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Physical review. B, Condensed matter

Electron-phonon dynamics in optically excited quantum dots: Exact solution for multiple ultrashort laser pulses

Alexei Vagov, V. M. Axt, T. Kühn

Published Oct 23, 2002• 152 citations
Publisher

Abstract

A model of semiconductor quantum dots coupled to phonons and laser light, which is relevant in the limit of strong electronic confinement, is investigated. For an arbitrary sequence of excitations by ultrafast pulses, analytical solutions are obtained for all pertinent density-matrix elements. The results are nonperturbative with respect to the coupling to both phonons and laser light. The derivation depends neither on a particular choice of electronic wave functions nor on a particular wave-vector dependence of the phonon interaction or phonon dispersion. All components of the density matrix exhibit oscillatory dependences on the pulse areas of the exciting pulses analogously to the Rabi oscillations known from simple two-level systems. Three typical applications of the general results are worked out: (a) the influence of phonons on four-wave-mixing spectra, (b) the coherent control of electronic dot occupations in the presence of phonons, and (c) the dynamics of phonon correlations including the formation of a stable polaron spatially localized in the dot and the emission of a pulsed phonon wave packet that leaves the dot.

DOI
10.1103/physrevb.66.165312

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•Jan 1, 2008•1 citation
A model of semiconductor quantum dots coupled to phonons and laser light, which is relevant in the limit of strong electronic confinement, is investigated. For an arbitrary sequence of excitations by ultrafast pulses, analytical solutions are obtained for all pertinent density-matrix elements. The results are nonperturbative with respect to the coupling to both phonons and laser light. The derivation depends neither on a particular choice of electronic wave functions nor on a particular wave-vector dependence of the phonon interaction or phonon dispersion. All components of the density matrix exhibit oscillatory dependences on the pulse areas of the exciting pulses analogously to the Rabi oscillations known from simple two-level systems. Three typical applications of the general results are worked out: (a) the influence of phonons on four-wave-mixing spectra, (b) the coherent control of electronic dot occupations in the presence of phonons, and (c) the dynamics of phonon correlations including the formation of a stable polaron spatially localized in the dot and the emission of a pulsed phonon wave packet that leaves the dot.
The dynamics in a GaAs-type quantum dot induced by excitation with Gaussian laser pulses of arbitrary duration are calculated in the density matrix formalism using the correlation expansion. In particular the back-action of nonequilibrium phonons, i.e., the coherent phonon amplitude and the nonequilibrium phonon occupation, on the electronic two-level system are studied. We find that especially for long pulses and low temperatures nonequilibrium phonons play an important role and cannot be neglected.
Electron-phonon interaction is a major source of optical dephasing in semiconductor quantum dots. Within a density matrix theory the electron-phonon interaction is considered up to the second order of a correlation expansion, allowing the calculation of the quantum kinetic dephasing dynamics of optically induced nonlinearities in GaAs quantum dots for arbitrary pulse strengths and shapes. We find Rabi oscillations renormalized and a damping that depends on the input pulse strength, a behavior not known from exponential dephasing mechanisms.
While the advanced coherent control of qubits is now routinely carried out in low frequency (GHz) systems like single spins, it is far more challenging to achieve for two-level systems in the optical domain. This is because the latter evolve typically in the THz range, calling for tools of ultrafast, coherent, nonlinear optics. Using four-wave mixing micro-spectroscopy, we here measure the optically driven dynamics of a single exciton quantum state confined in a semiconductor quantum dot. In a combined experimental and theoretical approach, we reveal the intrinsic Rabi oscillation dynamics by monitoring both central exciton quantities, i.e., its occupation and the microscopic coherence, as resolved by the four-wave mixing technique. In the frequency domain this oscillation generates the Autler-Townes splitting of the light-exciton dressed states, directly seen in the four-wave mixing spectra. We further demonstrate that the coupling to acoustic phonons strongly influences the FWM dynamics on the picosecond timescale, because it leads to transitions between the dressed states.
The effect of phonons on a nonlinear optical response of a quantum dot-cavity system in quantum strong coupling regime can be accounted for by a fully analytical treatment, provided that the exciton-phonon dynamics is much faster than the exciton-cavity dynamics. Modern experiments involving semiconductor quantum dots embedded in optical microcavities typically meet this criterion. We find that, for a relatively small exciton-cavity coupling, the effect of phonons is concentrated mainly in the polaron shift of the exciton frequency and reduction of exciton-cavity coupling by the Huang-Rhys factor. We have generalized this result to an arbitrary optical nonlinearity and demonstrated a good agreement with the exact solution in a wide range of temperatures. This generalization provides access to higher rungs of the Jaynes-Cummings ladder, where exact numerical approaches are impractical or even impossible. At larger coupling strengths and low temperatures, our approximation is also in good agreement with the exact solution, which makes it a very useful tool for addressing the phonon contribution to the coherent dynamics of a nonlinear optical system. We demonstrate our results for third-order optical polarization with varying observation time and delay time between excitation pulses in the form of two-dimensional spectra. These spectra provide useful information about the coherent coupling between the exciton and the cavity modes. The presented analytical approach is also compared with another useful approximation, having the form of a matrix product, which is a special case of the asymptotically exact solution in the limit of a short phonon memory time.
The interaction of a light field with a quantum-mechanical system can be studied in an optically controlled semiconductor quantum dot. When driven by a continuous light field switched on instantaneously, the quantum dot occupation performs Rabi oscillations. Unlike an atomic system, the quantum dot is coupled to phonons, which leads to a damping of the Rabi oscillations. Here we model the time-resolved probe spectra to monitor these dynamics and study the influence of phonons on the spectra. The spectra consist of up to three peaks, similar to the Mollow triplet known from quantum optics. We develop analytical equations within a rate equation model and show that they agree excellently with a numerical solution using a well established correlation expansion approach.
This work is focused on the optical dynamics of mesoscopic semiconductor heterostructures, using as prototypes zero-dimensional quantum dots and quantum cascade lasers which consist of quasitwo-dimensional quantum wells. Within a density matrix theory, a microscopic many-particle theory is applied to study scattering effects in these structures: the coupling to external as well as local fields, electron-phonon coupling, coupling to impurities, and Coulomb coupling. For both systems, the investigated effects are compared to experimentally observed results obtained during the past years. In quantum dots, the three-dimensional spatial confinement leads to the necessity to consider a quantum kinetic description of the dynamics, resulting in non-Markovian electron-phonon effects. This can be seen in the spectral phonon sidebands due to interaction with acoustic phonons as well as a damping of nonlinear Rabi oscillations which shows a nonmonotonous intensity and pulse duration dependence. An analysis of the inclusion of the self-interaction of the quantum dot shows that no dynamical local field terms appear for the simple two-level model. Considering local fields which have their origin in many quantum dots, consequences for a two-level quantum dot such as a zero-phonon line broadening and an increasing signal in photon echo experiments are found. For the use of quantum dots in an optical spin control scheme, it is found that the dephasing due to the electron-phonon interaction can be dominant in certain regimes. Furthermore, soliton and breather solutions are studied analytically in nonlinear quantum dot ensembles. Generalizing to quasi-two-dimensional structures, the intersubband dynamics of quantum cascade laser structures is investigated. A dynamical theory is considered in which the temporal evolution of the subband populations and the current density as well as the influence of scattering effects is studied. In the nonlinear regime, the scattering dependence and the importance of coherence for Rabi oscillations is investigated. The optically induced charge dynamics is discussed with respect to coherent effects. Calculations of the electronic density and pump-probe signals within a microscopic theory of dephasing show coherent transport effects such as gain oscillations, in agreement with recent experimental results.