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Physical Review Letters

Nonlinear Nano-Optics: Probing One Exciton at a Time

N. H. Bonadeo, Gang Chen, Dan Gammon, Douglas Scott Katzer, D. Park, Duncan G. Steel

Published Sep 28, 1998• 184 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.81.2759

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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.
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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.
We present a series of coherent nonlinear optical experiments that show semiconductor quantum dots have optical properties very similar to simple atomic systems but are surprisingly robust against decoherence and have large dipole moments. By combining advances in nano-optical probing methodologies with the power of coherent nonlinear optical spectroscopy techniques, the measurements have enabled us to extend concepts of coherent optical control and wave function engineering to a single quantum dot exciton.
Transient nonlinear optical spectroscopy, performed on excitons confined to single GaAs quantum dots, shows oscillations that are analogous to Rabi oscillations in two-level atomic systems. This demonstration corresponds to a one-qubit rotation in a single quantum dot which is important for proposals using quantum dot excitons for quantum computing. The dipole moment inferred from the data is consistent with that directly obtained from linear absorption studies. The measurement extends the artificial atom model of quantum dot excitonic transitions into the strong-field limit, and makes possible full coherent optical control of the quantum state of single excitons using optical pi pulses.