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Optics and Spectroscopy

Coherent control of thermalized luminescence in semiconductor quantum dots

Федоров Анатолий Валентинович, Alexander V. Baranov, Yasuaki Masumoto

Published Oct 1, 2002• 7 citations
Publisher

Abstract

A theoretical study of the time-integrated signal of thermalized luminescence excited by a pair of phase-locked light pulses shows that the idea of coherent control should be efficient for measuring the total dephasing rates of high-energy excitonic transitions. This approach can be used for studying both the homogeneously and inhomogeneously broadened systems, which is highly important in studies of the semiconductor quantum dots. It is found that the method of coherent control makes it possible not only to obtain information about the relaxation constants but also to make conclusions about the statistical properties of frequency distributions of the excitonic transitions responsible for broadening the optical spectra.

DOI
10.1134/1.1517080

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A theoretical study of the time-integrated signal of thermalized luminescence excited by a pair of phase-locked light pulses shows that the idea of coherent control should be efficient for measuring the total dephasing rates of high-energy excitonic transitions. This approach can be used for studying both the homogeneously and inhomogeneously broadened systems, which is highly important in studies of the semiconductor quantum dots. It is found that the method of coherent control makes it possible not only to obtain information about the relaxation constants but also to make conclusions about the statistical properties of frequency distributions of the excitonic transitions responsible for broadening the optical spectra.
A detailed theoretical study of the time-integrated signal of spontaneous quasi-elastic secondary emission excited by a pair of phase-locked pulses has shown that coherent control is a promising method for measuring the total dephasing rate of a resonant optical transition. This method may be used to study both the homogeneously and inhomogeneously broadened systems, which is highly important in studies of semiconductor quantum dots. Analysis of components of the secondary emission in the framework of the developed theory has allowed us to find a physically justified criterion for separating the scattering and luminescence signals. The role of spectral filtering of the measured signal in determination of the phase and energy relaxation parameters is elucidated.
A new optical effect, the coherent control of spontaneous secondary emission with the participation of optical phonons in systems with discrete spectra of electronic transitions, is studied theoretically. Analytical formulas are obtained that describe the time-integrated signals of secondary emission excited resonantly by a pair of phase-locked pulses in the homogeneously and inhomogeneously broadened systems of semiconductor quantum dots. It is shown that coherent control is a promising method for measuring the total dephasing rates of a resonance optical transition. A physically justified criterion for discriminating between scattering and luminescence in the secondary emission is found. The role of spectral filtering of the signal in the measurements of phase and energy relaxation parameters is elucidated.
We report on coherent control of the fundamental exciton state in a single quantum dot by means of two phase-locked picosecond laser pulses. By analyzing the experiments performed in the Rabi regime and comparing them to numerical simulations, we show that we can address the exciton coherence and get an insight into the involved dephasing processes. The total decoherence time T2{T}_{2}T2​ (170 ps) is comparable to the effective exciton lifetime T1{T}_{1}T1​ (200 ps), although not reaching the upper theoretical limit of 2T12{T}_{1}2T1​. We conclude that energy relaxation and pure dephasing processes due to virtual scattering with phonons both contribute on an equal footing to the loss of coherence in this kind of monolayer-step-induced GaAs quantum dots.
We have investigated the manipulation of the phase and amplitude of the state of a three-level exciton system by excitation with pairs of phase-locked optical pulses. We demonstrate coherent control over the phase of quantum beating between the light- and heavy-hole excitons which are the components of the system. The state of the system is monitored by time-resolved detection of the resonant secondary emission coupled out of the system in non-phase-matched directions by virtue of the static disorder. We show that the amplitude of the coherent manipulation must diminish as a function of time delay between the components of the pulse pair in a way which takes into account both the dephasing of the excitons and their unphasing which arises from inhomogeneous broadening.
The focus of the thesis is nonlinear transient optical properties and coherent control of single interface fluctuation quantum dots (QD's). When single exciton and biexciton resonances were driven by strong resonant laser pulses, Rabi oscillations of these transitions were observed in the differential transmission (DT) geometry. These results extend the concept of coherent control to the limit of single quantum confined systems in solids and have important implications for the feasibility of building quantum information processing devices using semiconductor QD's. Exciton Rabi oscillations are equivalent to arbitrary single-bit operations. The pulsed control of the exciton-biexciton transition is utilized as the optical operation for building a two-bit controlled rotational gates (CROT) in a single QD. A fidelity of 0.79 was obtained from numerical evaluation of the gate operation itself assuming typical decay parameters measured from these dots. Next, the nonradiative quantum coherence between two orthogonally polarized excitons confined in a single QD was studied. By using pulses with large enough bandwidth and the proper polarization, two exciton states are simultaneously excited. The quantum beats between the two exciton states were temporally resolved as the relative phase between the two dipole oscillations changed. It was found that the nonradiative coherence time is limited by the lifetimes of the excitons involved even in the strong field regime. In the basis of the pseudo-spin Bloch vectors of exciton transitions, the total wavefunction following the pulsed excitation is an entangled state, i.e. the wavefunction is non-factorizable. Finally, the quantum coherence between the biexciton, exciton, and the crystal ground states was studied in a novel quantum beat experiment, where the oscillations only existed when the pump and probe pulses overlapped in time. Laser pulses generated after a passive pulse shaper with just enough bandwidth to cover both the exciton and biexciton transitions were used in this experiment. The appearance of the beats is indicative of a reasonably long coherence time between the biexciton and other states even in the presence of strong pulsed excitations.