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Physical Review A

Pump-probe spectroscopy in degenerate two-level atoms with arbitrarily strong fields

T. Zigdon, A. D. Wilson‐Gordon, Harry Friedmann

Published Mar 19, 2008• 18 citations
Publisher

Abstract

We study the pump and probe absorption spectra, as a function of the probe detuning, in a degenerate two-level atomic system, for the case where the probe intensity is high enough to affect the pump absorption. The theory is valid for any ${F}_{g}\ensuremath{\rightarrow}{F}_{e}$ alkali-metal transition interacting with an arbitrarily intense pump and probe (with general Rabi frequencies ${\ensuremath{\Omega}}_{1,2}$) which are perpendicularly polarized with either ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ or $\ensuremath{\pi}$ polarization. We have constructed a computer program that can calculate the spectra without requiring one to write out the Bloch equations explicitly. We show that, when the pump is ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ polarized and the probe $\ensuremath{\pi}$ polarized, or vice versa, the pump and probe absorptions depend on the Zeeman coherences between the nearest-neighboring ground or excited Zeeman sublevels, whereas when the pump is ${\ensuremath{\sigma}}_{+}$ polarized and the probe ${\ensuremath{\sigma}}_{\ensuremath{-}}$ polarized, or vice versa, the Zeeman coherences that directly determine the absorption are between next-nearest neighbors. We report calculations of the pump and probe absorption spectra for the cycling ${F}_{g}=2\ensuremath{\rightarrow}{F}_{e}=3$ transition in the ${D}_{2}$ line of $^{87}\text{R}\text{b}$, interacting with a resonant ${\ensuremath{\sigma}}_{+}$-polarized pump and either a $\ensuremath{\pi}$- or a ${\ensuremath{\sigma}}_{\ensuremath{-}}$- polarized probe. The probe and pump absorption spectra are analyzed by considering the contributions that derive from the individual ${m}_{g}\ensuremath{\rightarrow}{m}_{e}$ transitions. We then show how these contributions depend on the ground- and excited-state populations and Zeeman coherences, and investigate the role played by transfer of coherence from the excited to the ground hyperfine state. We show that the pump and probe absorption spectra are mirror images of each other when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}>\ensuremath{\Gamma}$, and have the same behavior at line center and complementary behavior in the wings, when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}<\ensuremath{\Gamma}$ ($\ensuremath{\Gamma}$ is the rate of spontaneous decay from ${F}_{e}$ to ${F}_{g}$).

DOI
10.1103/physreva.77.033836

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We review our previous work on pump-probe spectroscopy in realistic degenerate two-level systems and model systems. In particular, we discuss the role of transfer of coherence (TOC) between the ground and excited hyperfine states in producing electromagnetically-induced transparency (EIA) peaks in the probe spectrum, when an Fg goes to Fe = Fg +1 transition in an alkali-metal atom interacts with a strong pump and weak probe that have perpendicular polarizations. When the pump is rho+ polarized and the probe pi polarized, this system can be modelled by an N system. We also discuss the role of transfer of population (TOP) between the Zeeman levels of the ground hyperfine state in producing EIA peaks when the pump and probe have the same polarization. This system can be modelled using a double two-level system. The role of Doppler broadening and phase-changing collisions in modifying the EIA-TOC and EIA-TOP absorption and refraction spectra is also discussed. All these spectra were calculated using MATLAB programs that both construct and solve the relevant Bloch equations. In our recent work, we consider the effect of a strong probe on the pump absorption and refraction spectra when the pump and probe polarizations are linear and perpendicular. It is difficult to solve this problem numerically due to the large number frequencies involved. In order to simplify the problem, we considered two cases: (i) rho+ polarized pump and pi polarized probe, and (ii) rho+ polarized pump and rho- polarized probe, and investigated a series of transitions in both Rb and Cs, using modified versions of the MATLAB programs devised for the weakprobe case. A number of interesting differences from the weak-probe case were found. For example, when the probe is sufficiently strong, we found the pump and probe spectra to show complementary behavior. In addition, as the number of Zeeman levels increase, the EIA peaks become progressively sharper, and are accompanied by steeper dispersion.

