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AIP conference proceedings

Effect of pressure dependent quantum interference on the ac stark shifting of a four-photon resonance

M. G. Payne, L. Deng, J. Y. Zhang, W. R. Garrett

Published Jan 1, 1995• 1 citation
Publisher

Abstract

We report an experiment in xenon which confirms the theoretical predictions (Payne et al, Phys. Rev. A48, 2334 (1993)) on the pressure dependent suppression of the ac Stark shifting of even‐photon resonances. In the co‐propagating configuration the ac Stark due to a second laser is totally suppressed at elevated concentrations due to a destructive interference between two excitation pathways. The ac Stark shift persists in the counter‐propagating configuration because of the absence of destructive interference.

DOI
10.1063/1.47637

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Effect of Pressure Dependent Quantum Interference on the ac Stark Shifting of a Four-Photon Resonance

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We report an experiment in xenon which confirms theoretical predictions [Payne et al., Phys. Rev. A 48, 2334 (1993)] on the pressure dependent suppression of the ac Stark shifting of even-photon resonances. In the copropagating configuration the ac Stark shift introduced by a second laser is totally suppressed at elevated concentrations due to a very complete destructive interference between two pumping pathways. The ac Stark shift persists in the counterpropagating configuration.

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Effect of pressure-dependent quantum interference on the ac Stark shifting of two-photon resonances

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We describe ac Stark shift production and measurement in a two-laser mode where a first laser is tuned through a two-photon resonance between the ground state and an excited state in order to record a line shape for the corresponding resonantly enhanced multiphoton ionization. A second laser is tuned to a fixed wavelength which is close to a resonance between the upper state in the two-photon transition and a third state which has dipole-allowed transitions back to the ground state. At low concentrations the second laser leads to very large ac Stark shifts in the two-photon excitation and in the related resonantly enhanced multiphoton ionization. However, at high concentrations a destructive interference occurs involving the three-photon coupling between the third state and the ground state and the one-photon coupling due to the four-wave-mixing field at frequency 2${\mathrm{\ensuremath{\omega}}}_{\mathit{L}1}$\ifmmode\pm\else\textpm\fi{}${\mathrm{\ensuremath{\omega}}}_{\mathit{L}2}$. This interference leads to a pressure-dependent suppression of the amplitude for the third state. When this destructive interference occurs, the ac Stark shift due to the second laser undergoes a corresponding pressure-dependent suppression. The criteria for the pressure to be high enough to completely suppress the ac Stark shift is that the real part of phase mismatch \ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert} at the angular frequency 2${\mathrm{\ensuremath{\omega}}}_{\mathit{L}1}$\ifmmode\pm\else\textpm\fi{}${\mathrm{\ensuremath{\omega}}}_{\mathit{L}2}$ and (or) the absorption coefficient \ensuremath{\beta} at the same frequency should be very large, so that with unfocused focused beams \ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert}L>5[(${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$\ensuremath{\tau}${]}^{1/2}$, where L is the thickness of gas penetrated before the shift is measured, ${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$ is the maximum ac Stark shift at very low pressure, and \ensuremath{\tau} is the pulse length of the lasers.At positions and concentrations such that 1\ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert}L\ensuremath{\le}2[(${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$\ensuremath{\tau})${]}^{1/2}$ the ac Stark shift is present but the two-photon excitation is suppressed due to a destructive interference between excitation by two photons from the first laser and by two-photon excitation between a four-wave-mixing photon and a photon from the second laser.

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We use resonance ionization involving two colors in single-pass and retroreflected geometries to study the suppression of excitation of a four-photon resonance by an interference involving four-wave sum-frequency generation occurring near an intermediate three-photon resonance. The 6p[1/2](J=0) state of xenon is excited by three blue photons plus one infrared photon. One beam, focused to ${\mathit{I}}_{1}$\ensuremath{\simeq}7\ifmmode\times\else\texttimes\fi{}${10}^{9}$ W/${\mathrm{cm}}^{2}$, is nearly three-photon resonant with the 6s[3/2](J=1) resonance; the second, unfocused beam (${\mathit{I}}_{2}$\ensuremath{\simeq}2\ifmmode\times\else\texttimes\fi{}${10}^{7}$ W/${\mathrm{cm}}^{2}$) is tuned to maintain exact four-photon resonance with the 6p[1/2](J=1) state. One additional blue photon ionizes from the four-photon level. Third-harmonic light is generated by the first, nearly three-photon-resonant beam by four-wave sum-frequency mixing. One third-harmonic photon plus one photon from the second laser form a second excitation pathway to the four-photon level; destructive interference between the two pathways results in a reduction in the observed ionization. The degree of reduction depends on the xenon density and the detuning (both positive and negative) from three-photon resonance. This interference may be overcome by retroreflecting the nearly three-photon-resonant beam to provide an additional excitation pathway which generates no third harmonic.The study provides detailed information on the pressure-dependent range from exact resonance over which the familiar three-photon cancellation effect is operative; it shows that the interference occurs in high- and low-energy regions about three-photon resonance; and it establishes that interference is produced for large values of the phase mismatch even if the absorption of the interfering field is low. We compare our measurements of the reduction in ionization with predictions published by us elsewhere [M. G. Payne, J. C. Miller, R. C. Hart, and W. R. Garrett, Phys. Rev. A 44, 7684 (1991)]; excellent agreement is observed. We also report the observation of suppression of pressure-induced wing absorption into the three-photon state observed in a classic ``hybrid'' resonance mode of excitation.

