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arXiv:1702.05057 · Physical review. B./Physical review. B

Time-resolved photon echoes from donor-bound excitons in ZnO epitaxial layers

S. V. Poltavtsev, Alexander N. Kosarev, Ilya A. Akimov, Dmitri R. Yakovlev, Sergey Sadofev, Joachim Puls, S. P. Hoffmann, Maximilian Albert, Cedrik Meier, T. Meier, M. Bayer

Published Jul 21, 2017• 10 citations
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Abstract

The coherent optical response from 140 nm and 65 nm thick ZnO epitaxial layers is studied using four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (${\mathrm{D}}^{0}{\mathrm{X}}_{\text{A}}$) at temperature of 1.8 K we evaluate optical coherence times ${T}_{2}=33--50$ ps corresponding to homogeneous line widths of $13--19\phantom{\rule{0.222222em}{0ex}}\ensuremath{\mu}\mathrm{eV}$, about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is determined mainly by the population decay with time ${T}_{1}=30--40$ ps, while pure dephasing is negligible. Temperature increase leads to a significant shortening of ${T}_{2}$ due to interaction with acoustic phonons. In contrast, the loss of coherence of the donor-bound B exciton (${\mathrm{D}}^{0}{\mathrm{X}}_{\text{B}}$) is significantly faster (${T}_{2}=3.6\phantom{\rule{0.16em}{0ex}}\mathrm{ps}$) and governed by pure dephasing processes.

DOI
10.1103/physrevb.96.035203

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•Jan 1, 1990•0 citations
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We present subpicosecond time-resolved four-wave-mixing studies on GaAs/AlAs short-period superlattices having different miniband widths. Photon echoes are observed as a consequence of the inhomogeneous broadening of the excitonic resonance. In addition, the photon-echo signal exhibits periodic modulations as a function of the time delay between the excitation laser pulses. Free excitons and excitons bound to neutral acceptors are identified as the underlying three-level system leading to the observed photon-echo quantum beats. From the beat period we can directly infer the dissociation energy of the bound exciton. In accordance with theory, we find that the dissociation energy decreases with increasing miniband width, i.e., when the excitons become less confined. In addition, we find that the dephasing rate of bound excitons is about one order of magnitude less than that of free excitons and is mainly determined by energy relaxation.
We study Rabi oscillations detected in the coherent optical response from various exciton complexes in a 20-nm-thick CdTe/(Cd,Mg)Te quantum well using time-resolved photon echoes. In order to evaluate the role of exciton localization and inhomogeneous broadening we use selective excitation with spectrally narrow ps pulses. We demonstrate that the transient profile of the photon echo from the localized trion (${\mathrm{X}}^{\ensuremath{-}}$) and the donor-bound exciton (D0X{\mathrm{D}}^{0}\mathrm{X}D0X) transitions strongly depends on the strength of the first pulse. It acquires a non-Gaussian shape and experiences significant advancement for pulse areas larger than $\ensuremath{\pi}$ due to non-negligible inhomogeneity-induced dephasing of the oscillators during the optical excitation. Next, we observe that an increase of the area of either the first (excitation) or the second (rephasing) pulse leads to a significant damping of the photon echo signal, which is strongest for the neutral excitons and less pronounced for the donor-bound exciton complex (D0X{\mathrm{D}}^{0}\mathrm{X}D0X). The measurements are analyzed using a theoretical model based on the optical Bloch equations which accounts for the inhomogeneity of optical transitions in order to reproduce the complex shape of the photon echo transients. In addition, the spreading of Rabi frequencies within the ensemble due to the spatial variation of the intensity of the focused Gaussian beams and excitation-induced dephasing are incorporated in our model, which is able to explain the fading and damping of Rabi oscillations. By analyzing the results of the simulation for ${\mathrm{X}}^{\ensuremath{-}}$ and D0X{\mathrm{D}}^{0}\mathrm{X}D0X complexes we are able to establish a correlation between the degree of localization and the transition dipole moments determined as $\ensuremath{\mu}({\mathrm{X}}^{\ensuremath{-}}$)=73 D and $\ensuremath{\mu}({\mathrm{D}}^{0}\mathrm{X}$)=58 D.
This work presents new results of experimental studies of exciton relaxation in GaAs/AlGaAs multiple quantum well materials, using transient nonlinear laser spectroscopy techniques. In the low excitation regime, effective optical Bloch equations similar to the density matrix formalism of a two-level system describe the response. Solutions of these equations appropriate for three-pulse scattering studies are presented, along with a discussion of new experimental techniques used in this work. Non-ideal conditions present in the molecular beam epitaxy growth process introduce monolayer fluctuations in the quantum well thickness, leading to inhomogeneous broadening and exciton localization at sites of minimum energy. Localized excitons are separated in energy from extended, quasi-delocalized states by the mobility edge. Studies of localized exciton relaxation indicate that these excitons relax on a much slower timescale than delocalized excitons. The temperature dependence of the localized exciton relaxation rate shows that above 15K, the excitons are thermally activated to extended states above the mobility edge. Below 15K the excitons relax by phonon assisted migration between localization sites. For temperatures above 5K, and for exciton energies greater than 1 meV below line center, an extra dephasing mechanism characterizes the exciton relaxation. The inhomogeneous broadening of the exciton leads to the emission of stimulated photon echoes in the experimental geometry used in this work. The time-resolved emission demonstrates the stimulated photon echo nature at low excitation densities. At higher excitation densities, the decay dynamics is more complex. The time-resolved emission shows the presence of a stimulated photon echo and a free polarization decay. This unusual result suggests that both a homogeneous and an inhomogeneous exciton distribution comprise the exciton resonance. Exciton relaxation at low excitation densities represents the interaction of the exciton with the lattice. At higher excitation densities, exciton-exciton and exciton-free carrier interactions modify the relaxation rates. The dependence of the exciton relaxation rate on excitation density shows that many-body effects play an important role in the exciton physics. Free carrier interactions are more efficient at increasing the exciton relaxation rate; both types of interactions are more important in quantum well systems than in bulk materials.