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Physical Review B

Transient nonlinear optical spectroscopy studies involving biexciton coherence in single quantum dots

Xiaoqin Li, Yanwen Wu, Xiaodong Xu, Duncan G. Steel, D. Gammon

Published Apr 14, 2006• 6 citations
Publisher

Abstract

Transient differential transmission measurements were performed to study coherent dynamics involving the biexciton resonance confined in a single $\mathrm{GaAs}$ quantum dot. When laser pulses with sufficient bandwidth were tuned to cover both the exciton and biexciton transitions, an oscillatory behavior in the probe transmission was observed. These oscillations persist only as long as the pump and probe pulses overlap in time, in contrast to the usual quantum beat phenomena.

DOI
10.1103/physrevb.73.153304

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Physical Review Letters•Sep 11, 2001•696 citations
Transient differential transmission measurements were performed to study coherent dynamics involving the biexciton resonance confined in a single GaAs\mathrm{GaAs}GaAs quantum dot. When laser pulses with sufficient bandwidth were tuned to cover both the exciton and biexciton transitions, an oscillatory behavior in the probe transmission was observed. These oscillations persist only as long as the pump and probe pulses overlap in time, in contrast to the usual quantum beat phenomena.
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.
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.
Summary form only given. We use transient nonlinear optical spectroscopy to demonstrate Rabi oscillations between each of the dipole coupled states, corresponding to qubit rotations. The interface fluctuation GaAs quantum dots are probed with sub-micron spatial resolution. The resonant excitation of the biexciton requires a two-color scheme in a hyper Raman gain configuration. To demonstrate exciton Rabi oscillations, the laser wavelength is fixed at the exciton resonance. Exciton and biexciton Rabi oscillations correspond to qubit rotations of the |00> to |01> or |10> state and the |01> or |10> to |11> state respectively, depending on the polarization of the excitation field.
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.
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.
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.