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Optics Letters

Optical selectivity in optically dense media driven by optimized Gaussian-type ultrashort pulse pairs

Han Xu, Heping Zeng

Published May 15, 2005• 0 citations
Publisher

Abstract

We theoretically demonstrate that selective resonant excitation can be achieved in a dense collection of V-type three-level atoms by optimizing the pulse delay and peak intensity ratio of an applied phase-tailored ultrashort pulse pair. Near-dipole-dipole interaction plays an important role in the quantum control of selective excitations since it brings about an intrinsic frequency shift in the atomic resonance, which builds up various excitation pathways. As a consequence, we can control the quantum interference between various pathways by shaping the excitation pulse pair to steer the atomic excitation selectively toward a desired quantum state.

DOI
10.1364/ol.30.001198

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We theoretically demonstrate that selective resonant excitation can be achieved in a dense collection of V-type three-level atoms by optimizing the pulse delay and peak intensity ratio of an applied phase-tailored ultrashort pulse pair. Near-dipole-dipole interaction plays an important role in the quantum control of selective excitations since it brings about an intrinsic frequency shift in the atomic resonance, which builds up various excitation pathways. As a consequence, we can control the quantum interference between various pathways by shaping the excitation pulse pair to steer the atomic excitation selectively toward a desired quantum state.
Selective resonant excitations can be realized with a shaped ultrashort pulse in an optically dense collection of multilevel individual atoms, where the near dipole-dipole interactions induce intrinsic frequency shifts of the atomic resonance. A proper transform-limited pulse and modulation of excitation pulses can be controlled to establish constructive or destructive quantum interference between different excitation pathways towards a desired selective resonant excitation, even driven by pulses with broadband spectral components.
Selective multiphoton excitations can be achieved by tailoring the driving pulses to manipulate the outcome of the light-matter interaction. While single-photon transitions of single atoms driven by ultrashort pulses, dependent mainly on the resonant frequency component, and thus possesses no optical selectivity no matter how the excitation pulse shapes [1]. Interestingly, when an ultrashort pulse interacts with an optically dense medium, quantum controllable optical selectivity can be achieved in a single-photon process.
V-type three-level systems, where two excited states share a common ground state, serve as fundamental models for exploring coherent light-matter interactions in a range of quantum systems, from atomic gases to semiconductor nanostructures. In this work, we investigate the coherent evolution of such a system under strong femtosecond-pulse excitation by numerically solving the optical Bloch equations. Our analysis shows that the coherent evolution of a three-level system critically depends on the product of the excitation-pulse duration and energy separation between the excited states. Building on this understanding, we extend our analysis to simulate two-dimensional coherent spectra in a high-intensity regime. We demonstrate a control over the coherent pathway contributions to the nonlinear optical response of a V-type system by varying the intensity of the excitation pulses. This control is manifested through the ability to selectively turn individual spectral features on or off in the 2D spectra, each corresponding to distinct quantum pathways. Furthermore, the pulse intensities are varied to precisely adjust the phase of these peaks. Our approach provides a simple and robust framework for achieving control of coherent response of multilevel systems.
Strong-field quantum-state control is investigated, taking advantage of the full---amplitude and phase---characterization of the interaction between matter and intense ultrashort pulses via transient-absorption spectroscopy. As an example, we apply the method to a nondegenerate VVV-type three-level system modeling atomic Rb, and use a sequence of intense delayed pulses, whose parameters are tailored to steer the system into a desired quantum state. We show how to experimentally enable this optimization by retrieving all quantum features of the light-matter interaction from observable spectra. This provides a full characterization of the action of strong fields on the atomic system, including the dependence upon possibly unknown pulse properties and atomic structures. Precision and robustness of the scheme are tested, in the presence of surrounding atomic levels influencing the system's dynamics.
We describe optimized coherent control methods for two-photon transitions in atoms of a ladder-type three-state energy configuration. Our approach is based on the spatial coherent control scheme, which uses counterpropagating ultrashort laser pulses to produce complex excitation patterns in an extended space. Because coherent control requires constructive interference of constituent transition pathways, applying it to an atomic transition with a specific energy configuration requires specially designed laser pulses. We show in an experimental demonstration that two-photon transition with an intermediate resonant energy state can be coherently controlled and retrieved from the resonance-induced background, when phase flipping of the laser spectrum near the resonant intermediate transition is used. A simple reason for this behavior is the fact that the transition amplitude function (added to give an overall two-photon transition) changes its sign at the intermediate resonant frequency and, thus, by proper spectral-phase programing, the excitation patterns (or the position-dependent interference of the transition given as a consequence of the spatial coherent control) can be well isolated in space along the focal region of the counterpropagating pulses.