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Physical Review B

Theory of ultrafast nonlinear optics of Coulomb-coupled semiconductor quantum dots: Rabi oscillations and pump-probe spectra

J. Danckwerts, Kwang Jun Ahn, Jens Förstner, A. Knorr

Published Apr 18, 2006• 65 citations
Publisher

Abstract

We investigate the optical properties of a Coulomb-coupled double-quantum dot system excited by coherent light pulses. Basic effects of Coulomb coupling regarding linear and nonlinear optical processes are discussed. By numerically solving the Heisenberg equation of motion we are able to present the temporal evolution of the system's density matrix for a wide range of coupling parameters. The two main coupling effects in dipole approximation, biexcitonic shift and F\"orster energy transfer, are investigated and their qualitative and quantitative influence on absorption spectra, Rabi oscillations, and single- and two-pulse excitation is discussed. We present simulated differential transmission spectra to allow for comparison with recent experimental studies.

DOI
10.1103/physrevb.73.165318

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We investigate the optical properties of a Coulomb-coupled double-quantum dot system excited by coherent light pulses. Basic effects of Coulomb coupling regarding linear and nonlinear optical processes are discussed. By numerically solving the Heisenberg equation of motion we are able to present the temporal evolution of the system's density matrix for a wide range of coupling parameters. The two main coupling effects in dipole approximation, biexcitonic shift and F"orster energy transfer, are investigated and their qualitative and quantitative influence on absorption spectra, Rabi oscillations, and single- and two-pulse excitation is discussed. We present simulated differential transmission spectra to allow for comparison with recent experimental studies.
We provide a theoretical study for the dynamical behavior of two-photon Rabi oscillations in two coupled quantum dots. Each dot is a three-level quantum system (ground, one-exciton, and biexciton states). We describe the optical dynamics within the density matrix formalism framework. The two-photon Rabi oscillations are found to be significantly affected by the strength of the interdot dipolar interaction. Using a detuned laser pulse with an exciton state of the driven quantum dot in our numerical simulations, a direct coherent excitation between the biexciton states can be established, but whether Rabi oscillations can be observed depend mainly on the strength of the dipolar interaction and bandwidth of the excitation laser. When the strength of the dipolar coupling is less than the excitation laser bandwidth, the time-dependent populations of the various two biexciton states of the system exhibit coherent oscillations with several frequencies. However, as we increase the dipolar coupling strength, the population transfer between the quantum dots levels amazingly becomes forbidden, and the excitation gets trapped at the initial state. The reduction of the influence of the dipolar interaction leads to a manipulation of two-photon Rabi oscillation in an ultrashort timescale (∼ps), opening possibilities to achieve ultrafast quantum state control and quantum logic gate generation.
The focus of the thesis is nonlinear transient optical properties and coherent control of single interface fluctuation quantum dots (QD's). When single exciton and biexciton resonances were driven by strong resonant laser pulses, Rabi oscillations of these transitions were observed in the differential transmission (DT) geometry. These results extend the concept of coherent control to the limit of single quantum confined systems in solids and have important implications for the feasibility of building quantum information processing devices using semiconductor QD's. Exciton Rabi oscillations are equivalent to arbitrary single-bit operations. The pulsed control of the exciton-biexciton transition is utilized as the optical operation for building a two-bit controlled rotational gates (CROT) in a single QD. A fidelity of 0.79 was obtained from numerical evaluation of the gate operation itself assuming typical decay parameters measured from these dots. Next, the nonradiative quantum coherence between two orthogonally polarized excitons confined in a single QD was studied. By using pulses with large enough bandwidth and the proper polarization, two exciton states are simultaneously excited. The quantum beats between the two exciton states were temporally resolved as the relative phase between the two dipole oscillations changed. It was found that the nonradiative coherence time is limited by the lifetimes of the excitons involved even in the strong field regime. In the basis of the pseudo-spin Bloch vectors of exciton transitions, the total wavefunction following the pulsed excitation is an entangled state, i.e. the wavefunction is non-factorizable. Finally, the quantum coherence between the biexciton, exciton, and the crystal ground states was studied in a novel quantum beat experiment, where the oscillations only existed when the pump and probe pulses overlapped in time. Laser pulses generated after a passive pulse shaper with just enough bandwidth to cover both the exciton and biexciton transitions were used in this experiment. The appearance of the beats is indicative of a reasonably long coherence time between the biexciton and other states even in the presence of strong pulsed excitations.
