Two quantum control spectroscopic techniques were applied to study InAs quantum dot (QD) devices, which contain different strain-reducing layers. By adaptively control light matter interaction, a delayed resonant response from the InAs QDs was found to be encoded into the optimal phase profile of ultrafast optical pulse used. We verified the delayed resonant response to originate from excitons coupled to acoustic phonons of InAs QDs with two-dimensional coherent spectroscopy. Our study yields valuable dynamical information that can deepen our understanding of the coherent coupling process of exciton in the quantum-confined systems.
Two quantum control spectroscopic techniques were applied to study InAs quantum dot (QD) devices, which contain different strain-reducing layers. By adaptively control light matter interaction, a delayed resonant response from the InAs QDs was found to be encoded into the optimal phase profile of ultrafast optical pulse used. We verified the delayed resonant response to originate from excitons coupled to acoustic phonons of InAs QDs with two-dimensional coherent spectroscopy. Our study yields valuable dynamical information that can deepen our understanding of the coherent coupling process of exciton in the quantum-confined systems.
Controlling the quantum states of charge (excitons) or spin-polarized carriers in semiconductor quantum dots (QDs) has been the focus of a considerable research effort in recent years due to the strong promise of using this approach to develop solid state quantum computing hardware. The long-term scalability of this type of quantum computing architecture is enhanced by the use of QDs emitting in the telecom band, which would exploit the established photonic infrastructure. This thesis reports the use of all optical infrared experimental techniques to control exciton dynamics in two different QD samples consisting of InAs/GaAs QDs and InAs/InP QDs within a planar microcavity. An infrared quantum control apparatus was developed and used to apply optimized shaping masks to ultrafast pulses from an optical parametric oscillator. Pulse shaping protocols designed to execute a two-qubit controlled-rotation operation on an individual semiconductor QD were demonstrated and characterized. The quantum control apparatus was then implemented in simultaneous single qubit rotations using two uncoupled, distant InAs/GaAs QDs. These optimal control experiments demonstrated high fidelity optical manipulation of exciton states in the two QDs using a single broadband laser pulse, representing a step forward on the path to a scalable QD architecture and showcasing the power of pulse shaping techniques for quantum control on solid state qubits. As an alternative to single QDs, which have very low optical signals, subsets of QDs within an ensemble can be used in quantum computing applications. To investigate the mediation of inhomogeneities in a QD ensemble, pump-probe experiments were performed on InAs/InP QDs within a dielectric Bragg stack microcavity. Two different excitation geometries showed that the angle dependence of the microcavity transmission allowed for the spectral selection of QD subsets with transition energies resonant with the cavity mode. The microcavity mitigated inhomogeneities in the ensemble while providing a basis for addressing QD subsets which could be used as distinguishable quantum bits. This thesis work shows significant advances towards an optical computing architecture using quantum states in semiconductor QDs.
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.
Semiconductor quantum dots have been featured in a number of proposals for quantum computing because of the advantages afforded by confinement on the nanoscale, such as well separated, discrete energy levels and ease of optical manipulation. In addition, they can leverage established semiconductor fabrication techniques and, like the quantum dots used in this work, can be designed to match the telecommunication band, improving the scalability and potential integration of the platform into existing technologies. This thesis work applied optical pulse engineering to manipulate exciton qubits in self-assembled InAs quantum dots. Optimal quantum control theory was used to design pulse shapes that implement high fidelity single-qubit and two-qubit operations, with constraints on the numerical optimization that ensure that the pulses can be accurately implemented using a commercial 4f pulse shaper. In the case of single-qubit operations, the results showed that two uncoupled qubits can be manipulated in parallel using a single phase-shaped laser pulse, provided their optoelectronic properties are sufficiently different. It was demonstrated that targeted differences in inversion and phase between the qubits can be achieved on an ultrafast timescale with high fidelity. In the case of two-qubit operations, the controlled-rotation gate was optimized using amplitude-only and phase-only pulse shaping schemes. The shaped pulses for both schemes were shown to produce higher fidelity operations. The ability to implement robust state inversion on short timescales is particularly useful for technologies such as ultrafast optical switches, single-photon sources, and entangled-photon sources. This work has demonstrated state inversion in a single InAs quantum dot via adiabatic rapid passage using linearly chirped laser pulses. The achieved gate times were an order of magnitude shorter than previous demonstrations. Theoretical predictions of the dependence of the inversion efficiency of the exciton on the sign of the pulse chirp were also verified experimentally, allowing for the identification of phonon-mediated dephasing as the dominant source of decoherence.
We investigate the dephasing mechanism of optically-induced exciton coherence in an ensemble of InAs self-assembled quantum dots (QDs) using a two-pulse photon-echo (PE) technique. The sample was fabricated on an InP (311)B substrate using strain compensation to control the emission wavelength. This technique also enabled us to fabricate a 150-layer stacked QD structure for enhancing the PE signal intensity. We show the measured decay time of PE signal intensity for resonant excitation of ground-state transition is extremely long, which corresponds to ultralong coherence times of excitons in our QDs. We confirmed that non-radiative population relaxation and pure dephasing are considerably smaller than the radiative relaxation at low temperature. Furthermore, we demonstrate the ultrafast coherent control of QD exciton polarization by changing the pulse areas (Rabi oscillations) in the PE experiment. We also propose a new scheme for implementing QD quantum memory by using the PE technique.
While the advanced coherent control of qubits is now routinely carried out in low frequency (GHz) systems like single spins, it is far more challenging to achieve for two-level systems in the optical domain. This is because the latter evolve typically in the THz range, calling for tools of ultrafast, coherent, nonlinear optics. Using four-wave mixing micro-spectroscopy, we here measure the optically driven dynamics of a single exciton quantum state confined in a semiconductor quantum dot. In a combined experimental and theoretical approach, we reveal the intrinsic Rabi oscillation dynamics by monitoring both central exciton quantities, i.e., its occupation and the microscopic coherence, as resolved by the four-wave mixing technique. In the frequency domain this oscillation generates the Autler-Townes splitting of the light-exciton dressed states, directly seen in the four-wave mixing spectra. We further demonstrate that the coupling to acoustic phonons strongly influences the FWM dynamics on the picosecond timescale, because it leads to transitions between the dressed states.
In this presentation, we observed the coherent optical nonlinear interaction of exciton in a single InAs/GaAs self-assembled QD by using coherent control technique at the wavelength 1127 nm, 4.2 K. Due to the large diameter of InAs QDs in the longer wavelength range, dipole moment of confined excitons is predicted to be large so that coherent optical interaction such as Rabi oscillation is expected to be observed. Large dipole moment is one of the most important criteria to realize strong interaction between photons and excitons in QDs.