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The Journal of Chemical Physics

Coherent control of quantum chaotic diffusion: Diatomic molecules in a pulsed microwave field

Jiangbin Gong, Paul W. Brumer

Published Aug 22, 2001• 28 citations
Publisher

Abstract

Extensive phase control of quantum chaotic diffusion is demonstrated for diatomic molecules periodically kicked with microwave pulses. In particular, both complete suppression of chaotic diffusion as well as its enhancement can be achieved by varying the phase of the initial superposition state. The origin of this control in deviations from random matrix theory is also discussed. The results should motivate experiments that are relevant to both coherent control and to quantum chaos.

DOI
10.1063/1.1389306

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•Jan 1, 2012•1 citation
Extensive phase control of quantum chaotic diffusion is demonstrated for diatomic molecules periodically kicked with microwave pulses. In particular, both complete suppression of chaotic diffusion as well as its enhancement can be achieved by varying the phase of the initial superposition state. The origin of this control in deviations from random matrix theory is also discussed. The results should motivate experiments that are relevant to both coherent control and to quantum chaos.
We consider the quantum dynamics of the kicked rotor model in the regime where the last stable resonance islands in the classical phase space disappear. It is found that phase space regions with lower local diffusion rates are able to preserve quantum population. The low-diffusion regions can be moved through phase space in a quasi-adiabatic way by smoothly varying the parameters of the kicking field. With appropriately chosen time-scales for the variation of the field parameters, wave packets initially localized around the low-diffusion areas remain localized around these regions as the regions are moved. The wave packets can then be carried to desired regions of space despite the predominantly chaotic character of the classical phase space. We also comment on the Gong–Brumer scenario of coherent control of quantum chaotic diffusion [Phys. Rev. Lett. 86 1741 (2001)]. While our phase-space inspired control has a clear semiclassical interpretation, it appears that the Gong–Brumer control has a predominantly quantum origin. Furthermore, it is found that our control over wave packet localization disappears in the deeply chaotic regime, while the Gong–Brumer control over the chaotic diffusion persists in this regime but becomes increasingly unstable with increasing chaoticity.
New experimental results are presented for short-pulse microwave ionization of highly excited hydrogen atoms. A comparison of these results with quantum numerical computations and analytical predictions provides for the first time experimentally grounded evidence of the localization phenomenon that leads to the suppression of the quantum version of the chaotic diffusion in action space occurring in the classical limit. The onset of chaotic motion in externally driven classical systems is a key problem in nonlinear dynamics that is now well understood in its essential aspects. In many physically interesting cases, as the perturbation strength increases beyond some critical value, the system starts absorbing energy in a diffusive way. The question whether “diffusive” excitation processes can take place also in externally driven quantum systems is then a very interesting one for the physics of atoms and molecules in external electromagnetic fields. This is a deep question involving the nature and the validity of the quasiclassical approximation when the underlying classical dynamics is chaotic. The question of “quantum diffusion” was first addressed in a simple model system, the kicked rotator. It was chosen because the features of classical chaos in it were relatively clean and well understood. Besides that, the numerical simulation of its quantum dynamics could be easily accomplished. The major indication of this model was that quantum mechanics suppresses the classical chaotic diffusion in action via a destructive interference effect similar to that responsible for the Anderson localization well known in condensed matter physics.
Control over the quantum dynamics of chaotic kicked rotor systems is demonstrated. Specifically, control over a number of quantum coherent phenomena is achieved by a simple modification of the kicking field. These include the enhancement of the dynamical localization length, the introduction of classical anomalous diffusion assisted control for systems far from the semiclassical regime, and the observation of a variety of strongly nonexponential line shapes for dynamical localization. The results provide excellent examples of controlled quantum dynamics in a system that is classically chaotic and offer opportunities to explore quantum fluctuations and correlations in quantum chaos.
The main goal of this PhD work is an experimental study of coherent excitation of atomic and molecular wavepackets, i.e. superpositions of many quantum eigenstates, by shaped femtosecond pulses. Approaches allowing nearly complete population transfer between quantum eigenstates were well studied in the past within the two level approximation. In this work we focus on adiabatic and non-adiabatic methods of population transfer beyond the two-level approximation. Excitation of multi-level target states is possible due to broad spectrum of an ultrashort pulse which contains frequencies needed for multiple transitions to different states in the final superposition. At the same time, the spectrum of an ultrashort pulse can be modified, or ``shaped'', in order to affect the excitation process and control the amplitudes in the final superposition. Both non-adiabatic and quasi-adiabatic methods were first implemented and studied in electronic wavepackets in alkali atoms. The non-adiabatic approach revealed features linked to the strong-field perturbations of the energy level structure of the quantum system. An adiabatic method was implemented for the first time on a femtosecond time scale, and was thoroughly characterized. The control over complex amplitudes in the target superposition was demonstrated as well as completeness of the population transfer. In the second part of this work, we focused on coherent control of rotational wavepackets in diatomic molecules. Rotational excitation by a periodic train of femtosecond pulses was investigated in the context of ``delta-kicked'' rotor - a paradigm system for studying quantum chaos, and the effect of quantum resonance was demonstrated for the first time in a system of true quantum rotors. Control of uni-directional molecular rotation was proposed and demonstrated with a novel ``chiral pulse train'' - a sequence of femtosecond pulses with polarization rotating from pulse to pulse by a predefined angle. All the developed techniques offer new tools in coherent control of atomic and molecular wavepackets on an ultrashort time scale.