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Laser Physics

Correlated stimulated photon echo signals under three-photon femtosecond excitation of CdSe–CdS colloidal quantum dots

В. В. Самарцев, Tatiana G. Mitrofanova

Published Oct 28, 2016• 7 citations
Publisher

Abstract

Abstract The possibility and conditions of the correlated signals of stimulated photon echo (SPE) generation under three-photon femtosecond excitation of a sample, which is an ensemble of N semiconductor nanoparticles, are investigated. Each of these nonoparticles consists of a CdSe core covered by a CdS shell. The phase matching conditions for correlated SPE signal formation in such a sample are obtained.

DOI
10.1088/1054-660x/26/12/125203

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Abstract The possibility and conditions of the correlated signals of stimulated photon echo (SPE) generation under three-photon femtosecond excitation of a sample, which is an ensemble of N semiconductor nanoparticles, are investigated. Each of these nonoparticles consists of a CdSe core covered by a CdS shell. The phase matching conditions for correlated SPE signal formation in such a sample are obtained.
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The possibility and the conditions of the formation of correlated “gratings” of electrons and their spins in a semiconductor film containing CdSe/CdS nanoparticles (which are the quantum dots) have been studied. Notably, the induction of electron spin “gratings” on quantum dots has been considered for the first time. We have suggested to perform an excitation of the film in the two photon absorption mode using two crossed (at an angle of 60?) femtosecond laser beams. As a result of the excitation, two nonequilibrium “gratings” are induced simultaneously in the excitation area of the film. If the exciting pulses have the same polarizations, then induced “gratings” of electrons are formed. However, in the case when the exciting pulses have mutually orthogonal polarizations, the formation of induced “gratings” of electron spins takes place. The same exciting pulses excite the electrons of CdSe/CdS nanoparticles into a superposition state. Then the free induction decay signal is generated. This signal being diffracted by induced “gratings” plays the role of a probe pulse in the suggested experimental scheme. The diffracted signals propagating in two mutually opposite directions are correlated (i.e., they are identical). Their wavefronts can carry the correlated transient holograms. Other possible applications of correlated “gratings” (in spintronics and in coherent femtosecond laser spectroscopy) are also discussed.
Abstract Nonlinear optical properties of colloidal quantum dots are studied to elucidate the significance and nature of many‐body effects. Two‐pulse photon echo studies of nanocrystalline CdSe quantum dots are reported for samples dispersed in a poly(butylmethacrylate) film (4.4 K). Oscillations are observed in the experimental data that are attributed to 1S3/21Se–2S3/21Se biexciton cohererences. Signals are simulated using a phenomenological model based on the many‐body description of the dynamics (the average polarization model). It is found that the electronic coherences and the nonlinear response originating from biexciton source terms are important, but their manifestation in the photon echo signals is strongly influenced by the interplay between homogeneous and inhomogeneous line broadening. (© 2004 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)