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Conference on Lasers and Electro-Optics

Coherent control of two-photon excited fluorescence with ultrabroadband optical pulses

Masahiro Tanaka, Keisuke Isobe, Akira Suda, Fumihiko Kannari, Hiroyuki Kawano, Hideaki Mizuno, Atsushi Miyawaki, Katsumi Midorikawa

Published May 1, 2008• 0 citations
Publisher

Abstract

We present that adaptive control can be applied to achieve the highest contrast ratio at the desired fluorescence intensity from a target fluorophore in the selective excitation with ultrabroadband optical pulses.
DOI
10.1109/cleo.2008.4552288

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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.
The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited-state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markers, these ranging from quantum dots to green fluorescence protein. Expressions are presented for the laser-controlled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively.
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.