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Physical Review A

Role of electromagnetically induced transparency in resonant four-wave-mixing schemes

Jon C. Petch, Christoph H. Keitel, P. L. Knight, J. P. Marangos

Published Jan 1, 1996• 102 citations
Publisher

Abstract

The effect of electromagnetically induced transparency in resonant four-wave-mixing schemes is investigated in an analysis that goes beyond perturbation theory in the coherent driving field. In addition we examine the case where the two-photon pump field is sufficiently strong to necessitate a nonperturbative treatment. This allows us to examine the cases where either one or both of the driving fields are strong. Phase matching is included in a plane-wave propagation treatment that matches the situation most likely to be encountered in actual experiments. The calculations are in part intended to model real experimental situations and thus incorporate driving and pump-field linewidths via the phase-diffusion model and Doppler broadening. With a strong pump-field laser, large enhancements in the efficiency of light generation occur at frequencies corresponding to the Autler-Townes satellites induced by the strong driving field. In this situation gain and high four-wave-mixing efficiency are simultaneously present, resulting in the production of a large intensity of coherent radiation. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.543

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Effects of four-wave mixing on four-photon resonance excitation and ionization in the presence of a three-photon intermediate state resonance enhancement

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We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.

Physical Review A•Dec 1, 1991•19 citations
The effect of electromagnetically induced transparency in resonant four-wave-mixing schemes is investigated in an analysis that goes beyond perturbation theory in the coherent driving field. In addition we examine the case where the two-photon pump field is sufficiently strong to necessitate a nonperturbative treatment. This allows us to examine the cases where either one or both of the driving fields are strong. Phase matching is included in a plane-wave propagation treatment that matches the situation most likely to be encountered in actual experiments. The calculations are in part intended to model real experimental situations and thus incorporate driving and pump-field linewidths via the phase-diffusion model and Doppler broadening. With a strong pump-field laser, large enhancements in the efficiency of light generation occur at frequencies corresponding to the Autler-Townes satellites induced by the strong driving field. In this situation gain and high four-wave-mixing efficiency are simultaneously present, resulting in the production of a large intensity of coherent radiation. \textcopyright{} 1996 The American Physical Society.
We investigate a four-state system interacting with long and short laser pulses in a weak probe beam approximation. We show that when all lasers are tuned to the exact unperturbed resonances, part of the four-wave mixing (FWM) field is strongly absorbed. The part that is not absorbed has the exact intensity required to destructively interfere with the excitation pathway involved in producing the FWM state. We show that with this three-photon destructive interference, the conversion efficiency can still be as high as 25%. Contrary to common belief, our calculation shows that this process, where an ideal one-photon electromagnetically induced transparency is established, is not most suitable for high-efficiency conversion. With appropriate phase matching and propagation distance, and when the three-photon destructive interference does not occur, we show that the photon flux conversion efficiency is independent of probe intensity and can be close to 100%. In addition, we show clearly that the conversion efficiency is not determined by the maximum atomic coherence between two lower excited states, as commonly believed. It is the combination of phase matching and constructive interference involving the two terms arising in producing the mixing wave that is the key element for the optimized FWM generation. Indeed, in this scheme no appreciable excited state is produced, so that the atomic coherence between states |0〉 and |2〉 is always very small.
We report experiments that investigate the generation of coherent VUV radiation at 123.6 nm via a resonant sum-difference frequency mixing scheme in Kr. One of the mixing fields at 212.55 nm was in two-photon resonance with the transition between the 4p61S{4p}^{6}{}^{1}S4p61S ground state and the 4p55p[0,12]{4p}^{5}5p[0,\frac{1}{2}]4p55p[0,21​] excited state $(94093.7 {\mathrm{cm}}^{\ensuremath{-}1}).$ The second field (the coupling field) at 759 nm was in single-photon resonance with the transition between the 4p55p[0,12]{4p}^{5}5p[0,\frac{1}{2}]4p55p[0,21​] state and the 4p55s[1,12]{4p}^{5}5s[1,\frac{1}{2}]4p55s[1,21​] state at $80917.6 {\mathrm{cm}}^{\ensuremath{-}1}.$ The presence of the coupling field leads to electromagnetically induced transparency (EIT) at the wavelength of the generated field, 123.6 nm. This is predicted to enhance the four-wave-mixing efficiency by a large factor. We have studied the dependence of the four-wave mixing process on the detuning and strength of the coupling field. The efficiency for four-wave mixing was found to be enhanced by a significant factor (>5) by the EIT effect when the resonant coupling field strength exceeded about half the Doppler width $(0.1 {\mathrm{cm}}^{\ensuremath{-}1}).$ A calculation for monochromatic fields and a uniform slab of gas provided qualitative agreement with the results of experiment. The relative conversion efficiency for this resonant mixing scheme is found to be 104{10}^{4}104 times greater than that for a similar scheme where the coupling laser is tuned far $(1270 {\mathrm{cm}}^{\ensuremath{-}1})$ off resonance. A substantial part of this resonant enhancement can thus be attributed to the EIT effect.
We analyze a four-wave-mixing (FWM) scheme in a five-level atomic system based on electromagnetically induced transparency (EIT). We show that EIT suppresses both two-photon and three-photon absorptions in the FWM scheme and enables the four-wave mixing to proceed through real, resonant intermediate states without absorption loss. The scheme results in a several orders of magnitude increase in the FWM efficiency in comparison with a recent scheme [Phys. Rev. Lett. 88, 143902 (2002)] and may be used for generating short-wavelength radiation at low pump intensities.
We extend the study on a four-wave mixing (FWM) scheme of contiuous-wave lasers in a hot rubidium vapor when the probe and coupling fields work in the electromagnetically induced transparency (EIT) regime while the pump and signal fields work in the two-photon Raman regime. Our experimental results show that the generated signal field is well contained in an EIT dip of the incident probe field as a result of efficient FWM. We find, in particular, that an optimal FWM process can only be attained when the coupling and pump fields are well matched in intensity. If the probe intensity is far beyond the EIT condition, however, the nonlinear efficiency of energy transfer from the probe field to the signal field will be greatly reduced.
A very large number of physical phenomena in the resonant interaction of atomic-molecular systems with the radiation fields can be studied by treating the atomic system as a two level system and by examining its response to the applied fields. Various perturbative results are well known. A number of recent experimental works require the knowledge of the nonperturbative response functions, when both the applied fields are strong. These include a variety of experiments on instabilities(1) in lasers involving the switching from a single mode to for example two mode operation. Similarly recent nonlinear mixing experiments, where not only four wave mixing but also higher mixing in saturating fields has been studied. Pump probe experiments have also been repeated with probes whose intensity could be large. The purpose of this paper is to formulate the general theory and use it to understand the experiments. The formulation we present is also well suited for studying the effect of collisions. Details of various collisional induced coherences in fourwave and six wave mixing etc. can be studied.
We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.