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physica status solidi (b)

Single Quantum Dot Nonlinear Optical Spectroscopy

N. H. Bonadeo, Gang Chen, D. Gammon, Duncan G. Steel

Published Sep 1, 2000• 23 citations
Publisher

Abstract

We report a study of the coherent nonlinear optical response of individual excitons localized in GaAs quantum dots. Our data show that the nonlinear response is comprised of an incoherent contribution dominated by saturation of the oscillator strength and a coherent contribution giving rise to population pulsations. The results compare well with present theory and show the similarities with atoms and quantum dots in their coherent optical interaction with light. The measured energy relaxation and dephasing rates are comparable, reflecting the absence of significant pure dephasing at low temperatures. In addition, we use nonlinear spectroscopy to investigate quantum dot coupling showing the presence of an incoherent coupling leading to fast energy relaxation. The polarization properties as well as the fine structure splitting are also discussed.

DOI
10.1002/1521-3951(200009)221:1<5::aid-pssb5>3.0.co;2-h

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We report a study of the coherent nonlinear optical response of individual excitons localized in GaAs quantum dots. Our data show that the nonlinear response is comprised of an incoherent contribution dominated by saturation of the oscillator strength and a coherent contribution giving rise to population pulsations. The results compare well with present theory and show the similarities with atoms and quantum dots in their coherent optical interaction with light. The measured energy relaxation and dephasing rates are comparable, reflecting the absence of significant pure dephasing at low temperatures. In addition, we use nonlinear spectroscopy to investigate quantum dot coupling showing the presence of an incoherent coupling leading to fast energy relaxation. The polarization properties as well as the fine structure splitting are also discussed.
Coherent nonlinear optical spectroscopy of individual excitons in GaAs quantum dots is demonstrated and shows strong similarities with atoms in their coherent optical interaction, unlike higher dimensional heterostructures. The nonlinear response is dominated by an incoherent contribution (saturation) and a coherent contribution (population pulsations) of the single dot and compares well with present theory. The data shows that energy relaxation and dephasing rates are comparable, reflecting the absence of significant pure dephasing, and also demonstrate the presence of interdot energy transfer.
The nonlinear response of single GaAs quantum dots is studied in femtosecond near-field pump-probe experiments. At negative time delays, transient reflectivity spectra show pronounced oscillatory structure around the quantum dot exciton line, providing the first evidence for a perturbed free induction decay of the excitonic polarization. Phase-disturbing Coulomb interactions between the excitonic polarization and continuum excitations dominate the optical nonlinearity on ultrafast time scales. A theoretical analysis based on the semiconductor Bloch equations accounts for this behavior.
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.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
Nonlinear optical response and optical coherence of excitons in semiconductor dense quantum dots in GaAs single quantum wells has been studied by using photon echo techniques. At low temperatures, the optical coherence is estimated to be 2 ns from the decay curve in the photon echo signal. Rabi oscillations are also observed. Unlike the results for a single quantum dot in the literature to date, the oscillation shows nonlinear behavior affected strongly by the pre-excited carrier density. The results can be explained by the theory of the local field correction originating from exciton-exciton interaction between the inter dots.
A detailed understanding of the population and coherence dynamics in optically driven individual emitters in solids and their signatures in ultrafast nonlinear-optical signals is of prime importance for their applications in future quantum and optical technologies. In a combined experimental and theoretical study on exciton complexes in single semiconductor quantum dots we reveal a detailed picture of the dynamics employing three-beam polarization-resolved four-wave mixing (FWM) micro-spectroscopy. The oscillatory dynamics of the FWM signals in the exciton-biexciton system is governed by the fine-structure splitting and the biexciton binding energy in an excellent quantitative agreement between measurement and analytical description. The analysis of the excitation conditions exhibits a dependence of the dynamics on the specific choice of polarization configuration, pulse areas and temporal ordering of driving fields. The interplay between the transitions in the four-level exciton system leads to rich evolution of coherence and population. Using two-dimensional FWM spectroscopy we elucidate the exciton-biexciton coupling and identify neutral and charged exciton complexes in a single quantum dot. Our investigations thus clearly reveal that FWM spectroscopy is a powerful tool to characterize spectral and dynamical properties of single quantum structures.