting may result, allowing more than one frequency to have the same Raman wavelength, possibly resulting in a temporal instability.
Effective relaxation rates for atomic cesium pumped by doubled Alexandrite radiation are presented. Laser radiation levels are 8S 1/2 and 9S 1/2; resonance levels 3 = 8P 1/2 and 8P 1/2, respectively. In addition, Raman gain is represented in two graphs which plot chi per atom (10 to the -13 power) at Raman peak versus the infrared wave number per centimeter and the corresponding doubled Alexandrite wave number. One graph covers resonance level 8P, the other 9P; in both cases cesium is pumped with a peak pulse height of 0.5 MW in a 200 micron diameter spot size.
The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.
We have considered the excitation spectra for a three-level atom interacting simultaneously with a strong pump field and a weak signal field. The atom consists of an upper excited state ‖2〉 and two lower states ‖1〉 and ‖3〉 where the transition ‖1〉↔‖3〉 is electric-dipole forbidden from parity considerations. The pump field, whose frequency mode ωb is initially populated, operates near resonance between the states ‖2〉 and ‖3〉, ‖2〉↔‖3〉, while the signal field describes the radiative decays ‖2〉→‖3〉 and ‖2〉→‖1〉, respectively. Using the Green function method, the spectral functions for the signal field have been calculated in the limit of high photon densities of the pump field describing the following processes: (i) one-photon process; the spectra consist of a main peak at the signal frequency ω=ω21 and a pair of sidebands at ω=ω21±Ω−(ω23−ωb)/2, where Ω2=Ω2b/2+(ω23−ωb)2/4 with Ωb and (ω23−ωb) being the Rabi frequency and the detuning of the pump field, respectively. The intensity of the main peak at ω=ω21 is positive indicating signal-field absorption while those of the sidebands are always negative implying amplification (stimulated emission) of the signal field. The sum of the intensities (in absolute value) of the sidebands is twice that of the main peak at resonance while in the off-resonance case it depends on the value of the ratio (ω23−ωb)/2Ω. (ii) Stimulated three-photon process; the spectra consists of a pair of sidebands peaked at ω=ω21−2ωb±Ω−(ω23−ωb)/2 whose intensity is negative indicating amplification. At resonance the sidebands have equal intensities but at finite detuning asymmetry arises enhancing one peak while diminishing the intensity of the other. (iii) Stimulated two-photon process; the stimulated Raman spectra consist of a peak at ω=ω31, which has a delta function distribution, and a pair of strongly amplified sidebands at ω=ω31±Ω+(ω23−ωb)/2. The computed spectra for the three processes are presented graphically for different values of Rabi frequencies and detunings.
Measurements of stimulated Raman gain in rubidium vapor are made and compared with a detailed model. Amplification of a weak probe laser is observed in a \ensuremath{\Lambda}-type three-level system that is driven by a strong cw coupling laser. The intensity of the coupling laser is sufficiently strong that it both optically pumps the atomic levels, causing a population inversion in the ground-state hyperfine levels, and drives the stimulated Raman process producing gain. A theory that models all aspects of the gain mechanism is presented. The model includes all interactions between the external fields and the atomic transitions, including those processes that involve multiple fields interacting with the same transition. Numerical calculations are compared with gain measurements made at several coupling laser intensities and detunings from the D1D1D1 line in 85Rb.{}^{85}\mathrm{Rb}.85Rb.
We have studied the stimulated Raman spectra arising from the interaction of a three-level atom with two strong electromagnetic fields whose initially populated modes ω a and ω b are in resonance with the two atomic transition frequencies. The Green's function formalism has been used in the limit of high photon densities to calculate the excitation spectra near the frequencies ω = ± ω ab = ± (ω a - ω b ). Expressions are derived for the relative intensities, which describe, apart from the usual Raman peak at the frequency ω = ω ab , four pairs of lorentzian lines peaked at the frequencies ω - ω ab = ± Ω a /√2, ± Ω b /√2, ± Ω and ± 2Ω, respectively, and having spectra widths of the order of 3γ0/4. The parameter Ω is defined as Ω2 = (Ω a 2 + Ω b 2)/2, where Ω a and Ω b are the Rabi frequencies of the two laser fields and γ0 is the spontaneous emission probability. Numerical calculations for selected values of the Rabi frequencies are graphically presented and discussed. Conditions have been established for which Raman gain processes are anticipated to take place.