We theoretically investigate the influence of dynamic Coulomb interaction on optical bistability and Rabi oscillations in a driven two-level semiconductor quantum dot system under laser irradiation. Using density matrix equations derived from the Coulomb-interaction model proposed by Lu et al. [Phys. Rev. A 103, 043504 (2021)], we obtain analytical solutions for population inversion under the rotating wave approximation. Our analysis shows that the Coulomb interaction induces optical bistability, governed by a cubic equation. The thresholds and the shapes of the hysteresis loops are tunable and can be controlled by various parameters, including electron density, confinement potential, detuning, and dephasing. Additionally, our numerical simulations demonstrate the potential for achieving high-efficiency population inversion and predicting bifurcation and anharmonic regimes in Rabi oscillations under monochromatic excitation.
Quantum dots have been the focus of both fundamental and applied research due to their atomic-like properties. The delta-function-like density of states along with strong nonlinear optical properties have made quantum dots the focus of novel opto-electronic devices and of quantum computing proposals. The key issue for implementing quantum dots in devices such as quantum computers is the ability to coherently entangle separately localized quantum dot states. Using continuous wave coherent nonlinear optical spectroscopy techniques, this thesis focuses on creating coherent super-position states built from separately localized quantum dot states. The narrow bandwidths and mutual coherence of the applied laser fields allow for the creation of radiative and nonradiative coherences which can be understood from the coherent nonlinear optical response. The quantum dots under study are formed due to the width fluctuations of a thin quantum well. By applying nondegenerate mutually coherent fields on the sample in the traditional pump and probe geometry and homodyne detecting the nonlinear signal field, nonradiative coherences between two laterally coupled quantum dots are created and the coupling between their states examined. The coherent nonlinear optical response is compared with theoretical predictions based on the density matrix formalism for the interacting two exciton model. From this comparison, binding energies of the two-exciton bound state created with separately localized excitons is found to be on the order of 20 mueV for like-polarized excitons and on the order of 100 mueV for unlike-polarized excitons. A second order coherence between the ground and two-exciton state is also noted in the experimental data after comparison with theory. Further work attempting to study a vertically coupled quantum dot system was unsuccessful. The spectrum of a quantum dot is further understood from the comparison of the linear and nonlinear excited state spectra. Excited states which appear in both spectra imply a Coulomb interaction between them and their respective ground states. Coherent nonlinear optical signatures of excited states correlated with their linear excitation spectra are presented, and the importance of such states for a quantum computer read-out is described.
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.
In this thesis, the coherent interaction of single semiconductor quantum dots and ultrafast optical pulses is studied. Under certain conditions, localized exciton transitions in quantum dots can be seen as semi-isolated two-level systems. While this description is sufficient for the explanation of some observations in coherent experiments, it is sometimes necessary to explicitly consider coupling of the discreet quantum states confined to the dot with the environment. We start out from simple, classical examples of coherent spectroscopy and then turn towards experiments where the interaction with the vicinity of the dot becomes an important factor. First, a novel method for transient differential reflectivity spectroscopy of single quantum systems is introduced. It is a pure far-field optical technique which does not require any sophisticated sample preparation steps which makes it applicable to a broad range of structures. Pump pulses excite the sample structure and probe pulses read out the pump-induced changes in the system after a variable delay time. In the case of a single dipole, the signal is given in the form of the spectral inteferogram between the backscattered wave from the particle and the probe light which is reflected at the sample surface. This form of homodyne detection amplifies the weak scattered wave from the particle and thus makes this kind of spectroscopy for single quantum dots feasible. In the remainder of this thesis our spectroscopic method is applied to either characterize the coherent properties of single quantum dots, to prepare and read-out a desired quantum state or to deliberately manipulate them. Coherence times and oscillator strengths are determined for localized exciton transitions. Arbitrary population states can be written by driving coherent population oscillations using resonant pulses, while entangled superpositions of two exciton states in a single dot are investigated by quantum beats on transient differential spectra. We finally exploit the interaction between the dot and a nearby absorbing layer to switch the dot's absorption spectrum on ultrafast timescales via light-induced transient electric fields.