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Quantum Electronics

Nonresonant interaction of ultrashort electromagnetic pulses with multilevel quantum systems

É. M. Belenov, Vladimir A. Isakov, A. Nazarkin

Published Nov 30, 1993• 11 citations
Publisher

Abstract

A theory is derived for the excitation of a multilevel quantum system by an electromagnetic pulse whose length is much shorter than the reciprocal of the frequency of transitions between levels. This interaction is characterized by a selectivity of a new type, which does not involve resonant properties of the substance. It instead stems from selection rules for transitions between levels and from the vanishing of the "area" defined by the integral of the electromagnetic field intensity. This selectivity mechanism could be exploited to create a deviation from equilibrium in a multilevel quantum system. In particular, there is the possibility of a nonresonant excitation and dissociation of molecules by femtosecond electromagnetic pulses.

DOI
10.1070/qe1993v023n11abeh003222

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A theory is derived for the excitation of a multilevel quantum system by an electromagnetic pulse whose length is much shorter than the reciprocal of the frequency of transitions between levels. This interaction is characterized by a selectivity of a new type, which does not involve resonant properties of the substance. It instead stems from selection rules for transitions between levels and from the vanishing of the "area" defined by the integral of the electromagnetic field intensity. This selectivity mechanism could be exploited to create a deviation from equilibrium in a multilevel quantum system. In particular, there is the possibility of a nonresonant excitation and dissociation of molecules by femtosecond electromagnetic pulses.
Some features of the excitation of multilevel quantum systems under the action of electromagnetic pulses which are shorter than the inverse frequency of interlevel transitions are considered. It is shown that the interaction is characterized by a specific type of selectivity which is not connected with the resonant absorption of radiation. The simplest three-level model displays the inverse population of upper levels. The effect of an ultrashort laser pulse on a multilevel molecule was regarded as an instant reception of the oscillation velocity by the oscillator and this approach showed an effective excitation and dissociation of the molecule. The estimations testify to the fact that these effects can be observed using modern femtosecond lasers.
The Maxwell–Schrödinger equations describing the ultrashort laser pulse propagation in multilevel molecular media are shown to be analytically solvable and to reduce to nonlinear multisine-Gordon equations for certain models of the field–molecule system. Special cases of level schemes are shown to lead to soliton propagation. A numerical study is presented in order to examine the effect of nonresonant (virtual) transitions on pulse propagation and amplification in a three-level molecular system as a function of intensity and detuning.
Based on an approximate solution of the Schrödinger equation, the effect that a pair of extremely short small-amplitude subcycle pulses has on a quantum system is studied. It is shown that, if the pulses are shorter than the inverse frequencies of atomic transitions, the probability of transitions between levels is determined by the electric area of the pulses and the time delay between them. As a consequence, a unipolar pulse can more efficiently affect the system than a bipolar one, while a sequence of pulses realizes a selective action on quantum objects, despite a nonresonant character of the interaction.
Here, I discuss the interaction of two matched ultrashort pulses with a \ensuremath{\Lambda}-like system in which the upper intermediate state is replaced by a manifold of discrete states. Many of these states are simultaneously accessed by the broad bandwidth of the two excitation pulses. The equations of motion for the probability amplitudes of the levels involved in the excitation process are solved analytically in the quasi-impulsive regime. In this regime, the excitation pulses are made shorter than the characteristic time of the excited manifold; population is then transferred to the manifold without Rabi cycling. Under the appropriate conditions, this ``multi-\ensuremath{\Lambda}'' system can exhibit coherence effects such as coherent population trapping and electromagnetically induced transparency of one of the excitation pulses.
Efficient excitation of an ensemble of atoms and molecules to a desired state is of fundamental importance not only for spectroscopy but also for quantum control of molecular dynamics in chemical and biological processes. The latter usually occurs on a much shorter time scale (in the femtosecond range) giving rise to steadily advanced problem how to excite one of the nearby levels, even when they are well within the broad fs pulse spectrum. We propose a new effective method for selective excitation of atoms based on the atomic coherence and discuss a sensitive method to verify experimentally the proposed mechanism using the technique of quantum beating in pump-probe experiments.