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Physical Review A

Phase control of nonadiabatic optical transitions

F. A. Hashmi, M. A. Bouchène

Published Feb 18, 2009• 13 citations
Publisher

Abstract

We theoretically study the interaction of two time delayed, phase-locked, and nonresonant pulses with a two-level system in the strong field regime. The population transfer is shown to be extremely sensitive to the phase shift $\ensuremath{\phi}$ between the pulses, with efficient population transfer taking place only for $\ensuremath{\phi}$ close to $\ensuremath{\pi}$. This effect is explained in terms of nonadiabatic jump and rapid adiabatic passage phenomena.

DOI
10.1103/physreva.79.025401

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We theoretically study the interaction of two time delayed, phase-locked, and nonresonant pulses with a two-level system in the strong field regime. The population transfer is shown to be extremely sensitive to the phase shift \ensuremathϕ\ensuremath{\phi}\ensuremathϕ between the pulses, with efficient population transfer taking place only for \ensuremathϕ\ensuremath{\phi}\ensuremathϕ close to \ensuremathπ\ensuremath{\pi}\ensuremathπ. This effect is explained in terms of nonadiabatic jump and rapid adiabatic passage phenomena.
We investigate the problem of population transfer in a two-states system driven by an external electromagnetic field featuring a few cycles, until the extreme limit of two or one cycle. Taking the physical constraint of zero-area total field into account, we determine strategies leading to ultrahigh-fidelity population transfer despite the failure of the rotating wave approximation. We specifically implement adiabatic passage based on adiabatic Floquet theory for a number of cycles as low as 2.5 cycles, finding and making the dynamics follow an adiabatic trajectory connecting the initial and targeted states. Nonadiabatic strategies with shaped or chirped pulses, extending the π-pulse regime to two- or single-cycle pulses, are also derived.
Features of the adiabatic population transfer are studied with the spatial evolution of interacting pulses propagating in an optically dense medium of three-level Λ-atoms taken into account. A self-consistent analytical solution describing the spatial-temporal dynamics of interacting short pulses under the conditions of adiabatic population transfer is constructed in the adiabatic approximation with consideration for the first nonadiabatic correction. Practically complete inversion on a forbidden transition determined by coherent (adiabatic) population transfer is shown to take place over a length of the medium, which may exceed the absorption length of a weak probing pulse in the absence of control radiation on the adjacent transition by several orders of magnitude.
Coherent interactions between light fields and simple quantum systems, such as $\ensuremath{\pi}$-pulses and adiabatic passage through frequency chirps and stimulated Raman interactions, generally use one- or two-photon processes. This limits the use of such interactions to energy scales close to the photon energy of the control field. However, recent calculations have shown that a 3-level system, generic to ionized diatomic molecules, shows such a strong multiphoton coupling that $\ensuremath{\pi}$-pulses are possible on at least 12-photon transitions. In this paper, we show that adiabatic transfer of population is also possible on such high-order multiphoton transitions. Full one-dimensional quantum mechanical two-electron calculations confirm this effect even in a system with many excited states and an ionization continuum.
We study the effect of coupling between molecular vibrational modes attendant the excitation of Raman transitions using ultrafast chirped laser pulses. We model Raman-active vibrational modes by two-level systems (TLSs) with nondegenerate ground states and a predetermined initial relative phase. Chirp of the pump and Stokes pulses is the same in magnitude and opposite in sign for the whole pulse duration. To reveal the nonadiabatic effects induced by the coupling between the vibrational modes, we compare the model of two uncoupled TLSs with the one of two TLSs coupled by the external fields. The first model shows population inversion. Within the second model, the coupling induces nonadiabatic effects leading to a mixed population distribution. By introducing the time delay between the Stokes and pump pulses, nearly complete population transfer is realized in both coupled TLSs.
A chirped laser pulse transfers population from one level to another level accessible by one photon dipole transition. We have used a pair of phase-locked chirped pulses of same frequency instead of a single chirped pulse to achieve phase control over the population transfer and thus creating coherent population distribution in hydrogen molecule. Simultaneous actions of the phase controlled interference and rapid adiabatic passages due to chirped pulses lead to the control in population transfer from the ground X(v = 0, j = 0) level to the C(v = 2, j = 1) level. We have extended this two-level system to a three-level 1 + 1 ladder system for population transfer from the X level to the J(v = 2, j = 2) level via the C intermediate level using two pairs of phase-locked laser chirped pulses and have achieved laudable control over the coherent population distribution.
A strong nonresonant, asymmetric ultrashort pulse drives an atomic transition and causes a complete population inversion because of a sudden nonadiabatic jump. This jump is probed in real time by propagating a weak ultrashort pulse in the system which is resonant on an adjacent transition. The probe at the exit of the medium presents an oscillatory structure with the nonadiabatic jump marked in time by the onset of oscillations. The nonadiabatic jump thus acts as a ``turn-on'' switch for the shaping of the probe.