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Register a new userRole of excited states in the dynamics of excitons and their spins in diluted magnetic semiconductors
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We theoretically investigate the impact of excited states on the dynamics of the exciton ground state in diluted magnetic semiconductor quantum wells. Exploiting the giant Zeeman shift in these materials, an external magnetic field is used to bring transitions between the exciton ground state and excited states close to resonance. It turns out that, when treating the exciton dynamics in terms of a quantum kinetic theory beyond the Markov approximation, higher exciton states are populated already well below the critical magnetic field required to bring the exciton ground state in resonance to an excited state. This behavior is explained by exciton-impurity correlations that can bridge energy differences on the order of a few meV and require a quantum kinetic description beyond the independent-particle picture. Of particular interest is the significant spin transfer toward states on the optically dark $2p$ exciton parabola which are protected against radiative decay.
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Phonons are well known to be the main mechanism for the coupling between bright and dark excitons in nonmagnetic semiconductors. Here, we investigate diluted magnetic semiconductors where this process is in direct competition with the scattering at localized magnetic impurities. To this end, a recently developed quantum kinetic description of the exciton spin dynamics in diluted magnetic semiconductor quantum wells is extended by the scattering with longitudinal acoustic phonons. A strong phonon impact is found in the redistribution of exciton momenta on the exciton parabola that becomes especially prominent for high temperatures and exciton distributions further away from the exciton resonance which are optically dark. Despite their impact on the energetic redistribution, acoustic phonons virtually do not affected the exciton spin dynamics as the exciton-impurity interaction always dominates. Furthermore, it turns out that the exciton spin lifetime increases by roughly one order of magnitude for nonequilibrium hot exciton distributions and, in addition, pronounced quantum kinetic signatures in the exciton spin dynamics appearing after resonant optical excitation are drastically reduced.
We explore the impact of a Rashba-type spin-orbit interaction in the conduction band on the spin dynamics of hot excitons in diluted magnetic semiconductor quantum wells. In materials with strong spin-orbit coupling, we identify parameter regimes where spin-orbit effects greatly accelerate the spin decay and even change the dynamics qualitatively in the form of damped oscillations. Furthermore, we show that the application of a small external magnetic field can be used to either mitigate the influence of spin-orbit coupling or entirely remove its effects for fields above a material-dependent threshold.
We present a dynamical model that successfully explains the observed time evolution of the magnetization in diluted magnetic semiconductor quantum wells after weak laser excitation. Based on the pseudo-fermion formalism and a second order many-particle expansion of the exact p-d exchange interaction, our approach goes beyond the usual mean-field approximation. It includes both the sub-picosecond demagnetization dynamics and the slower relaxation processes which restore the initial ferromagnetic order in a nanosecond time scale. In agreement with experimental results, our numerical simulations show that, depending on the value of the initial lattice temperature, a subsequent enhancement of the total magnetization may be observed within a time scale of few hundreds of picoseconds.
The doping of semiconductors with magnetic impurities gives rise not only to a spin-spin interaction between quasi-free carriers and magnetic impurities, but also to a local spin-independent disorder potential for the carriers. Based on a quantum kinetic theory for the carrier and impurity density matrices as well as the magnetic and non-magnetic carrier-impurity correlations, the influence of the non-magnetic scattering potential on the spin dynamics in DMS after optical excitation with circularly polarized light is investigated using the example of Mn-doped CdTe. It is shown that non-Markovian effects, which are predicted in calculations where only the magnetic carrier-impurity interaction is accounted for, can be strongly suppressed in the presence of non-magnetic impurity scattering. This effect can be traced back to a significant redistribution of carriers in $mathbf{k}$-space which is enabled by the build-up of large carrier-impurity correlation energies. A comparison with the Markov limit of the quantum kinetic theory shows that, in the presence of an external magnetic field parallel to the initial carrier polarization, the asymptotic value of the spin polarization at long times is significantly different in the quantum kinetic and the Markovian calculations. This effect can also be attributed to the formation of strong correlations which invalidates the semiclassical Markovian picture and it is stronger when the non-magnetic carrier-impurity interaction is accounted for. In an external magnetic field perpendicular to the initial carrier spin, the correlations are also responsible for a renormalization of the carrier spin precession frequency.
Magnetically doped semiconductors are well known for their giant Zeeman splittings which can reach several meV even in relatively small external magnetic fields. After preparing a nonequilibrium exciton distribution via optical excitation, the spin dynamics in diluted magnetic semiconductor quantum wells is typically governed by spin-flip scattering processes due to the exciton-impurity exchange interaction. Our theoretical calculations show that the giant Zeeman splitting in these materials in combination with the influence of longitudinal acoustic phonons lead to a quantum ratchet-type dynamics, resulting in an almost complete reversal of the carrier spin polarization at very low temperatures. Furthermore, we find that the predictions of a much simpler rate-equation approach qualitatively agree with a more advanced and numerically demanding quantum kinetic description of the spin dynamics for a wide range of temperatures, although quantitative difference are noticeable.
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