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Physical Review Letters

Switched Wave Packets: A Route to Nonperturbative Quantum Control

Jonathan G. Underwood, Michael Spanner, Misha Ivanov, Jeff Mottershead, Benjamin Sussman, Albert Stolow

Published Jun 4, 2003• 150 citations
Publisher

Abstract

The dynamic Stark effect due to a strong nonresonant but nonionizing laser field provides a route to quantum control via the creation of novel superposition states. We consider the creation of a field-free "switched" wave packet through adiabatic turn-on and sudden turn-off of a strong dynamic Stark interaction. There are two limiting cases for such wave packets. The first is a Raman-type coupling, illustrated by the creation of field-free molecular axis alignment. An experimental demonstration is given. The second case is that of dipole-type coupling, illustrated by the creation of charge localization in an array of quantum wells.

DOI
10.1103/physrevlett.90.223001

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arXiv:physics/9905019•Canadian Journal of Physics•Jan 1, 1999•6 citations
The dynamic Stark effect due to a strong nonresonant but nonionizing laser field provides a route to quantum control via the creation of novel superposition states. We consider the creation of a field-free "switched" wave packet through adiabatic turn-on and sudden turn-off of a strong dynamic Stark interaction. There are two limiting cases for such wave packets. The first is a Raman-type coupling, illustrated by the creation of field-free molecular axis alignment. An experimental demonstration is given. The second case is that of dipole-type coupling, illustrated by the creation of charge localization in an array of quantum wells.
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We discuss an approach to quantum control based on initial adiabatic tuning of the field-free Hamiltonian by a strong laser field to optimize the system for the desired transitions induced by the control laser pulse. As an illustration, we describe single-qubit, two-qubit, and some qudit logical gates within rotational and vibrational states of a diatomic molecule. Gate operations use resonant Raman transitions, and the prior adjustment of the Hamiltonian is done by a strong nonresonant aligning field.
Based on the idea of reverse engineering, we design an optimal laser pulse to control strong-field multiphoton atomic transitions. Starting from the time-dependent Schr\"odinger equation of the full system, we adiabatically eliminate the nonessential states and apply the rotating-wave approximation to arrive at an effective two-state representation that involves dynamic Stark shifts and multiphoton coupling. Solving this equation inversely for the field, we obtain an analytical laser pulse shape that is expected to induce the full system's evolution according to user-defined quantum pathways. In our procedure, the amplitude and phase of the laser pulse are engineered such that the dynamically shifted electronic states are resonantly coupled during the action of the pulse at each moment of time. As a result, the driven system evolves from an arbitrary initial population distribution to any desired final quantum state superposition at a predefined rate. The proposed scheme is demonstrated using the example of the $3s\ensuremath{\rightarrow}4s$ two-photon transition of atomic sodium. By solving the time-dependent Schr\"odinger equation of the single-active electron with two different methods, either propagating time-dependent coefficients of many field-free states or directly propagating the three-dimensional electronic wave packet on a grid, we demonstrate the robustness as well as the limitations of the presented reverse engineering scheme.
A method to optically control a dark transition, for instance, the coupling between different spin states, is proposed. The control is achieved by manipulating the direction, amplitude, and duration of dynamic Stark shifts. Laser-driven spin switches can be prepared by conveniently generalizing different optical techniques, such as $\ensuremath{\pi}$-pulse schemes and adiabatic passage schemes. The efficiency and robustness of the schemes is analyzed for both two-level and multilevel systems, implying quantum state selective wave packet transfer between states of different multiplicity.
The application of nonresonant lasers to quantum systems can modify energy levels in a general way. This approach, using the nonresonant dynamic Stark effect, is an effective mechanism for modifying chemical dynamics. These molecular techniques have analogous implementations in quantum technologies. Applications include controlling vacuum fluctuations to create molecular alignment and broadband light sources, photonic catalysis, quantum memories in atomic vapours, and photonics in bulk diamond phonons. The links between these different applications are investigated.
In this paper, a coherent superposition of angular-momentum states created by absorption of polarized light by molecules is analyzed. Attention is paid to the time evolution of wave packets representing the spatial orientation of the internuclear axis of a diatomic molecule. Two examples are considered in detail. Molecules absorbing light in a permanent magnetic field experiencing the Zeeman effect and molecules absorbing light in a permanent electric field experiencing the quadratic Stark effect. In a magnetic field, we have a wave packet that evolves in time exactly as a classical dipole oscillator in a permanent magnetic field (classical-physics picture of the Zeeman effect). In the second case, we have a wave packet that goes through periodical changes of shape of the packet with revivals of the initial shape. This is pure quantum behavior. The classical motion of angular momentum in an electric field in the case of a quadratic Stark effect is known to be a periodic. Solutions obtained for wave packet evolution are briefly compared with Rydberg-state coherent wave packets and harmonic-oscillator wave packets. Zeeman and Stark effects in small molecules continuously attract the attention of researchers, theoreticians, as well as experimentalists. These investigations allow us to obtain a deeper understanding of the interaction of molecules with stationary external fields and also can be used as a practical tool to measure different molecular characteristics, such as permanent electric or magnetic dipole moments, intramolecular perturbations, etc. It is worthwhile analyzing these effects as an evolution of wave packets. All this motivates a comparison of the quantum and classical picture of Zeeman and Stark effects in molecules.PACS No.: 33.55.Be