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Bulletin of the Russian Academy of Sciences Physics

Entangled femtosecond free induction signals in a cadmium sulfide crystal at room temperature

A. V. Leontiev, Vladimir S. Lobkov, Tatiana G. Mitrofanova, В. В. Самарцев, A. G. Shmelyov

Published Dec 1, 2012• 0 citations
Publisher

Abstract

Entangled free induction decay (EFID) femtosecond signals are experimentally observed for the first time at a wavelength of 790 nm in a cadmium sulfide (CdS) crystal in the two-photon absorption (TPA) regime upon excitation by two crossed (angle, 60°) laser beams. The sample emitted two EFID signals simultaneously in opposite directions. The signals were diffracted by nonequilibrium electric polarization gratings induced by two laser beams in accordance with the laws of energy and momentum conservation. The possibility of exciting EFID signals in the three-photon absorption regime is discussed.

DOI
10.3103/s1062873812120210

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Entangled free induction decay (EFID) femtosecond signals are experimentally observed for the first time at a wavelength of 790 nm in a cadmium sulfide (CdS) crystal in the two-photon absorption (TPA) regime upon excitation by two crossed (angle, 60°) laser beams. The sample emitted two EFID signals simultaneously in opposite directions. The signals were diffracted by nonequilibrium electric polarization gratings induced by two laser beams in accordance with the laws of energy and momentum conservation. The possibility of exciting EFID signals in the three-photon absorption regime is discussed.
A new method of two-photon excitation of femtosecond signals of ``entangled'' free induction decay (EFID) by two crossed 790-nm laser beams in a CdS crystal at room temperature has been realized for the first time. This ``entangled'' (through the wave vectors) coherent response appears only in the case when the photons involved to the process of two-photon excitation of the sample belong to the different laser beams. This technique allows one to separate the EFID signal from the exciting femtosecond pulses and to vary the response wavelength by varying the angle between their wave vectors. The most optimal case occurs when the angle between the wave vectors of exciting pulses as well as the angle between each of these wave vectors and that of the response is equal to 60°.
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.
Time-resolved and integrated degenerated four-wave mixing experiments with two-photon excitation at a wavelength of 600–710 nm on a 30–40 μm thick cadmium sulfide crystal are presented for a temperature range from 5 to 300 K. A photon echo is observed showing quantum beats both at positive and negative delay times τ with a period of 0.7–0.8 ps. The signal decays exponentially with time constants of ≈170 fs at τ>0 and half as large at τ<0, independent of temperature. The results are discussed in terms of the decay of a high-density gas of e–h pairs, excitons and excitonic molecules highly out of equilibrium.
The possibility and conditions for generation of the correlated signals of cluster superfluorescence (CSF) under two and three-quantum excitation of nanostructured samples CdSe/CdS by two crossed at the angle of 60° femtosecond beams of the Ti:Sapphire laser radiation are investigated. It is shown that intensity of the CSF signals is proportional to the cube of the number of clusters and that these collective signals are generated in mutually opposite directions k1 – k2 and k2 – k1, where k1, k2 are the wavevectors of the exciting pulses.