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Canadian Journal of Physics•Nov 1, 1994•4 citations

Theory of the effect of odd-photon destructive interference on optical shifts in resonantly enhanced multiphoton excitation and ionization

M. G. Payne, L. Deng, W. R. Garrett

We present a theory for two- and three-photon excitation, optical shifting, and four-wave mixing when a first laser is tuned onto, or near, a two-photon resonance and a second much more intense laser is tuned near or on resonance between the two-photon resonance and a second excited state. When the second excited state has a dipole-allowed transition back to the ground state and the concentration is sufficiently high, a destructive interference is produced between three-photon coupling of the ground state and the second excited state and one-photon coupling between the same states by the internally generated four-wave mixing field. This interference leads to several striking effects. For instance, as the onset of the interference occurs, the optical shifts in the two-photon resonance excitation line shape become smaller in copropagating geometry so that the line shapes for multiphoton ionization enhanced by the two-photon resonance eventually become unaffected by the second laser. In the same range of concentrations the four-wave mixing field evolves to a concentration-independent intensity. With counterpropagating laser beams the line shape exhibits normal optical shifts like those observed for both copropagating and counterpropagating laser beams at very low concentrations. The theoretical work presented here extends our earlier works by including the effect of laser bandwidth and by removing the restriction of having the second laser be tuned far from three-photon resonance. In this way we have now included, as a special case, the effect of both laser bandwidth and interference on laser-induced transparency. Unlike other effects related to odd-photon destructive interference, the effect of a broad bandwidth is to bring about the predicted effects at much lower concentrations. Studies in rubidium show good agreement between theory and experiment for both ionization line shapes and four-wave mixing intensity as a function of concentration.

