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Physical Review A

Effect of quantum interference on multiphoton resonant excitation involving high-lying Rydberg orbitals

L. Deng, W. R. Garrett, M. G. Payne, D. Z. Li

Published Feb 1, 1996• 1 citation
Publisher

Abstract

We report observations of destructive quantum interference in multiphoton resonant excitation of high-lying Rydberg states in xenon. In a recent laser-induced breakdown experiment by Peet [Phys. Rev. A 51, 3982 (1995)], it was claimed that the interference was absent for such high-lying states. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.1194

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We report observations of destructive quantum interference in multiphoton resonant excitation of high-lying Rydberg states in xenon. In a recent laser-induced breakdown experiment by Peet [Phys. Rev. A 51, 3982 (1995)], it was claimed that the interference was absent for such high-lying states. \textcopyright{} 1996 The American Physical Society.
Through multiphoton ionization measurements, the polarization effects in destructive quantum interference under three-photon resonant excitation have been studied. Recent observations [V. Peet, Phys. Rev. A 74, 033406 (2006)] have indicated that contrary to the well-known pattern of a total suppression of resonance excitation, the destructive interference becomes incomplete if three-photon transition is driven by crossed beams with orthogonal polarization planes. These observations have been tested for a more general case of two-color excitation and very similar polarization-dependent anomalies in the interference character have been registered. It has been shown that the destructive interference is modified and the resonance excitation does occur if two crossed laser beams have opposite circular polarizations. The pressure-induced evolution of the uncanceled ionization peaks has the ratio of blue shift to width close to 0.5 exactly as it is known for resonance ionization peaks registered under excitation by counterpropagating laser beams.
Three-photon excitation and associated wave mixing near the 6s6s6s and $6{s}^{\ensuremath{'}}$ resonances of xenon have been studied utilizing resonance-enhanced multiphoton ionization in angled beams with different polarizations. It has been shown that a complete cancellation of three-photon resonant atomic excitation caused by the well-known destructive wave-mixing interference occurs in sss and ppp polarization of angled beams but distinct resonance ionization enhancement is observed when pump beams have orthogonal polarization planes. Pressure-induced evolution of the resonance ionization peak in cross-polarized beams is identical to that observed with counterpropagating beams. The reason for such resonance ionization enhancement is unknown and cannot be explained within the frame work of existing theory. The effect may result from some peculiarities of wave-mixing interference in a multilevel atomic system, where different degenerate magnetic sublevels of the upper atomic state and multiple interfering excitation processes are involved. Another possibility is that the resonance ionization enhancement results from a process where weak counterpropagating light is generated within the excitation region of cross-polarized angled beams.
Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J=2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2]1o{]}_{1}^{\mathit{o}}]1o​ state. The well-known destructive interference for the ``on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide a new insight in interference effects involved in multiphoton-excitation processes.
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.
Partial cancellation of the ionization signal in the four-photon-resonant five-photon ionization via J = 2 4f and 5f resonances in Xe has been observed at increased gas pressures. Experiments with one and two counterpropagating laser beams provide strong evidence that cancellation is due to destructive interference at the three-photon step between the coherent three- and one-photon excitation channels, the latter involving one vacuum ultraviolet photon of the third-harmonic generation that occurs above the 6s[3/2]1o state. The well-known destructive interference for the ''on-resonance'' case is now shown to occur also for large detuning from the resonance (up to 2000 cm-1) probed by four-photon-resonant five-photon ionization. This type of cancellation may provide new insight in interference effects involved in multiphoton-excitation processes.
We conduct a systematic investigation of the oscillations of the Rydberg-state populations as a function of intensity arising from strong-field multiphoton excitation of Rydberg atoms. By numerically solving the time-dependent Schrödinger equation and by constructing a quantum model based on Freeman resonances, we elucidate the underlying physical mechanisms governing the intensity-dependent oscillatory behavior of the Rydberg-state population dynamics. Our analysis shows that these oscillations originate from the synergistic interplay of three distinct quantum-interference mechanisms: (1) interference between excitation pathways at the rising and falling edges of the laser pulse (long-time interference), (2) interference between different optical cycles within the same side of the laser pulse (short-time interference), and (3) interference within individual optical cycles (intracycle interference). Additionally, we find that ground-state depletion has varying degrees of influence on the oscillation patterns formed by the three interference mechanisms under different laser-intensity conditions.