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Physical Review A

Rydberg-atom stabilization against photoionization: An analytically solvable model with resonance

Antoni Wójcik, R. Parzyński

Published Sep 1, 1994• 17 citations
Publisher

Abstract

Stimulated by a recent experiment [L. D. Noordam et al., Phys. Rev. Lett. 68, 1496 (1992)], we present a model of Rydberg-atom photoionization whose essential feature is the resonance between the initially populated Rydberg state and an additional state lying below Rydberg quasicontinuum. Despite the infinite number of discrete states involved in our model we have obtained the expressions for photoionization yield and discrete-state populations in completely analytical form. These expressions cover both short- and long-time scales, i.e., when laser-pulse duration is shorter or longer than the classical round-trip time of the Rydberg electron. The short-time scale corresponds to the conditions met in the experiment of Noordam et al. and, on the basis of our expressions, we have gained at least qualitative understanding of their observations. In the case of long pulses, which in our considerations are never longer than 54 ps, near resonance is shown to be the origin of a profound ionization suppression, particularly for some specific frequencies, which we identify as those ensuring the formation of a perfectly dark dressed state of zero width and thus unionizable. This dark state is shown to be populated with a probability increasing when laser gets stronger. We discuss the connection between stabilization and formation of this perfectly dark state as well as of additional dressed states, which are dark in the sense that they have the property of becoming very narrow as laser intensity increases. The undamped perfectly dark state, created at specific laser frequencies, has given us rise to introduce what we call the zero-pole approximation for ionization yield, which, as we have shown, works well if duration and intensity of laser pulse are appropriately combined.

DOI
10.1103/physreva.50.2475

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Basic Energy Sciences, under Award number DE-SC0012193.

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ization of Rydberg atoms by a single-cycle pulse, and also its implications for the strong field ionization of ground state. The required threshold field amplitude (for 10% ionization probability) scales inversely with the binding energy of initial states and also the pulse-duration square when the pulse duration becomes much shorter than the classical Rydberg period. A simple model is introduced to understand this threshold behavior, where the nonzero displacement induced by a single-cycle pulse plays a critical role. By combining with the adiabatic-ionization threshold in the low-frequency limit, an ionization window is expected for the ionization of different states. The ionization-probability curve exhibits a “ripple” structure as a function of the pulse duration and the field amplitude, which is sensitive to the angular distribution of initial states. The observation of larger emitted-electron energy for the ionization of lower-lying Rydberg states in a recent experiment [S Li and R. R. Jones, Phys. Rev. Lett. 112, 143006 (2014)] is confirmed in our calculations for both sodium and hydrogen atoms. The differences between the ionization dynamics in a single-cycle pulse and that in a multi-cycle pulse are also discussed and presented.

