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arXiv:2312.03156 · Physical review. B./Physical review. B

Optical coherence storage in dark exciton states using spin-dependent three-pulse photon echo

I. A. Solovev, Roman S. Nazarov, A. A. Butiugina, Sergei A. Eliseev, V. A. Lovtcius, Yu. P. Efimov, Yury V. Kapitonov, I. A. Yugova

Published Jan 16, 2025• 0 citations
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Abstract

Extension of coherence time is a desired goal in the field of all-optical information processing implemented in both classical and quantum ways. Here we show how the decay time of a coherent signal from localized excitons can be significantly increased utilizing the spin degree of freedom. To experimentally demonstrate this effect, we studied three-pulse photon echoes from excitons in a single InGaAs/GaAs quantum well subject to a transverse magnetic field. Field-induced quantum beats lead to oscillation of the exciton population between short-lived bright and long-lived dark states during the coherence storage period between the second and third excitation pulses. In the aperiodic regime, the echo signal decay time tends to the dark exciton lifetime, which leads to an increase in the photon echo decay time by an order of magnitude.

DOI
10.1103/physrevb.111.045423

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Extension of coherence time is a desired goal in the field of all-optical information processing implemented in both classical and quantum ways. Here we show how the decay time of a coherent signal from localized excitons can be significantly increased utilizing the spin degree of freedom. To experimentally demonstrate this effect, we studied three-pulse photon echoes from excitons in a single InGaAs/GaAs quantum well subject to a transverse magnetic field. Field-induced quantum beats lead to oscillation of the exciton population between short-lived bright and long-lived dark states during the coherence storage period between the second and third excitation pulses. In the aperiodic regime, the echo signal decay time tends to the dark exciton lifetime, which leads to an increase in the photon echo decay time by an order of magnitude.
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The ability to extend the time scale of the coherent optical response from large ensembles of quantum emitters is highly appealing for applications in quantum information devices. In semiconductor nanostructures, spin degrees of freedom can be used as auxiliary, powerful tools to modify the coherent optical dynamics. Here, we apply this approach to negatively charged (In,Ga)As/GaAs self-assembled quantum dots which are considered as excellent quantum emitters with robust optical coherence and high bandwidth. We study 3-pulse spin-dependent photon echoes subject to moderate transverse magnetic fields up to 1 T. We demonstrate that the timescale of coherent optical response can be extended by at least an order of magnitude by the field. Without magnetic field, the photon echo decays with T2T_ 2T2​ = 0.45 ns which is determined by the radiative lifetime of trions T1T_1T1​ = 0.27 ns. In the presence of the transverse magnetic field, the decay of the photon echo signal is given by spin dephasing time of the ensemble of resident electrons T2,eT_{2,e}T2,e​ ~ 4 ns. We demonstrate that the non-zero transverse g-factor of the heavy holes in the trion state plays a crucial role in the temporal evolution and magnetic field dependence of the long-lived photon echo signal.
Larmor precession of the quasiparticle spin about a transverse magnetic field leads to the oscillations in the spontaneous photon echo signal due to the shuffling of the optical coherence between optically accessible (bright) and inaccessible (dark) states. Here we report on a new nonoscillating photon echo regime observed in the presence of nonequal dephasing rates of bright and dark states. This regime enables the observation of the long-lived dark optical coherence. As a simple mechanical analogy, we suggest a charged particle moving in the magnetic field through the medium with anisotropic viscous friction. We demonstrate the dark coherence retrieval in the spontaneous photon echo from excitons in the InGaAs/GaAs quantum well.
We have studied experimentally spin-dependent photon echoes from excitons in an InGaAs/GaAs quantum well subject to a transverse magnetic field (Voigt geometry). Larmor precession of the spins of the electron and heavy hole in an exciton leads to a periodic transfer of coherence between bright and dark exciton states. The increase in dephasing time due to the transition to the dark states could be useful for coherent control development. A comprehensive analysis shows a good agreement between a four-wave mixing experiment and the predictions of a theoretical treatment based on a five-level exciton model comprising a ground state and two pairs of bright and dark states. The extracted optical dephasing time of bright and dark excitons is equal to 30 and 130 ps, respectively. Exploiting the photon echo reveals evidence of electron Larmor precession with in-plane ggg factor $|{g}_{e,\ensuremath{\perp}}|=0.44\ifmmode\pm\else\textpm\fi{}0.05$ and heavy hole precession as well. The precession frequency of the latter depends nonlinearly on the applied magnetic field, and the corresponding ggg factor reaches a value of $|{g}_{h,\ensuremath{\perp}}|\ensuremath{\approx}0.3$ at B=6B=6B=6 T. Estimates for the heavy hole ggg-factor spreading as well as the isotropic exchange interaction constant are provided.
We use spontaneous (two-pulse) and stimulated (three-pulse) photon echoes for studying the coherent evolution of optically excited ensemble of trions which are localized in semiconductor CdTe/CdMgTe quantum well. Application of transverse magnetic field leads to the Larmor precession of the resident electron spins, which shuffles optically induced polarization between optically accessible and inaccessible states. This results in several spectacular phenomena. First, magnetic field induces oscillations of spontaneous photon echo amplitude. Second, in three-pulse excitation scheme, the photon echo decay is extended by several orders of magnitude. In this study, short-lived optical excitation which is created by the first pulse is coherently transferred into a long-lived electron spin state using the second optical pulse. This coherent spin state of electron ensemble persists much longer than any optical excitation in the system, preserving information on initial optical field, which can be retrieved as a photon echo by means of third optical pulse.
Optical coherence time and nonlinear optical response of excitons localized to quantum dots in a GaAs/AlGaAs single quantum well are investigated by the three-pulse photon echo technique. At low temperature, the optical coherence time is estimated to be 1.8 ns from the decay curve of the photon echo signal. The decay profile for short time delay shows the strong dependence on the input pulse area of the third pulse. Rabi oscillations are also observed. The oscillations exhibit nonlinear behavior, which is affected by the pre-excited polarization. Such behavior can be qualitatively explained by the local field effect due to the exciton-exciton interaction between the excitons.