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arXiv:physics/0609074 · Physical Review A

Selective excitation of metastable atomic states by femto- and attosecond laser pulses

Alexey D. Kondorskiy, Леонид Петрович Пресняков, Yuri V. Ralchenko

Published Sep 20, 2006• 0 citations
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Abstract

The possibility of achieving highly selective excitation of low metastable states of hydrogen and helium atoms by using short laser pulses with reasonable parameters is demonstrated theoretically. Interactions of atoms with the laser field are studied by solving the close-coupling equations without discretization. The parameters of laser pulses are calculated using different kinds of optimization procedures. For the excitation durations of hundreds of femtoseconds direct optimization of the parameters of one and two laser pulses with Gaussian envelopes is used to introduce a number of simple schemes of selective excitation. To treat the case of shorter excitation durations, optimal control theory is used and the calculated optimal fields are approximated by sequences of pulses with reasonable shapes. A way to achieve selective excitation of metastable atomic states by using sequences of attosecond pulses is introduced.

DOI
10.1103/physreva.74.033410

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The possibility of achieving highly selective excitation of low metastable states of hydrogen and helium atoms by using short laser pulses with reasonable parameters is demonstrated theoretically. Interactions of atoms with the laser field are studied by solving the close-coupling equations without discretization. The parameters of laser pulses are calculated using different kinds of optimization procedures. For the excitation durations of hundreds of femtoseconds direct optimization of the parameters of one and two laser pulses with Gaussian envelopes is used to introduce a number of simple schemes of selective excitation. To treat the case of shorter excitation durations, optimal control theory is used and the calculated optimal fields are approximated by sequences of pulses with reasonable shapes. A way to achieve selective excitation of metastable atomic states by using sequences of attosecond pulses is introduced.
The development of methods of generation of ultrashort pulses (USP) of femto- and attosecond duration ranges with controlled parameters necessitates the theoretical study of features of their interaction with a matter. Among such features that do not exist in case of “long” pulses should first of all be the nonlinear dependence of the photoprocess probability W on the USP duration as well as the dependence on the carrier phase with respect to the pulse envelope. It should be noted that if the dependence of the probability W on the phase manifests itself either only for very short pulses, when ωt 1 too for fields of moderate strength, when the perturbation theory is applicable. The present work is dedicated to the theoretical analysis of two-photon excitation of hydrogen atom in a discrete energy spectrum by ultrashort electromagnetic pulses of femto- and subfemtosecond ranges of durations. As examples, excitation of hydrogen atom from the ground state to excited states with a zero orbital moment is considered.
Abstract The dynamics of photoexcitation of the hydrogen atom in the discrete and continuous spectra under the action of laser pulses in the attosecond range of time and pulse durations has been analyzed using perturbation theory. It is shown that over time interval shorter than or on the order of pulse duration, the time dependence of the photoexcitation probability is generally oscillating by nature. It has been established that for certain values of parameters, the envelope of this dependence has a peak, the position of which is determined by the pulse duration and carrier frequency.
The development of methods of generation of ultrashort pulses (USP) of femto- and attosecond duration ranges with controlled parameters necessitates the theoretical study of features of their interaction with a matter [1]. Among such features that do not exist in case of “long” pulses should first of all be the nonlinear dependence of the photoprocess probability W on the USP duration (τ) [2] as well as the dependence on the carrier phase with respect to the pulse envelope (φ) [3-4]. It should be noted that if the dependence of the probability W on the phase φ manifests itself either only for very short pulses, when ωτ < 1 (ω is carrier frequency of the pulse), or in case of a nonlinear photoprocess [3], the function W(τ) can differ from a linear function in the limit ωτ> 1 too for fields of moderate strength, when the perturbation theory is applicable [2].
Optimal laser control for ultrafast selection of closely lying excited states whose energy separation is smaller than the laser bandwidth is reported on the two-photon transition of atomic cesium; Cs(6S-->7D(J), J=5/2 and 3/2). Selective excitation was carried out by pulse shaping of ultrashort laser pulses which were adaptively modulated in a closed-loop learning system handling eight parameters representing the electric field. Two-color fluorescence from the respective excited states was monitored to measure the selectivity. The fitness used in the learning algorithm was evaluated from the ratio of the fluorescence yields. After fifty generations, a pair of nearly transform-limited pulses were obtained as an optimal pulse shape, proving the effectiveness of the "Ramsey fringes" mechanism. The contrast of the selection ratio was improved by approximately 30% from the simple "Ramsey fringes" experiment.
Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.
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.