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Frontiers in Optics

Generation of maximal coherence in a two-level system via breaking adiabaticity

Yuri V. Rostovtsev, Hichem Eleuch, Anatoly A. Svidzinsky, Marlan O. Scully

Published Jan 1, 2008• 0 citations
Publisher

Abstract

We study population transfer and the generation of quantum coherence in a two- level system interacting with a strong off-resonance ultra-short laser pulse. We derive analytical solutions for an an untra-short pulse of arbitrary shape.
DOI
10.1364/fio.2008.fmk5

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The interactions of sub-cycle and single-cycle pulses with two- or three-level quantum systems are studied, respectively. For the two-level quantum system, two cases in which the carrier frequency of pulses is in resonance and far from resonance with the atom are analysed. The ultrafast complete population transfer can be obtained. The sub-cycle pulse with a far off-resonant carrier frequency is found to be more suitable for the population transfer. The relation between the area of pulses and population transfer is clarified in the sub-cycle and single-cycle domain. For the Lambda-type three-level quantum system, more than 90% of population transfer can be achieved from one level to another. The scheme is insensitive to the variation of the laser parameters such as the peak Rabi frequency and the carrier frequency for both two- and three-level quantum systems.
Two approaches of achieving population transfer and coherence are investigated for the three-level Λ system in the adiabatic limit. The effects of the laser pulse sequence on the population transfer efficiency and coherence are studied. Coherent control of quantum state and population is studied by numerical simulation based on self-consistent set of density matrix equations. It can be seen that the counterintuitive pulse sequence is more efficient in population transfer and coherence than the intuitive one.
The dynamics of populations of the vibrational states in a NO molecule (one-photon absorption) and of the electronic states in a 4,4'-bis(dimethylamino) stilbene molecule (two-photon absorption) is studied versus the frequency, intensity and shape of the laser pulse. We show that specially designed infrared laser pulses can build selective populations of certain vibrational states. A detuning of light frequency from the vibrational resonance qualitatively changes the dynamics of populations. It is found out that the populations of the nonresonant levels follow the pulse shape adiabatically if the detuning significantly exceeds the inverse characteristic time of the change of the pulse. Depopulation of the nonresonant vibrational states leads to a high population of the resonant state at the end of the pulse. Complete breakdown of the standard rotating wave approximation for a two-photon absorption process is observed even for a rather small intensity of the laser pulse. An analytical solution for the interaction of a pulse with a three-level system beyond the rotating wave approximation is obtained, and it is in close agreement with the strict numerical solution of the amplitude equations. Special attention is paid to the population dynamics of randomly oriented molecules. The orientational disorder as well as the vibrations limit the coherent population transfer. Calculations show the strong role of the anisotropy of photoexcitation in the coherent control of populations which can affect the anisotropy of photobleaching.
An analytic theory of the adiabatic passage (AP) regime of interaction of short frequency chirped laser pulses with a two-level quantum system (QS) being initially in the superpositional quantum state is presented. We show that the initial value of the non-diagonal elements of the density matrix can influence the dynamics of the population transfer during the action of the laser pulse, but do not influence essentially the final populations of the states of the QS obtained at the end of the interaction near the AP regime. A novel solution to the Bloch equations is obtained in the form of a converging power series generalizing the ordinary AP solution.