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arXiv:1509.04571 · Physical Review A

Selective strong-field enhancement and suppression of ionization with short laser pulses

N. A. Hart, James Strohaber, Alexandre A. Kolomenskii, G. G. Paulus, D. Bauer, Hans A. Schuessler

Published Jun 28, 2016• 27 citations
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Abstract

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 $(>{10}^{12}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2})$. 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.

DOI
10.1103/physreva.93.063426

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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.
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.
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.
We present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2 + 1 + 1 resonance enhanced multi-photon ionization (REMPI) proceeds via the strongly driven two-photon transition 4s←←3s, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3 + 1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark shifts and level crossings. In particular, we show that under the experimental conditions the passage through an uncommon three-state 'bow-tie' level crossing allows the preparation of coherent superposition states.
We have observed suppression of ionization in Rydberg atoms irradiated by an intense short-pulse laser field. We find that single-photon ionization of the outer electron in a Ba 6snk Stark state can be severely suppressed relative to high-order (\ensuremath{\ge}3 photon) nonresonant multiphoton ionization of the tightly bound 6s core electron. This population trapping occurs in intense short laser pulses, where the bandwidth of the ionizing laser is greater than the spacings between adjacent Stark states, and may be due to a substantial modification of the initial Stark state via stimulated Raman processes through the continuum. The Ba+∗{\mathrm{Ba}}^{+\mathrm{*}}Ba+∗ ion should be left in a higly excited superposition state, or wave packet.
We propose and analyze a scheme for adiabatic creation of maximum coherence of 0.5 with a controllable phase between a ground state and the excited state in a model Λ-structured atom using two short laser pulses. One of the pulses has constant carrier frequency quasi-resonant with transition between an initially empty ground and the excite states. The frequency of the second pulse is swept through the resonance with the adjacent transition between the initially populated ground state and the common excited state of the atom. We demonstrate high degree of robustness of the scheme against variation of parameters of the laser radiation in relatively broad region of values. The proposed scheme may find practical applications in the field of multi-photon ionization, high-order harmonics and Raman sideband generation, as well as in nonlinear wave mixing in coherently prepared media.
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.