Physical Review A•Aug 1, 1998•10 citations
We report an experiment in xenon which confirms the theoretical predictions (Payne et al, Phys. Rev. A48, 2334 (1993)) on the pressure dependent suppression of the ac Stark shifting of even‐photon resonances. In the co‐propagating configuration the ac Stark due to a second laser is totally suppressed at elevated concentrations due to a destructive interference between two excitation pathways. The ac Stark shift persists in the counter‐propagating configuration because of the absence of destructive interference.
We report detailed experimental results in xenon that confirm theoretical predictions [Payne et al., Phys. Rev. A 48, 2334 (1993)] on the interference-based suppression of ac Stark shifting of even-photon resonances under circumstances where the shift is produced through strong coupling to a state that is also coupled back to the ground state. In the copropagating-beam configuration and in the pressure range of 0.5--250 Torr, the multiphoton ionization spectral line shape is unchanged regardless of the presence of the second laser field, i.e., the ac Stark shift introduced by the second laser is totally suppressed due to a complete destructive interference between two excitation pathways. In the counterpropagating-beam configuration, however, the ac Stark shift persists in the range of the pressure studied. By choosing a different set of energy levels where no four-wave-mixing field is permitted, we show that the very same ac Stark shift introduced by the second laser field persists even with copropagating-beam configuration, as predicted by theory.
We describe ac Stark shift production and measurement in a two-laser mode where a first laser is tuned through a two-photon resonance between the ground state and an excited state in order to record a line shape for the corresponding resonantly enhanced multiphoton ionization. A second laser is tuned to a fixed wavelength which is close to a resonance between the upper state in the two-photon transition and a third state which has dipole-allowed transitions back to the ground state. At low concentrations the second laser leads to very large ac Stark shifts in the two-photon excitation and in the related resonantly enhanced multiphoton ionization. However, at high concentrations a destructive interference occurs involving the three-photon coupling between the third state and the ground state and the one-photon coupling due to the four-wave-mixing field at frequency 2${\mathrm{\ensuremath{\omega}}}_{\mathit{L}1}$\ifmmode\pm\else\textpm\fi{}${\mathrm{\ensuremath{\omega}}}_{\mathit{L}2}$. This interference leads to a pressure-dependent suppression of the amplitude for the third state. When this destructive interference occurs, the ac Stark shift due to the second laser undergoes a corresponding pressure-dependent suppression. The criteria for the pressure to be high enough to completely suppress the ac Stark shift is that the real part of phase mismatch \ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert} at the angular frequency 2${\mathrm{\ensuremath{\omega}}}_{\mathit{L}1}$\ifmmode\pm\else\textpm\fi{}${\mathrm{\ensuremath{\omega}}}_{\mathit{L}2}$ and (or) the absorption coefficient \ensuremath{\beta} at the same frequency should be very large, so that with unfocused focused beams \ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert}L>5[(${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$\ensuremath{\tau}]1/2{]}^{1/2}]1/2, where L is the thickness of gas penetrated before the shift is measured, ${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$ is the maximum ac Stark shift at very low pressure, and \ensuremath{\tau} is the pulse length of the lasers.At positions and concentrations such that 1\ensuremath{\Vert}\ensuremath{\Delta}k\ensuremath{\Vert}L\ensuremath{\le}2[(${\mathrm{\ensuremath{\Delta}}}_{\mathit{s}}^{(\mathrm{max})}$\ensuremath{\tau})]1/2{]}^{1/2}]1/2 the ac Stark shift is present but the two-photon excitation is suppressed due to a destructive interference between excitation by two photons from the first laser and by two-photon excitation between a four-wave-mixing photon and a photon from the second laser.
We use resonance ionization involving two colors in single-pass and retroreflected geometries to study the suppression of excitation of a four-photon resonance by an interference involving four-wave sum-frequency generation occurring near an intermediate three-photon resonance. The 6p[1/2](J=0) state of xenon is excited by three blue photons plus one infrared photon. One beam, focused to I1{\mathit{I}}_{1}I1​\ensuremath{\simeq}7\ifmmode\times\else\texttimes\fi{}109{10}^{9}109 W/cm2{\mathrm{cm}}^{2}cm2, is nearly three-photon resonant with the 6s[3/2](J=1) resonance; the second, unfocused beam (I2{\mathit{I}}_{2}I2​\ensuremath{\simeq}2\ifmmode\times\else\texttimes\fi{}107{10}^{7}107 W/cm2{\mathrm{cm}}^{2}cm2) is tuned to maintain exact four-photon resonance with the 6p[1/2](J=1) state. One additional blue photon ionizes from the four-photon level. Third-harmonic light is generated by the first, nearly three-photon-resonant beam by four-wave sum-frequency mixing. One third-harmonic photon plus one photon from the second laser form a second excitation pathway to the four-photon level; destructive interference between the two pathways results in a reduction in the observed ionization. The degree of reduction depends on the xenon density and the detuning (both positive and negative) from three-photon resonance. This interference may be overcome by retroreflecting the nearly three-photon-resonant beam to provide an additional excitation pathway which generates no third harmonic.The study provides detailed information on the pressure-dependent range from exact resonance over which the familiar three-photon cancellation effect is operative; it shows that the interference occurs in high- and low-energy regions about three-photon resonance; and it establishes that interference is produced for large values of the phase mismatch even if the absorption of the interfering field is low. We compare our measurements of the reduction in ionization with predictions published by us elsewhere [M. G. Payne, J. C. Miller, R. C. Hart, and W. R. Garrett, Phys. Rev. A 44, 7684 (1991)]; excellent agreement is observed. We also report the observation of suppression of pressure-induced wing absorption into the three-photon state observed in a classic ``hybrid'' resonance mode of excitation.
A system is described in which a real molecular state is tuned into and out of resonance with the intermediate level of a two-photon transition, by the laser-induced ac-Stark effect. Two narrow-band CO2 wave-guide lasers are utilized to induce rovibrational transitions in the ν3 ladder of SF6. A weak probe laser monitors the absorption for the [Formula: see text] two-photon transition. Simultaneously, a strong pump laser is in resonance with the [Formula: see text] one-photon transition. The ac-Stark splitting is observed and quantum interferences between two-photon amplitudes involving different intermediate states occur. It is demonstrated that destructive interference allows suppression of the two-photon excitation for an appropriate pump laser power. Simulations based on the Dressed State Picture and the optical Bloch equations show a satisfactory agreement with the experiment.
We present a theory for two- and three-photon excitation, optical shifting, and four-wave mixing when a first laser is tuned onto, or near, a two-photon resonance and a second much more intense laser is tuned near or on resonance between the two-photon resonance and a second excited state. When the second excited state has a dipole-allowed transition back to the ground state and the concentration is sufficiently high, a destructive interference is produced between three-photon coupling of the ground state and the second excited state and one-photon coupling between the same states by the internally generated four-wave mixing field. This interference leads to several striking effects. For instance, as the onset of the interference occurs, the optical shifts in the two-photon resonance excitation line shape become smaller in copropagating geometry so that the line shapes for multiphoton ionization enhanced by the two-photon resonance eventually become unaffected by the second laser. In the same range of concentrations the four-wave mixing field evolves to a concentration-independent intensity. With counterpropagating laser beams the line shape exhibits normal optical shifts like those observed for both copropagating and counterpropagating laser beams at very low concentrations. The theoretical work presented here extends our earlier works by including the effect of laser bandwidth and by removing the restriction of having the second laser be tuned far from three-photon resonance. In this way we have now included, as a special case, the effect of both laser bandwidth and interference on laser-induced transparency. Unlike other effects related to odd-photon destructive interference, the effect of a broad bandwidth is to bring about the predicted effects at much lower concentrations. Studies in rubidium show good agreement between theory and experiment for both ionization line shapes and four-wave mixing intensity as a function of concentration.