•Jan 1, 2015•0 citations
Stimulated by a recent experiment [L. D. Noordam et al., Phys. Rev. Lett. 68, 1496 (1992)], we present a model of Rydberg-atom photoionization whose essential feature is the resonance between the initially populated Rydberg state and an additional state lying below Rydberg quasicontinuum. Despite the infinite number of discrete states involved in our model we have obtained the expressions for photoionization yield and discrete-state populations in completely analytical form. These expressions cover both short- and long-time scales, i.e., when laser-pulse duration is shorter or longer than the classical round-trip time of the Rydberg electron. The short-time scale corresponds to the conditions met in the experiment of Noordam et al. and, on the basis of our expressions, we have gained at least qualitative understanding of their observations. In the case of long pulses, which in our considerations are never longer than 54 ps, near resonance is shown to be the origin of a profound ionization suppression, particularly for some specific frequencies, which we identify as those ensuring the formation of a perfectly dark dressed state of zero width and thus unionizable. This dark state is shown to be populated with a probability increasing when laser gets stronger. We discuss the connection between stabilization and formation of this perfectly dark state as well as of additional dressed states, which are dark in the sense that they have the property of becoming very narrow as laser intensity increases. The undamped perfectly dark state, created at specific laser frequencies, has given us rise to introduce what we call the zero-pole approximation for ionization yield, which, as we have shown, works well if duration and intensity of laser pulse are appropriately combined.
We show that, when an atom prepared in a high Rydberg state is one-photon ionized by a laser, a near resonance with some lower-lying state permits the formation of a nondecaying dark state of the coupled laser–atom system. This dark state traps population in an amount that increases to some upper limit as the laser radiation used becomes stronger. Thus the dark state formed causes a decrease in the Rydberg-atom ionization with increasing laser intensity, i.e., stabilization, which survives even for long times. This long-time stabilization is described by a simple zero-pole formula, and the physical meaning of the term long time is explained. We estimate, for model situations, the laser frequencies that ensure dark-state formation and maximum ionization suppression. The laser pulse intensity and duration that are required for the observation of the dark state are evaluated.
We have observed that the amount of photoionization from an atomic Rydberg state with a pulsed laser depends critically on the length of the pulse, whereas lowest-order perturbation theory implies that the yield depends only on the fluence (the integrated intensity) of the pulse. We have measured the yield for one-photon ionization with short (0.5–2.7-ps) high-intensity laser pulses from the 27d Rydberg state in barium. With equal fluence, the yield decreases for pulses shorter than the Kepler orbit time of the outer electron (2.2 ps) because not all of its wave function comes near the core during the length of the pulse. The observations and this classical picture are confirmed by quantum-mechanical calculations.
We describe a detailed account of an experiment demonstrating light-induced stabilization against photoionization. The choice of initial state and atom is discussed in relation to the laser wavelength and laser pulse duration. In combination with a 100-fs, 620-nm probe pulse, the optimum choice is the circular 5g state in neon. A picosecond pump laser was used to prepare this Rydberg state. Initially, the population in this state was probed with a nanosecond laser pulse. Subsequently, the nanosecond probe pulse was replaced by an intense, (sub)picosecond pulse and the photoionization signal was studied. When the probe intensity is several times 1013{10}^{13}1013 W/cm2{\mathrm{cm}}^{2}cm2 a decrease in yield with respect to a less intense pulse with the same fluence is observed, which indicates stabilization. The results are in accordance with recent theoretical predictions.
When exposed to intense light of \ensuremath{\sim}580 nm, the ground state of K shifts up in energy, passing through two-photon resonances with Rydberg states and finally crossing the two-photon ionization limit. Using laser pulses of 0.5 to 13 ps duration, we have shown experimentally that ionization occurs for short pulses, but for long pulses the population is diverted into the Rydberg states where some population survives the peak intensity of the pulse, in excellent agreement with a dynamic Floquet model.
Photoionization of Rydberg atoms is considered in the framework of the quasiclassical (WKB) approach. Distribution of the photoelectron density in space and time is found and analyzed. This distribution is shown to consist of two main parts: the temporary population, which exists only as long as the light field is on; and the population corresponding to irreversible ionization. The irreversible-ionization wave packets are shown to experience the effect referred to as Coulomb narrowing. An origin of this effect and the conditions of its existence are discussed. In a strong field, rather simple analytical expressions are found for the partial probabilities of above-threshold ionization and for the total probability of ionization. In contrast to many earlier works, in the present theory neither the rotating-wave nor ``pole'' approximations are used, and the results are derived for an arbitrary pulse shape. Strong-field interference stabilization of Rydberg atoms is confirmed to occur at pulse durations shorter than the Kepler period. The arising regimes of interference stabilization are analyzed in comparison with the predictions of earlier works.
ization of Rydberg atoms by a single-cycle pulse, and also its implications for the strong field ionization of ground state. The required threshold field amplitude (for 10% ionization probability) scales inversely with the binding energy of initial states and also the pulse-duration square when the pulse duration becomes much shorter than the classical Rydberg period. A simple model is introduced to understand this threshold behavior, where the nonzero displacement induced by a single-cycle pulse plays a critical role. By combining with the adiabatic-ionization threshold in the low-frequency limit, an ionization window is expected for the ionization of different states. The ionization-probability curve exhibits a “ripple” structure as a function of the pulse duration and the field amplitude, which is sensitive to the angular distribution of initial states. The observation of larger emitted-electron energy for the ionization of lower-lying Rydberg states in a recent experiment [S Li and R. R. Jones, Phys. Rev. Lett. 112, 143006 (2014)] is confirmed in our calculations for both sodium and hydrogen atoms. The differences between the ionization dynamics in a single-cycle pulse and that in a multi-cycle pulse are also discussed and presented.