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Coherent control of strong-field two-pulse ionization of Rydberg atoms

Mikhail Vladimirovich Fedorov, Nikolay Poluektov

Published Feb 28, 2000• 7 citations
Publisher

Abstract

Strong-field ionization of Rydberg atoms is investigated in its dependence on phase features of the initial coherent population of Rydberg levels. In the case of a resonance between Rydberg levels and some lower-energy atomic level (V-type transitions), this dependence is shown to be very strong: by a proper choice of the initial population an atom can be made either completely or very little ionized by a strong laser pulse. It is shown that phase features of the initial coherent population of Rydberg levels and the ionization yield can be efficiently controlled in a scheme of ionization by two strong laser pulses with a varying delay time between them.

DOI
10.1364/oe.6.000117

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Journal of Physics B Atomic Molecular and Optical Physics•Feb 28, 1998•9 citations
Strong-field ionization of Rydberg atoms is investigated in its dependence on phase features of the initial coherent population of Rydberg levels. In the case of a resonance between Rydberg levels and some lower-energy atomic level (V-type transitions), this dependence is shown to be very strong: by a proper choice of the initial population an atom can be made either completely or very little ionized by a strong laser pulse. It is shown that phase features of the initial coherent population of Rydberg levels and the ionization yield can be efficiently controlled in a scheme of ionization by two strong laser pulses with a varying delay time between them.
It is shown that the rate and degree of ionization of an atom can be controlled by preparing a specific superposition of Rydberg states. This effect is due to the Raman interaction of Rydberg levels via resonant lower-lying levels of the atom. Depending on the initial population of an atom interacting with a strong laser field, the atom either ionizes completely or exhibits an extremely high degree of stability (in this case the probability of the atom remaining in a bound state when the laser pulse is switched off is close to 1). It is shown that states which are stable against ionization decay or, conversely, decay rapidly into the continuum can be prepared using double laser pulses with a controllable time delay.
We experimentally demonstrate robust selective excitation and attenuation of atomic Rydberg level populations in sodium vapor (Na i) using intense laser pulses in the strong-field limit (>1012W/cm2)(>{10}^{12}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2})(>1012W/cm2). Coherent control of the atomic population and related ionization channels is realized for intensities above the over-the-barrier ionization intensity. Moreover, atomic excitation selectivity and high ionization yield are simultaneously achieved without the need to tailor the spectral phase of the laser. A qualitative model confirms that this strong-field coherent control arises through the manifestation of a Freeman resonance.
Excitation and photoionization of Rydberg wave packets are described. Interference of bound-free transitions from many coherently populated Rydberg levels is shown to affect the dependence of the photoionization probability on the duration of interaction. Strong-field interference effects in such a system are described also. The most important of these is the field-induced interference stabilization of Rydberg atoms in a strong ionizing field. The intensity range in which this effect can exist is determined. The results derived are used for a qualitative model describing supercontinuum emission in the process of multiphoton ionization.
The coherent control of atomic energy level population is important for several areas physics and engineering including fluorescent spectroscopy, resonantly enhanced multiphoton ionization, harmonic generation, remote sensing and lasing. At low intensities where the Stark shift can be neglected, coherent control mechanisms usually exploit resonances created from stationary energy states dressed by integer multiples of the photon energy. However, in the strong field limit where large laser pulse intensities lead to significant Stark shifts, the resonant conditions are dynamic both in time and space and will likely not be satisfied for the entire laser pulse or beam.\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. We also make a direct measurement of the ponderomotive shift of the continuum. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.\n\n\nIn this research, we experimentally and theoretically demonstrate coherent control of atomic energy level population in sodium vapor as well as the selective excitation of sodium Rydberg levels using high intensity laser pulses. While techniques based on resonance interferences and rapid adiabatic passage have been introduced for selective excitation, the conditions that must be satisfied for these phenomena can be hampered by short femtosecond pulse durations and large Stark shifts. In contrast, a technique referred to here as Resonance Sampling, uses the AC Stark shifts to selectively induce Freeman resonances and is resilient to changes in the spectral phase. Freeman resonances established in this way can result in population inversion of the excited state, and may lead to new lasing mediums and remote sensing applications.
A theoretical analysis of the phase control of a two-channel atomic ionization scheme is given. We report results on phase-selective excitation, both with square and smooth laser pulses. We show that the phenomenon of population trapping, which is known to occur in this system, can be greatly influenced by the phase difference of the lasers involved in the excitation. As a result, the time dependences of the ionization probability, the populations in the bound states and the form of the photoelectron energy spectra can all be controlled by varying the phase difference of the lasers. We also show that for specific atomic and phase parameters population can be entirely trapped within a superposition state, totally immune to decay, with no ionization whatsoever.
A theoretical analysis of the phase control of a two-channel atomic ionization scheme is given. We report results on phase-selective excitation, both with square and smooth laser pulses. We show that the phenomenon of population trapping, which is known to occur in this system, can be greatly influenced by the phase difference of the lasers involved in the excitation. As a result, the time dependences of the ionization probability, the populations in the bound states and the form of the photoelectron energy spectra can all be controlled by varying the phase difference of the lasers. We also show that for specific atomic and phase parameters population can be entirely trapped within a superposition state, totally immune to decay, with no ionization whatsoever.