The work presented in this dissertation contains the first observation of spin-resolved resonance fluorescence from a single quantum dot and its application of direct measurement of electron spin dynamics. The Mollow triplet and the Mollow quintuplet, which are the hallmarks of resonance fluorescence, are presented as the non-spin-resolved and spin-resolved resonance fluorescence spectrum, respectively. The negligible laser background contribution, the near pure radiative broadened spectrum and the anti-bunching photon statistics imply the sideband photons are background-free and near transform-limited single photons. This demonstration is a promising step towards the heralded single photon generation and electron spin readout. Instead of resolving spectrum, an alternative spin-readout scheme by counting resonance fluorescence photons under moderate laser power is demonstrated. The measurements of n-shot time-resolved resonance fluorescence readout are carried out to reveal electron spin dynamics of the measurement induced back action and the spin relaxation. Hyperfine interaction and heavy- light hole mixing are identified as the relevant mechanisms for the back action and phonon-assistant spin-orbit interaction dominates the spin relaxation. After a detailed discussion on charge-spin configurations in coupled quantum dots system, the single-shot readout on electron spin are proposed.
The work presented in this dissertation contains the first observation of spin-resolved resonance fluorescence from a single quantum dot and its application of direct measurement of electron spin dynamics. The Mollow triplet and the Mollow quintuplet, which are the hallmarks of resonance fluorescence, are presented as the non-spin-resolved and spin-resolved resonance fluorescence spectrum, respectively. The negligible laser background contribution, the near pure radiative broadened spectrum and the anti-bunching photon statistics imply the sideband photons are background-free and near transform-limited single photons. This demonstration is a promising step towards the heralded single photon generation and electron spin readout. Instead of resolving spectrum, an alternative spin-readout scheme by counting resonance fluorescence photons under moderate laser power is demonstrated. The measurements of n-shot time-resolved resonance fluorescence readout are carried out to reveal electron spin dynamics of the measurement induced back action and the spin relaxation. Hyperfine interaction and heavy- light hole mixing are identified as the relevant mechanisms for the back action and phonon-assistant spin-orbit interaction dominates the spin relaxation. After a detailed discussion on charge-spin configurations in coupled quantum dots system, the single-shot readout on electron spin are proposed.
A single spin confined to a semiconductor quantum dot is a system of significant interest for quantum information science, as a potential optically-addressable qubit. In many respects, a quantum dot behaves like a single atom with high quality single photon emission. By controlling the light-matter coupling in such a system, it is possible to generate highly non-classical states of light and coherently control a single spin confined to the quantum dot. A departure from the ideal atomic picture appears once we consider the mesoscopic environment with which the quantum dot interacts. Charge fluctuations in the surroundings of the quantum dot affect the photon emission frequency leading to inhomogeneous broadening. Further broadening of the emission is caused by coupling to phonon modes of the host semiconductor material. Finally, coupling between the spin of a confined electron and a large bath of nuclear spins residing in the quantum dot leads to fast dephasing of the electron spin. All of these effects are typically considered detrimental to the potential use of quantum dots for quantum technologies. In this thesis, we develop the environmental coupling of a negatively charged quantum dot as a resource for quantum optics and spin control. First, the phonon-assisted fluorescence is shown to be a useful independent channel for feedback stabilisation of the quantum dot emission frequency, without requiring a measurement of the indistinguishable zero-phonon line. With stabilisation, the corresponding frequency broadening is drastically improved, and the sub-Hz frequency fluctuations are no longer resolved. Next, we show low-power resonance fluorescence emission spectra of the negatively charged trion transition. In the low power regime of resonance fluorescence, the excited state is not populated and most of the emission is coherent. In addition to elastic Rayleigh scattering, we observe coherent Raman sidebands, linked to an effective magnetic field created by the hyperfine interaction, the Overhauser field. This fluctuating effective field lifts the electron spin degeneracy in the absence of a magnetic field, and dictates the optical selection rules of the trion system. These spectra therefore allow for a measurement of the time-averaged distributions of in-plane and out-of-plane Overhauser field components. In the final part of the thesis, we use this hyperfine-generated Λ -scheme to optically create electron spin superpositions through two-colour excitation and coherent population trapping. We then show that rapid shifts in the relative phase of the lasers lead to initialisation of the electron spin into a rotated dark state.
Single spins confined in semiconductor quantum dots - artificial atoms in the solid-state - are attractive candidates for quantum mechanical bits, the fundamental units and building blocks of a quantum computer. The ability to address quantum dot spins optically allows us to initialise and manipulate the state of the quantum bit. Gaining information on the qubit, for example by reading out its state, not only requires state-selective optical excitation, but also access to the single photons scattered in response by the quantum dot. Further, for a distributed computer architecture where nodes of few quantum bits are interlinked via optical communication channels photonic quantum bits are required to faithfully transmit the quantum information. In this thesis we advocate resonant excitation of quantum dot transitions and collection of the resonance fluorescence to address two outstanding challenges: generating dephasing-free single photons for use as flying quantum bits and single-shot spin readout. To this end we investigate the spectral and first-order coherence properties of quantum dot resonance fluorescence. In particular, we directly observe highly coherent scattering in the low Rabi frequency limit which has remained unexplored for solid-state single photon emitters so far. At the same time, interactions with the semiconductor environment are revealed and quantified through their optical signatures: exciton-phonon coupling, nuclear spin dynamics and local electric field fluctuations signal a departure from the ideal atom-like behaviour. Taking advantage of the laser-like coherence of single phase-locked quantum dot photons in the Heitler regime, we demonstrate near-ideal two-photon quantum interference. This benchmark measurement is a precursor for the photonic entanglement of distant quantum dot spins in a quantum optical network, and the results here predict a high fidelity operation. Finally, moving to tunnel-coupled quantum dot molecules we show that the overlap of carrier wave functions in two closely spaced quantum dots forms new spin-selective optical transitions not available in single quantum dots. Then, the presence or absence of scattered photons reveals the electron spin. Intermittency in the quantum dot resonance fluorescence allowed us, for the first time, to observe spin quantum jumps in real-time. Both achievements - highly coherent photons and spin readout - provide the missing link to attempt creation of a small-scale quantum network now.
