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Nonlinear Optics

Quantum dots: Artificial atoms for quantum computing

Duncan G. Steel, E. T. Batteh, Gang Chen, Jun Cheng, Gurudev Dutt, Anthony S. Lenihan, Xiaoqin Li, Todd Stievatorm

Published Jan 1, 2002• 0 citations
Publisher

Abstract

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.

DOI
10.1364/nlo.2002.fa4

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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.
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.
Summary form only given. The optical properties of semiconductor quantum dots have been studied intensively in the past few years. Recently the experiment has demonstrated not only the ability to probe a single QD but also how to coherently control the exciton in a single QD on a time scale that is short compared with the decoherence time. We had proposed a scheme to use the excitons in QD as qubits and to use strong ultra-fast laser pulses to manipulate the qubits via Rabi flopping. As a result a full understanding of the multi-exciton coherent nonlinear spectroscopy with strong pump field is needed. In this work we present a non-perturbative calculation of the nonlinear CW pump-probe spectra.
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.
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.
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.