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.
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.
Spins localized in semiconductor nanostructures have been intensively investigated for quantum spintronics. These include the spin of single electron localized by quantum dots or impurities, and spins of the lattice nuclei. These localized spins can be exploited as carriers of quantum information, while in some circumstances they also play the role of deleterious noise sources for other quantum objects through their couplings. Quantum control of the spins in semiconductor nanostructures is therefore of central interest for quantum applications. In this thesis, we address several problems related to the quantum control of electron or hole spin and nuclear spins in semiconductor quantum dots and impurity centers. The first problem studied is the control of nuclear spin bath for a hole spin qubit in III-V semiconductor quantum dot. In quantum dots formed on III-V compounds, the direct band gap of the host material allows ultrafast optical addressability of a single electron or hole spin qubit. However, nonzero nuclear spins of group III and group V elements result in a large statistical fluctuation in the Zeeman splitting of the spin qubit which then dephases in nanosecond time scale. We present a novel feedback scheme to suppress the statistical fluctuation of the nuclear spin field for enhancing the coherence time of the hole spin qubit. We also find positive feedback control which can amplify the magnitude of the nuclear field, so that a bimodal distribution can develop, realizing a quantum environment that can not be described by a single temperature. The second problem addressed here is the control of donor spin qubits in silicon architecture which have ultra-long quantum coherence time. We developed the quantum control scheme to realize the quantum metrology of magnetic field gradient, based on the celebrated Kane’s architecture for quantum computation. The scheme can also be generalized to calibrate the locations of the donors. In the third part of the thesis, we investigate a novel type of quantum dot formed in a new class of two-dimensional semiconductors, monolayer transition metal dichalcogenides (TMDs), which exhibit interesting spin and pseudospin physics. This novel quantum dot system may offer new opportunity for quantum spintronics in the ultimate 2D limit, and we investigate here the valley pseudospin as a possible quantum bit carrier. A main finding is that, contrary to the intuition, the lateral confinement by the quantum dot potential does not lead to noticeable valley hybridization, and therefore the valley pseudospin in monolayer TMDs QD can well inherit the valley physics such as the valley optical selection rules from the 2D bulk which implies a variety of quantum control possibilities.
In this work, we study the resonant nonlinear optical response obtained when optical fields are used to excite charged semiconductor quantum dots (QDs). The basic physics of charged excitons (trions) created by optical excitation of charged QDs is of interest from the point of view of optically driven spin based quantum computing (QC). Stimulated Raman excitation, resonantly enhanced by the optical dipole coupling to the trion state, was used to optically generate electron spin coherence in the ground state of charged QDs. The evolution of the spin coherence was monitored through quantum beats in the phase-sensitively detected four wave mixing signal. The decay of the beats is a measure of the spin coherence time, which was found to be at least an order of magnitude greater than either the trion dipole coherence, or the Raman coherence time between excitons in a single neutral QD. A fascinating outcome of the experiment was the first observation of a contribution to the spin coherence induced by the vacuum field, which is also responsible for spontaneous emission from the trion state, known as spontaneously generated coherence (SGC). QC demands that coherent optical manipulations should be performed within the spin coherence time. We performed coherent optical control experiments, with a pair of phase-locked pump pulses, that showed the quantum nature of the coherence through interference of different quantum mechanical pathways. We showed both in experiment and theory that we can manipulate the spin coherence on the time scale of the Larmor frequency, as well as on an ultrafast femtosecond time scale, corresponding to the optical frequency of the trion state. Finally, resonant optical excitation of both the bright and nominally forbidden transitions from a single electron spin in a QD to the trion state were demonstrated. This allows for direct optical access to all the transitions required for optically driven QC with QD electron spins. We used frequency-domain nonlinear spectroscopy measurements on single QD trions to obtain the trion dipole decoherence and decay rates. Further, we demonstrated that the single electron spin coherence could be generated and detected optically, and found that the spin coherence time was significantly greater than in ensemble measurements at the same magnetic field.
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.
Self-assembled quantum dots can act as an interface between single spins and photons. They combine the flexibility and scalability of semiconductor systems with near-perfect two level systems, emitting highly coherent single photons. In potential quantum information processing architectures based upon optical networks, quantum dots permit light-matter coupling between matter qubits and photonic links. Single trapped charge carriers in quantum dots can be addressed optically, generating spin-photon entanglement between the matter qubits and \lq flying' photon qubits, a key first step in creation of a network. Such an optically linked network of spins in quantum dots has yet to be realized. The semiconductor environment presents a key challenge; it broadens the spectrum of the emitted light, which reduces the fidelity of schemes based upon photon exchange or interference. In addition, these quantum dots are subject to hyperfine coupling to a bath of > 105 nuclear spins. While this presents an opportunity to study the physics of a central spin in a spin bath, it degrades the spin coherence of a trapped electron or hole. The suggested gate operations to generate entanglement, and the spin measurements to verify a created state, rely upon photon detection. Thus a second limitation occurs due to low efficiency of detectors and photon collection probability. Recent developments in detector technology have enabled us to bring generation and verification of entangled states with quantum dots into the realm of possibility. This dissertation begins with a detailed study of the interaction of a single electron spin with the solid state environment of the quantum dot, analysing the intensity noise of scattered light under resonant excitation to uncover the timescales and relative amplitudes of identified noise sources. A technique for rapid characterization of samples is presented, focusing in particular upon comparison of spectral broadening of the optical transitions relevant to a spin-photon interface. Having identified the extent of environmental factors acting upon the quantum dots, we turn to a demonstration of photon-mediated entanglement between two distant electron spins using a probabilistic scheme. We are able to generate entangled states at 7 kHz, the fastest yet reported for photon-mediated protocols. The average state fidelity of the created Bell states is 63.5 ± 3.0 \%., violating the classical limit by over 4 standard deviations of the mean. In addition, we demonstrate full optical phase tuning of the Bell state ∣Ψ=21(∣↑∣↓+eiϕ∣↓∣↑). This is a proof of principle experiment, and sets a fidelity benchmark upon which gains can be made by mitigation of environmental dynamics.
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.