Semiconductor quantum dots tightly confine excited electron-hole pairs, called excitons, resulting in discrete energy levels similar to those of single atoms. Transition energies in the visible or near-infrared make quantum dots suitable for many applications in quantum optics and quantum information science, but to take advantage of all the properties of quantum dot emission, it is necessary to excite them coherently which has been a great challenge due to background scattering of the excitation laser. This dissertation presents the first coherent control of a single quantum dot with observation of its resonance fluorescence and decoherence phenomena. Strong continuous-wave excitation causes the dot to undergo several Rabi oscillations before emitting. These are visible as oscillations in the first- and second-order correlation functions of the emission, and the quantum dot states are "dressed", resulting in a Mollow triplet in the emission spectrum. Some resonantly excited dots, in addition to resonance fluorescence, also emit light from excited states several meV higher in energy. Such up-conversion fits existing theories of decoherence but has never been directly observed before. The up-conversion intensity is shown to be described well by a fairly simple three-level model with single-phonon absorption. The coherent phenomena of resonance fluorescence and the decoherence due to up-conversion paint a dual picture of single quantum dots wherein they can sometimes be treated as an ideal two-level system, but their interactions with the host crystal can lead to many complex behaviors.
A pair of tunnel-coupled quantum dots has advantages over single dots in tunability and spin coherence, but far less work has been done to measure and understand the quantum optics of this system. In particular, the two-electron singlet-triplet system with one electron in each dot generates an eight-level system in which two-level and four-level double-\ensuremath{\Lambda} systems are coupled only through the hyperfine interaction and other spin relaxation processes. We first measure the emission spectrum under resonant driving with a continuous-wave laser and then perform time-correlated Hanbury Brown-Twiss (HBT) and Hong-Ou-Mandel (HOM) interferometric measurements to examine nonclassical photon properties of spin-flip Raman emission and resonance fluorescence. The shapes of second-order correlation functions $[{g}^{(2)}(\ensuremath{\tau})]$ from HBT are strikingly different between resonance fluorescence and spin-flip Raman emission, reflecting the spin dynamics of the singlet-triplet system. In addition, our two-photon HOM measurements demonstrate a high raw visibility of 0.96, with a coherence time exceeding the radiative lifetime.
The thesis presents the investigations of the emission properties of the Mollow triplet (resonance fluorescence above emitter saturation) and dephasing effects in semiconductor quantum dots. The investigations of the Mollow triplet emission properties focus on the detuning dependent Mollow triplet emission especially the relative areas and width of the individual Mollow peaks. If both fine-structure components of the exciton are excited a Mollow quintuplet is experimentally observed, which is found to be in agreement with a theoretical model. In addition the indistinguishable photon emission from the individual Mollow sidebands is verified. The investigations on dephasing effects focus on the phonon-assisted incoherent excitation of a quantum dot and a comprehensive study of the emission properties under these excitation conditions. A second study focuses on the non-resonant emitter mode coupling of a quantum dot coupeld to two modes of the micro pillar cavity together with the corresponding emission properties.
InAs quantum dots (QDs) can be used as optically coupled quantum storage devices for quantum information applications. The QD can be charged with a single electron, where the spin state (up or down) provides a long lived quantum bit (qubit). The QD's optically excited states are used to initialize, manipulate, and read out the electron spin state with laser pulses. However, most practical quantum information applications require many interacting qubits, forming a quantum network. Since QDs are based on semiconductor technology, and are compatible with standard nano-fabrication processing, there is promise that they can provide a solid state platform where a scalable quantum information architecture is realizable. We focus on scaling the QD system to multiple qubits using intermediate spin-photon entangled states. In this work, experimental and theoretical techniques are developed to study the QD-light matter interaction at the single photon level. Resonance fluorescence from a single QD is experimentally realized, and the single photon nature of the scattered radiation is verified through intensity correlation experiments. Transient fluorescence measurements on resonantly excited QDs are performed using time correlated single photon counting techniques to measure the excited state lifetime. High speed electro-optic modulators are used to time gate narrow bandwidth lasers, so that a QD can be driven under step-wise excitation, allowing for the direct observation of time-dependent optical Rabi oscillations. From these measurements, we are able to extract a decoherence rate which is consistent with the lifetime limit, indicating that pure dephasing is negligible in this system. These techniques are applied to the QD spin system to demonstrate a spin-photon entangled state, by performing correlation measurements on the spin and photon state in two bases. A lower bound on the entanglement fidelity of 0.59(4) is achieved, which exceeds the classical limit of 0.5 by more than two standard deviations. The entanglement fidelity is limited primarily by the finite timing resolution of available single photon detectors. Taking this into account, we achieve 84% of the apparatus limited fidelity. These spin-entangled photons can be used to mediate entanglement between distant QD spins, providing the basis of an optically coupled QD spin network.