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Physical Review A

Phase control of resonantly enhanced photoionization in an optically dense medium

David Petrosyan, P. Lambropoulos

Published Mar 20, 2001• 9 citations
Publisher

Abstract

We present a self-consistent theory, as well as analytical and numerical results, for the three-photon--one-photon phase control of resonantly enhanced photoionization in an optically dense medium of xenon gas. We show that for an optically thick medium, the standard phase-control technique has a rather limited application since, independently of the initial relative phase between the two fields, over a very short scaled distance of propagation the medium tends to settle such a relative phase that exactly cancels the atomic excitation. Rather unusual results for an optically thin layer of atoms are also found.

DOI
10.1103/physreva.63.043417

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We present a self-consistent theory, as well as analytical and numerical results, for the three-photon--one-photon phase control of resonantly enhanced photoionization in an optically dense medium of xenon gas. We show that for an optically thick medium, the standard phase-control technique has a rather limited application since, independently of the initial relative phase between the two fields, over a very short scaled distance of propagation the medium tends to settle such a relative phase that exactly cancels the atomic excitation. Rather unusual results for an optically thin layer of atoms are also found.
We present a self-consistent theory and analytical results for the three-photon-one-photon coherent control of ionization in an optically dense autoionizing medium. We show that for an optically thick medium, over a short scaled propagation distance, the phase and amplitude of the harmonic field settle to values that are fully determined by the atomic and fundamental field parameters and are completely independent of the initial relative phase between the two fields, thus preventing efficient phase control of the autoionization and its products. Control of the autoionization and the branching ratio of its products is still feasible, however, through the variation of the detuning of the fundamental field from the atomic transition resonance.
We present a self-consistent theory, as well as an illustrative application to a realistic system, of phase control of photoabsorption in an optically dense medium. We demonstrate that, when propagation effects are taken into consideration, the impact on phase control is significant. Independent of the value of the initial phase difference between the two fields, over a short scaled distance of propagation, the medium tends to settle the relative phase so that it cancels the atomic excitation. In addition, we find some rather unusual behavior for an optically thin layer.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
We consider three-photon--one-photon phase control of resonance-enhanced photonioization with a phase-diffusion field. As is well known, control is achieved because excitation via the fundamental field interferes with excitation via the third harmonic field, and the form of the interference (i.e., constructive or destructive) depends on the relative phase difference between the two fields. In the problem, the stochastic nature of the field influences control because the propagation constant of a dispersive medium depends on the field's fluctuating frequency. Here, we approach the influence of laser phase noise on control via (i) a physically intuitive zeroth-order approximation, (ii) first-order perturbation theory, and (iii) numerical simulation. Our results show that first-order perturbation theory is not attractive for the study of this problem, since it requires the evaluation of very high order correlation functions associated with the fundamental field"s fluctuating frequency. More importantly, however, numerical simulation demonstrates that highly efficient control can be attained even in the presence of very large linewidth fields.
The destructive interference between the three-photon and the third-harmonic one-photon absorption in the vicinity of the 6s[3/2]1{]}_{1}]1​ state of Xe has been studied in the resonantly enhanced multiphoton ionization via nf states, through the cancellation of the nf, J=2 resonances of the spectrum, accessible by four-photon absorption. The gas-pressure, i.e., phase-matching, dependence of the three-photon detuning range from the 6s[3/2]1{]}_{1}]1​ state for which cancellation occurs has been investigated in one- and two-color experiments, including positive detuning from this state in positively dispersive regions. For obtaining cancellation, the theoretically predicted requirement of optically thick medium at the third-harmonic frequency is corroborated by present observations for negative detunings. The different cancellation behavior of the nf[3/2]2{]}_{2}]2​ and nf[5/2]2{]}_{2}]2​ states observed indicates the dependence of the effect on the atomic parameters of the coupled four-photon resonance. The experimental results are found to be in partial agreement with existing theoretical models.