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The absorption spectrum of a weak probe, interacting with a driven degenerate two-level atomic system, whose ground and excited hyperfine states are ${\mathrm{F}}_{g,e},$ can exhibit narrow peaks at line center. When the pump and probe polarizations are different, ${F}_{e}{=F}_{g}+1$ and ${F}_{g}>0,$ the electromagnetically induced absorption (EIA) peak has been shown to be due to the transfer of coherence (TOC) between the excited and ground states via spontaneous decay. We give a detailed explanation of why the TOC that leads to EIA (EIA-TOC) can only take place when ground-state population trapping does not occur, that is, when ${F}_{e}{=F}_{g}+1.$ We also explain why EIA-TOC is observed in open systems. We show that EIA can also occur when the pump and probe polarizations are identical and ${F}_{e}{=F}_{g}+1.$ This EIA is analogous to an effect that occurs in simple two-level systems when the collisional transfer of population (TOP) from the ground state to a reservoir is greater than that from the excited state. For a degenerate two-level system, the reservoir consists of the Zeeman sublevels of the ground hyperfine state, and of other nearby hyperfine states that do not interact with the pump. We will also discuss the four-wave mixing spectrum under the conditions where EIA-TOC and EIA-TOP occur.

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We study the pump and probe absorption spectra, as a function of the probe detuning, in a degenerate two-level atomic system, for the case where the probe intensity is high enough to affect the pump absorption. The theory is valid for any Fg\ensuremath→Fe{F}_{g}\ensuremath{\rightarrow}{F}_{e}Fg​\ensuremath→Fe​ alkali-metal transition interacting with an arbitrarily intense pump and probe (with general Rabi frequencies \ensuremathΩ1,2{\ensuremath{\Omega}}_{1,2}\ensuremathΩ1,2​) which are perpendicularly polarized with either \ensuremathσ\ifmmode±\else\textpm\fi{\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}\ensuremathσ\ifmmode±\else\textpm\fi​ or \ensuremathπ\ensuremath{\pi}\ensuremathπ polarization. We have constructed a computer program that can calculate the spectra without requiring one to write out the Bloch equations explicitly. We show that, when the pump is \ensuremathσ\ifmmode±\else\textpm\fi{\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}\ensuremathσ\ifmmode±\else\textpm\fi​ polarized and the probe \ensuremathπ\ensuremath{\pi}\ensuremathπ polarized, or vice versa, the pump and probe absorptions depend on the Zeeman coherences between the nearest-neighboring ground or excited Zeeman sublevels, whereas when the pump is \ensuremathσ+{\ensuremath{\sigma}}_{+}\ensuremathσ+​ polarized and the probe \ensuremathσ\ensuremath−{\ensuremath{\sigma}}_{\ensuremath{-}}\ensuremathσ\ensuremath−​ polarized, or vice versa, the Zeeman coherences that directly determine the absorption are between next-nearest neighbors. We report calculations of the pump and probe absorption spectra for the cycling Fg=2\ensuremath→Fe=3{F}_{g}=2\ensuremath{\rightarrow}{F}_{e}=3Fg​=2\ensuremath→Fe​=3 transition in the D2{D}_{2}D2​ line of 87Rb^{87}\text{R}\text{b}87Rb, interacting with a resonant \ensuremathσ+{\ensuremath{\sigma}}_{+}\ensuremathσ+​-polarized pump and either a \ensuremathπ\ensuremath{\pi}\ensuremathπ- or a \ensuremathσ\ensuremath−{\ensuremath{\sigma}}_{\ensuremath{-}}\ensuremathσ\ensuremath−​- polarized probe. The probe and pump absorption spectra are analyzed by considering the contributions that derive from the individual mg\ensuremath→me{m}_{g}\ensuremath{\rightarrow}{m}_{e}mg​\ensuremath→me​ transitions. We then show how these contributions depend on the ground- and excited-state populations and Zeeman coherences, and investigate the role played by transfer of coherence from the excited to the ground hyperfine state. We show that the pump and probe absorption spectra are mirror images of each other when \ensuremathΩ1\ensuremath≥\ensuremathΩ2>\ensuremathΓ{\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}>\ensuremath{\Gamma}\ensuremathΩ1​\ensuremath≥\ensuremathΩ2​>\ensuremathΓ, and have the same behavior at line center and complementary behavior in the wings, when \ensuremathΩ1\ensuremath≥\ensuremathΩ2<\ensuremathΓ{\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}<\ensuremath{\Gamma}\ensuremathΩ1​\ensuremath≥\ensuremathΩ2​<\ensuremathΓ (\ensuremathΓ\ensuremath{\Gamma}\ensuremathΓ is the rate of spontaneous decay from Fe{F}_{e}Fe​ to Fg{F}_{g}Fg​).
