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EPJ Web of Conferences

Correlated signals of cluster superfluorescence under two-and three-photon excitation of CdSe/CdS nanostructures

Самарцев Виталий Владимирович, Tatiana G. Mitrofanova

Published Jan 1, 2017• 0 citations
Publisher

Abstract

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.

DOI
10.1051/epjconf/201716103011

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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.
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.
Superfluorescence (SF) originates from the spontaneous buildup of macroscopic coherence among initially incoherent emitters. Its formation is highly sensitive to dephasing and collective coupling in the system. Here, we observe room-temperature SF in CdS/CdSe/CdS spherical quantum wells. With increasing excitation fluence, the peak emission intensity shows a nearly quadratic increase, while the emission delay and pulse width decrease. Burnham-Chiao ringing is also observed, revealing the characteristic collective radiation dynamics of SF. Further experiments with stripe excitation show that shortening the excitation length L changes the dominant fast emission from amplified spontaneous emission to SF. More importantly, the threshold for SF under stripe excitation is only about 1/30 of that under spot excitation. This large reduction indicates that the propagating radiation field provided by spatially extended excitation favors the buildup of cooperative coherence. These findings provide direct experimental evidence for understanding ultrafast many-body coherence dynamics and offer a route to actively control collective emission at room temperature.