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Ultrafast Phenomena and Nanophotonics

Controlling the emission time of photon echoes by optical freezing of exciton dephasing and rephasing in quantum-dot ensembles

Matthias Reichelt, Hendrik Rose, Alexander N. Kosarev, S. V. Poltavtsev, M. Bayer, Ilya A. Akimov, Christian Schneider, Martin Kamp, Sven Höfling, T. Meier

Published Mar 3, 2021• 0 citations
Publisher

Abstract

Following the ultrafast optical excitation of an inhomogeneously broadened ensemble, the macroscopic optical polarization decays rapidly due to dephasing. This destructive interference is, however, reversible in photon echo experiments. Here, we propose a concept in which a control pulse slows down either the dephasing or the rephasing of the exciton ensemble during its presence. We analyze and visualize this optical freezing process by showing and discussing results for different single and multiple sequences of control pulses using a simple model of inhomogeneously broadened two-level systems. This idea has been realized in experiments performed on self-assembled (In,Ga)As quantum dots where it was possible to retard or advance the photon echo emission time by several picoseconds. The measurements are in very good agreement with numerical simulations for a more realistic model which, in particular, takes the spatial shape of the laser pulses into account.

DOI
10.1117/12.2576887

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Following the ultrafast optical excitation of an inhomogeneously broadened ensemble, the macroscopic optical polarization decays rapidly due to dephasing. This destructive interference is, however, reversible in photon echo experiments. Here, we propose a concept in which a control pulse slows down either the dephasing or the rephasing of the exciton ensemble during its presence. We analyze and visualize this optical freezing process by showing and discussing results for different single and multiple sequences of control pulses using a simple model of inhomogeneously broadened two-level systems. This idea has been realized in experiments performed on self-assembled (In,Ga)As quantum dots where it was possible to retard or advance the photon echo emission time by several picoseconds. The measurements are in very good agreement with numerical simulations for a more realistic model which, in particular, takes the spatial shape of the laser pulses into account.
Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a novel concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2pi area. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
Abstract Semiconductor quantum dots are excellent candidates for ultrafast coherent manipulation of qubits by laser pulses on picosecond timescales or even faster. In inhomogeneous ensembles a macroscopic optical polarization decays rapidly due to dephasing, which, however, is reversible in photon echoes carrying complete information about the coherent ensemble dynamics. Control of the echo emission time is mandatory for applications. Here, we propose a concept to reach this goal. In a two-pulse photon echo sequence, we apply an additional resonant control pulse with multiple of 2πarea. Depending on its arrival time, the control slows down dephasing or rephasing of the exciton ensemble during its action. We demonstrate for self-assembled (In,Ga)As quantum dots that the photon echo emission time can be retarded or advanced by up to 5 ps relative to its nominal appearance time without control. This versatile protocol may be used to obtain significantly longer temporal shifts for suitably tailored control pulses.
Interaction of light with atomic-like solid-state systems, such as semiconductor quantum dots (QDs) with discrete energy levels, is key for the implementation of high-speed quantum gates and information processing in semiconductor-based devices. Of particular interest are degenerate multiwave-mixing processes under resonant conditions that establish strong light–matter interactions beyond the limits of perturbative nonlinear optics. Here, we exploit a multitude of picosecond optical pulses to manipulate the unitary evolution of excitons in (In,Ga)As QDs and address the role of resonance detuning in an inhomogeneously broadened ensemble. In particular, we use the two-pulse photon echo sequence to uncover the coherent dynamics of charged excitons, whereas the areas of two additional control pulses serve as tuning knobs for adjusting the magnitude and timing of the coherent emission in a wide range up to several hundred of picoseconds. Furthermore, we make use of the spin degeneracy of the ground and excited states of charged QDs to control the polarization state of the emitted light. We reveal that control pulses, whose durations are comparable to the dephasing time of the ensemble, lead to a temporal sorting of optical multiwave-mixing processes, which is in accordance with the developed theoretical model. Lifting the temporal degeneracy allows us to smoothly trace the transition from the perturbative to the regime of Rabi rotations and opens up new possibilities for the optical investigation of complex energy-level structures in so far unexplored material systems.
We investigate the dephasing mechanism of optically-induced exciton coherence in an ensemble of InAs self-assembled quantum dots (QDs) using a two-pulse photon-echo (PE) technique. The sample was fabricated on an InP (311)B substrate using strain compensation to control the emission wavelength. This technique also enabled us to fabricate a 150-layer stacked QD structure for enhancing the PE signal intensity. We show the measured decay time of PE signal intensity for resonant excitation of ground-state transition is extremely long, which corresponds to ultralong coherence times of excitons in our QDs. We confirmed that non-radiative population relaxation and pure dephasing are considerably smaller than the radiative relaxation at low temperature. Furthermore, we demonstrate the ultrafast coherent control of QD exciton polarization by changing the pulse areas (Rabi oscillations) in the PE experiment. We also propose a new scheme for implementing QD quantum memory by using the PE technique.
An ensemble of quantum dot excitons may be used for coherent information manipulation. Due to the ensemble inhomogeneity any optical information retrieval occurs in the form of a photon echo. We show that the inhomogeneity can lead to a significant deviation from the conventional echo timing sequence. Variation of the area of the initial rotation pulse, which generates excitons in a dot subensemble only, reveals this complex picture of photon echo formation. We observe a retarded echo for $\ensuremath{\pi}/2$ pulses, while for $3\ensuremath{\pi}/2$ the echo is advanced in time as evidenced through monitoring the Rabi oscillations in the time-resolved photon echo amplitude from (In,Ga)As/GaAs self-assembled quantum dot structures and confirmed by detailed calculations.
Quantum coherence control of two-pulse photon echoes has been demonstrated for a rephasing halt, resulting in storage-time extension using atom phase-controlled optical deshelving (optical locking) in a backward propagation scheme for the additional benefit of echo intensity enhancement. Compared with conventional forward two-pulse photon echoes, the backward two-pulse photon echo efficiency is enhanced by 15-fold even in a dilute sample, and the storage time is lengthened by spin dephasing time accelerated by spin inhomogeneous broadening. The mechanism of delayed photon echoes via optical locking is due to the temporal hold of the rephasing process by coherent population transfer to a robust spin state.