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Physical Review Letters

Quantum-Control Spectroscopy with Exact State Selectivity

Yoshiaki Teranishi

Published Aug 1, 2006• 9 citations
Publisher

Abstract

A method of exact state-selective spectroscopy is introduced, based on quantum control through four specific short laser pulses. The exact conditions for the two pairs of ultrafast pulses are set by the feedback control for selective excitation to one specific resonance state while the other state is destructively interfered as the shadow pair, leading to a state-selective spectrum.

DOI
10.1103/physrevlett.97.053001

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A method of exact state-selective spectroscopy is introduced, based on quantum control through four specific short laser pulses. The exact conditions for the two pairs of ultrafast pulses are set by the feedback control for selective excitation to one specific resonance state while the other state is destructively interfered as the shadow pair, leading to a state-selective spectrum.
A demonstration of coherent quantum control for ultrafast precise selection of closely-lying states is reported. A phase-locked pair of femtosecond laser pulses is generated through a pulse shaper to excite the ground-state cesium atom to the Cs(7D3∕2)\mathrm{Cs}(7{D}_{3∕2})Cs(7D3∕2​) and Cs(7D5∕2)\mathrm{Cs}(7{D}_{5∕2})Cs(7D5∕2​) states by two-photon absorption. The excited state population is measured by detecting fluorescence from each spin-orbit state. By controlling the phase-difference of the pulse pair, an ultrafast precise selection is accomplished. The contrast ratio of the maximal to minimal selection ratio exceeds 103{10}^{3}103 with the delay less than 400fs400\phantom{\rule{0.3em}{0ex}}\mathrm{fs}400fs.
Efficient excitation of an ensemble of atoms and molecules to a desired state is of fundamental importance not only for spectroscopy but also for quantum control of molecular dynamics in chemical and biological processes. The latter usually occurs on a much shorter time scale (in the femtosecond range) giving rise to steadily advanced problem how to excite one of the nearby levels, even when they are well within the broad fs pulse spectrum. We propose a new effective method for selective excitation of atoms based on the atomic coherence and discuss a sensitive method to verify experimentally the proposed mechanism using the technique of quantum beating in pump-probe experiments.
Optimal laser control for ultrafast selection of closely lying excited states whose energy separation is smaller than the laser bandwidth is reported on the two-photon transition of atomic cesium; Cs(6S-->7D(J), J=5/2 and 3/2). Selective excitation was carried out by pulse shaping of ultrashort laser pulses which were adaptively modulated in a closed-loop learning system handling eight parameters representing the electric field. Two-color fluorescence from the respective excited states was monitored to measure the selectivity. The fitness used in the learning algorithm was evaluated from the ratio of the fluorescence yields. After fifty generations, a pair of nearly transform-limited pulses were obtained as an optimal pulse shape, proving the effectiveness of the "Ramsey fringes" mechanism. The contrast of the selection ratio was improved by approximately 30% from the simple "Ramsey fringes" experiment.
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.
The most typical way to optically control population of atomic and molecular systems is to illuminate them with radiation, resonant to the relevant transitions. Here we consider a possibility to control populations with the subcycle and even unipolar pulses, containing less than one oscillation of electric field. Despite the spectrum of such pulses covers several levels at once, we show that it is possible to selectively excite the levels of our choice by varying the driving pulse shape, duration or time delay between consecutive pulses. The pulses which are not unipolar, but have a peak of electric field of one polarity much higher (and shorter) than of the opposite one, are also capable for such control.