We review our previous work on pump-probe spectroscopy in realistic degenerate two-level systems and model systems. In particular, we discuss the role of transfer of coherence (TOC) between the ground and excited hyperfine states in producing electromagnetically-induced transparency (EIA) peaks in the probe spectrum, when an Fg goes to Fe = Fg +1 transition in an alkali-metal atom interacts with a strong pump and weak probe that have perpendicular polarizations. When the pump is rho+ polarized and the probe pi polarized, this system can be modelled by an N system. We also discuss the role of transfer of population (TOP) between the Zeeman levels of the ground hyperfine state in producing EIA peaks when the pump and probe have the same polarization. This system can be modelled using a double two-level system. The role of Doppler broadening and phase-changing collisions in modifying the EIA-TOC and EIA-TOP absorption and refraction spectra is also discussed. All these spectra were calculated using MATLAB programs that both construct and solve the relevant Bloch equations. In our recent work, we consider the effect of a strong probe on the pump absorption and refraction spectra when the pump and probe polarizations are linear and perpendicular. It is difficult to solve this problem numerically due to the large number frequencies involved. In order to simplify the problem, we considered two cases: (i) rho+ polarized pump and pi polarized probe, and (ii) rho+ polarized pump and rho- polarized probe, and investigated a series of transitions in both Rb and Cs, using modified versions of the MATLAB programs devised for the weakprobe case. A number of interesting differences from the weak-probe case were found. For example, when the probe is sufficiently strong, we found the pump and probe spectra to show complementary behavior. In addition, as the number of Zeeman levels increase, the EIA peaks become progressively sharper, and are accompanied by steeper dispersion.
Spectroscopic features revealing the coherent interaction of a degenerate two-level atomic system with two optical fields are examined. A model for the numerical calculation of the response of a degenerate two-level system to the action of an arbitrarily intense resonant pump field and a weak probe in the presence of a magnetic field is presented. The model is valid for arbitrary values of the total angular momentum of the lower and upper levels and for any choice of the polarizations of the optical waves. Closed and open degenerate two-level systems are considered. Predictions for probe absorption and dispersion, field generation by four-wave mixing, population modulation, and Zeeman optical pumping are derived. On all these observables, subnatural-width coherence resonances are predicted and their spectroscopic features are discussed. Experimental spectra for probe absorption and excited-state population modulation in the D2{D}_{2}D2​ line of Rb vapor are presented in good agreement with the calculations.
We calculate the pump and probe absorption spectra for the cycling ${F}_{g}=4\ensuremath{\rightarrow}{F}_{e}=5$ transition D2{D}_{2}D2​ line of 133Cs^{133}\text{C}\text{s}133Cs in an atomic beam, interacting with a strong resonant ${\ensuremath{\sigma}}_{+}$-polarized pump and a probe of comparable intensity and either ${\ensuremath{\sigma}}_{\ensuremath{-}}$ or $\ensuremath{\pi}$ polarization. The aim is to reproduce and analyze the experiments of Dahl et al. [Opt. Lett. 33, 983 (2008)] who showed for a ${\ensuremath{\sigma}}_{+}$-polarized pump and ${\ensuremath{\sigma}}_{\ensuremath{-}}$-polarized probe that the pump absorption spectrum switches from an ``absorption within transparency'' (AWT) structure, when the probe is weaker than the pump, to a ``transparency within transparency'' (TWT) structure, when the probe is stronger than the pump. For all other polarization combinations, the pump spectrum displays AWT behavior at all probe intensities. We analyze our results by considering the contributions that derive from the individual ${m}_{g}\ensuremath{\rightarrow}{m}_{e}$ transitions. When the ${\ensuremath{\sigma}}_{+}$-polarized pump is stronger than the ${\ensuremath{\sigma}}_{\ensuremath{-}}$-polarized probe, the population is swept toward the ${m}_{g}\ensuremath{\rightarrow}{m}_{e}={m}_{g}+1$ transitions with the highest values of mg{m}_{g}mg​, and the pump absorption spectrum has an AWT structure and resembles that of an NNN system. However, when the probe is stronger than the pump, the population is swept toward the ${m}_{g}=\ensuremath{-}{F}_{g}\ensuremath{\rightarrow}{m}_{e}={m}_{g}\ensuremath{-}1$ transition when the probe is near resonance, and to the ${m}_{g}={F}_{g}\ensuremath{\rightarrow}{m}_{e}={m}_{g}+1$ transition when the probe is detuned from resonance. The pump and probe spectra are mirror images of each other and resemble those of a VVV system where the probe has a peak at line center and the pump spectrum has a TWT structure. For a strong ${\ensuremath{\sigma}}_{+}$ pump and an even stronger $\ensuremath{\pi}$ probe, the population concentrates in the intermediate transitions, and the AWT to TWT changeover does not occur. We also show that the narrow features in the spectra at line center derive from transfer of coherence from the excited to the ground hyperfine levels.
Spectroscopic features revealing the coherent interaction of a degenerate two-level atomic system with two optical fields are examined. A model for the numerical calculation of the response of a degenerate two-level system to the action of an arbitrarily intense resonant pump field and a weak probe in the presence of a magnetic field is presented. The model is valid for arbitrary values of the total angular momentum of the lower and upper levels and for any choice of the polarizations of the optical waves. Closed and open degenerate two-level systems are considered. Predictions for probe absorption and dispersion, field generation by four-wave-mixing, population modulation and Zeeman optical pumping are derived. On all these observables, sub-natural-width coherence resonances are predicted and their spectroscopic features are discussed. Experimental spectra for probe absorption and excited state population modulation in the D2 line of Rb vapor are presented in good agreement with the calculations
A numerical method is introduced that solves the optical Bloch equations describing a two-level atom interacting with a strong polychromatic pump field with an equidistant spectrum and an arbitrarily intense monochromatic probe field. The method involves a transformation of the optical Bloch equations into a system of equations with time-independent coefficients at steady state via double harmonic expansion of the density-matrix elements, which is then solved by the method of matrix inversion. The solutions so obtained lead immediately to the determination of the polarization of the atomic medium and of the absorption and dispersion spectra. The method is applied to the case when the pump field is bichromatic and trichromatic, and the physical interpretation of the numerically computed spectra is given.
The absorption spectrum of a weak probe, interacting with a driven degenerate two-level atomic system, whose ground and excited hyperfine states are Fg,e,{\mathrm{F}}_{g,e},Fg,e​, can exhibit narrow peaks at line center. When the pump and probe polarizations are different, Fe=Fg+1{F}_{e}{=F}_{g}+1Fe​=Fg​+1 and Fg>0,{F}_{g}>0,Fg​>0, the electromagnetically induced absorption (EIA) peak has been shown to be due to the transfer of coherence (TOC) between the excited and ground states via spontaneous decay. We give a detailed explanation of why the TOC that leads to EIA (EIA-TOC) can only take place when ground-state population trapping does not occur, that is, when Fe=Fg+1.{F}_{e}{=F}_{g}+1.Fe​=Fg​+1. We also explain why EIA-TOC is observed in open systems. We show that EIA can also occur when the pump and probe polarizations are identical and Fe=Fg+1.{F}_{e}{=F}_{g}+1.Fe​=Fg​+1. This EIA is analogous to an effect that occurs in simple two-level systems when the collisional transfer of population (TOP) from the ground state to a reservoir is greater than that from the excited state. For a degenerate two-level system, the reservoir consists of the Zeeman sublevels of the ground hyperfine state, and of other nearby hyperfine states that do not interact with the pump. We will also discuss the four-wave mixing spectrum under the conditions where EIA-TOC and EIA-TOP occur.