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Frontiers in Optics

Frequency resolved optical gating of atomic and molecular coherence: from weak to strong field regimes

Stanislav O. Konorov, Xiaoji G. Xu, John W. Hepburn, Valery Milner

Published Jan 1, 2011• 0 citations
Publisher

Abstract

Frequency resolved gating of laser-induced atomic coherence enables complete reconstruction of the quantum evolution of atomic and molecular systems driven by laser fields. The method is applied to characterization and control of laser-matter interactions.
DOI
10.1364/fio.2011.ftup2

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Understanding the effect of strong laser pulses on the evolution of an atomic or molecular wave function is important in the context of coherent control in the strong-field regime, when power broadening and dynamic Stark shifts become comparable with or bigger than the bandwidth of the control field. We experimentally demonstrate the method of complete characterization of a complex-valued amplitude of a quantum state driven by a strong two-photon field. The method is based on coherent scattering of a weak probe pulse from the strong-field-induced atomic coherence, followed by the detection of the time- and frequency-resolved parametric four-wave-mixing signal. We show that the proposed technique corresponds to a cross-correlation frequency-resolved optical gating (XFROG) of the highly perturbed evolution of an atomic quantum state. Utilizing the XFROG retrieval algorithm, we determine both the amplitude and phase of an atomic wave function at any time moment throughout the interaction with the driving field. The direct retrieval of the time-dependent phase of the wave function, rather than the population dynamics only, enables us to observe the strong-field effects with arbitrary time and frequency resolution.
The interaction of strong laser fields with matter causes light-shifts that play an important role in many fields as quantum optics, molecular physics and chemistry. Here the control results from the interference between two excitation quantum paths, corresponding to the absorption and to the emission by the dressed atomic system of one photon from/on the weak field mode respectively. This effect paves the way to many applications and we will describe a new method to slow the light in an atomic medium.
The goal of this work is to study and understand dynamics of atomic systems interacting with strong fields. To this end, a method referred to as strong-field spectroscopy is used, which measures the absorption spectrum of atoms interacting with such fields. In the scope of this work, a technique which allows the simultaneous measurement of absorption spectra of attosecond pulses and their reference signal is developed, which significantly increases the sensitivity to absorption changes. Additionally, a reconstruction method is introduced which retrieves the time-dependent evolution of the dipole response of an atomic system directly from a single absorption spectrum. Strong-field spectroscopy combines these techniques to examine the nonlinear strong-field dynamics in atomic and molecular systems and is applied to study the strongly correlated doubly excited states in helium. Furthermore, a measurement approach is introduced which uses the interaction with a high-intensity laser pulse to impose a time gate on the evolution of the coherent response of a system, which has previously been excited by an ultrashort laser pulse. With this approach the buildup of resonance phenomena in a wide range of physical systems can be studied. As a first application, the time-dependent buildup of a Fano resonance as well as the buildup of a whole Rydberg series are investigated.
Preface.Preliminaries of the Interaction of Light with Matter.Weak-Field Photodissociation.Weak-Field Coherent Control.Optimal Control Theory.Decoherence and Loss of Control.Case Studies in Coherent Control.Coherent Control of Bimolecular Processes.Coherent Control of the Synthesis and Purification of Chiral Molecules.Coherent Control Beyond the Weak-Field Regime: Bound States and Resonances.Photodissociation Beyond the Weak-Field Regime.Coherent Control Beyond the Weak-Field Regime: The Continuum.Strong-Field Coherent Control.Case Studies in Optimal Control.References.Author Index.Subject Index.
Traditionally, the phenomenon of optical coherence has been observed by detecting coherent transients (i.e., optical nutation, FID, photon echoes) propagating along the laser beam following passage through an absorbing medium. Recently, we have demonstrated that detection of the incoherent (spontaneous) emission from selectively prepared states provides the optical coherence of the ensemble. Our observation of the nutation and the photon echo at right angles to the exciting beam gives directly optical T_1, T_2, and the moment of the laser excited transition. This technique is simple and not susceptible to some of the problems inherent in coherent absorption experiments. Details about this laser technique will be presented. We will also discuss the different dynamical information one obtains about excited states in gases, molecular beams and solids.