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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Time Resolved Four-Wave Mixing in Nanocomposites

Olga M. Fedotova, Oleg Kh Khasanov, Никифоров Виктор Геннадьевич, Самарцев Виталий Владимирович

Published Jun 1, 2019• 0 citations

Abstract

We elaborate methods of femtosecond time resolved spectroscopy of nanocomposites. Features of photon echo (PE) and time resolved four-wave mixing (TRFWM) signals in nanocomposites consisted of semiconductor quantum dots (QD) incorporated into nonlinear dielectric matrix are studied. In particular, impacts of value and angular distribution of permanent dipole moments (PDM) as well as their spatial dispersion on two pulse responses are under investigation. As is known, large values of permanent dipole moments are inherent to many semiconductor QDs, including ZnO QDs. Moreover, the presence of giant dipole moment in cellulose nanocrystals what reaches 4400+400 Debye has been demonstrated [1]. To the best of our knowledge, the PDM impact on the signals of time resolved four-wave mixing as a whole, and, in particular, photon echo has been yet unrevealed.

DOI: 10.1109/cleoe-eqec.2019.8871483

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Abstract Methods of characterization of nanocomposites consisting of semiconductor quantum dots incorporated into a transparent nonlinear dielectric matrix are elaborated. Spectral composition, observation time, and phase-matching conditions for echo-responses excited by two noncollinear pulses are analysed. More specifically, spectral and spatial features of echo signals caused by permanent dipole moments (PDMs) inherent to quantum dots and local field effects in them, as well as by the angular distribution function of the PDM orientations and spatial dispersion of transition dipole moments, are considered.

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Recently, quantum information processing and communications using photons have been attracting attention. To increase the density of transmitted photonic qubits, it is necessary to develop broadband quantum memories and detectors that can handle ultrashort pulses. Although rare-earth-ion doped quantum memories [1] have been widely studied, due to their storage bandwidth of ~GHz, they are incapable of storing ultrashort pulses. In our group, we used the photon echo (PE) method with quantum dots (QDs) to realize ultra-short femtosecond pulse storage. However, we encountered many difficulties in realizing this method such as low PE efficiency from the QDs and the insufficient temporal resolution of the avalanche single-photon detectors. To solve these problems, we have applied a new quantum control method and utilized an up-conversion single-photon detector (UCSPD) [2]. In this presentation, we will introduce the techniques “1. Time-resolving measurement by UCSPD,” “2. PE quantum memory using QDs” and “3. enhancement of PE signals.”

A systematic theoretical and computational investigation of the microscopic factors which determine the phase of the signal field in time-resolved quasidegenerate three-pulse scattering experiments is presented. The third-order phase-matched response is obtained by density-matrix perturbation theory using a Green-function formalism for a system composed of two well-separated sets of closely spaced energy levels. Equations for calculating the electric field of four-wave-mixing signals generated by path-length delayed pulses are given. It is found that the phase of the signal field is determined by the excitation pulse phases, the dynamics of the nonlinear polarization decay, the product of four transition dipole matrix elements, and by a pulse-delay-dependent phase modulation at the frequency of the first dipole oscillation in the four-wave-mixing process. Analytic results for a two-level Bloch model show the phase shift from rapid nonlinear polarization decay. The product of dipole matrix elements is real and positive for three-level processes (bleached ground-state absorption and excited-state emission), but can be real and negative for some four-level Raman processes. The pulse-delay-dependent phase modulation treated here is closely related to the interferometric pulse-delay-dependent amplitude modulation observed in some collinear experiments, and plays a role in producing photon echos in inhomogeneously broadened samples. Numerical calculations of phase-resolved electric fields for finite duration pulses using a Brownian oscillator model appropriate for condensed-phase dynamics are presented. The ability of pulse-delay-dependent phase modulation to encode the frequency of the initially excited dipole onto the phase of the signal field can be exploited to examine energy-level connectivity, reveal correlations hidden under the inhomogeneous lineshape, and probe relaxation pathways in multilevel systems.