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.
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.
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.
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.
Single semiconductor quantum dots, which are considered as two-level systems in the artificial atom model, are promising structures for the realization of integrated devices such as single photon sources for quantum information applications. However, contrary to genuine atoms, they are condensed matter systems which suffer from the coupling to their solid environment, leading to a degradation of the coherence of the emitted photons. One possibility to avoid this coupling, thereby improving the coherence of the photons until the one imposed by the radiative limit T2 = 2T1, is to perform strictly resonant excitation of a quantum dot at low temperature. Using an experimental setup that spatially decouples the excitation and detection paths, we showed that a fine control of the electrostatic environment related to the nanostructures residual doping remains a major challenge to answer the widely encountered problem of the inhibition of the resonance fluorescence of a quantum dot. Meanwhile, thanks to quantum optics experiments and high resolution optical spectroscopy, we demonstrated that the resonant Rayleigh scattering regime where quantum dots emit single photons with the laser coherence time, paves the way to the development of "ultra-coherent" sources of single photons with high degrees of indistinguishability. In this regime where the laser tailors the coherence of the photons and where the radiative limit becomes a secondary requirement, two photons emitted successively by the same quantum dot are indistinguishable on time scales never obtained before for a solid nano-emitter (up to ten nanoseconds, comparing to the carriers lifetime and decoherence time of about a hundred of picoseconds).
New technologies based on the properties of quantum mechanics promise to revolutionise the way information is processed by outperforming what is possible using classical devices. Examples include massively parallel processing using quantum computers, verifiably secure communication using quantum cryptography, and measurement with sensitivity beyond classical limitation with quantum metrology. Realising the full potential of these technologies necessitates the ability to communicate quantum information over large distances, a key requirement for future quantum networks. However, developing practical implementations of long-distance quantum communication is challenging as it necessitates three major ingredients: light-matter interfaces, elementary quantum operations, and quantum memories. This thesis describes work that has been undertaken to address these requirements using semiconductor nanotechnology. We have first demonstrated that single InAs quantum dots embedded inside conventional diode structures constitute high-fidelity controllable interfaces between optical qubits and solid-state qubits. Indeed, the polarisation state of a photon was transferred into the spin state of an electron-hole pair and eventually restored through radiative recombination of the electron and the hole with a fidelity up to 95%. Moreover, spins were manipulated using subnanosecond modulation of a vertical electric field applied to the quantum dots. By controlling this electrical modulation, we demonstrated elementary phase-shift and spin-flip gate operations with near-unity fidelities. An electron-hole pair confi ned in a single quantum dot has a short radiative lifetime limiting therefore its use as an excitonic quantum memory. The solution we proposed was to use a quantum dot molecule to control the spatial separation of the electron and the hole and therefore prevent their recombination. Comprehensive studies of electric field eff ects upon the photoluminescence of quantum dot molecules lead to a clear understanding and a good control over their physical properties. Single photons were stored in individual quantum dot molecules up to 1μs and read out on a subnanosecond time scale. Moreover, the circular polarisation of individual photons was transferred into the spin state of electron-hole pairs with a fidelity above 90%, which does not degrade for storage times up to the 12.5 ns repetition period of the experiment. Our work on single quantum dots could be extended in the near future to allow for two-qubits quantum operations by con fining a second electron-hole pair to be electrically manipulated. Storage of a superposition of spin states in a quantum dot molecule should also be possible if the spin states are made degenerate, which is feasible using the electric fi eld dependence of the energy splitting between the spin states discussed in this thesis. We believe that combining both approaches will lead to the development of a controllable multi-qubit quantum memory for polarised light, a building block for long distance quantum communication based on semiconductor nanotechnology.
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.
Quantum networks lie at the heart of distributed quantum computing and secure quantum communication - research areas that have seen a strong increase of interest over the last decade. Their basic architecture consist of stationary nodes composed of quantum processors which are linked via photonic channels. The key requirement, and at the same time the most demanding challenge, is the efficient distribution of entanglement between distant nodes. The two ground states of single spins confined in self-assembled InGaAs quantum dots provide an effective two-level system for the implementation of quantum bits. Moreover, they offer strong transition dipole moments with outstanding photonic properties allowing for the realisation of close to ideal, high-bandwidth spin-photon interfaces. These properties are combined with the benefits of working in the solid state, such as scalability and integrability of devices, to form a promising candidate for the implementation of fast entanglement distribution. In this dissertation we provide the first implementation of a unit cell of a quantum network based on single electron spins in InGaAs. We use a probabilistic scheme based on spin-photon entanglement and the erasure of which path information to project the two distant spins into a maximally entangled Bell state. The successful generation of entanglement is verified through a reconstruction of the final two-spin state and we achieve an average fidelity of 61.6±2.3% at a record-high generation rate of 5.8kHz. One of the main constraints to the achieved fidelity is the limited coherence of the electron spin. We show that it can be extended by three orders of magnitude through decoupling techniques and develop a new measurement technique, allowing us to investigate the origins of the decoherence which has previously been obscured by nuclear feedback processes. Our results evidence that further extension of coherence is ultimately limited by intrinsic mechanisms closely related to local strain due to the growth method of self-assembled quantum dots. After establishing the intrinsic limits to the electron coherence we investigate the coherence properties of the single hole spin as an alternative two-level system with the potential for higher coherence times. We show that the hole spin coherence is indeed superior to the one of the electron and realise the first successful dynamic decoupling scheme implemented in these systems. We find that the decoherence at low external magnetic fields is still governed by coupling to the nuclear spins whereas it is dominated by electrical noise for fields exceeding a few Tesla. This noise source is extrinsic to the quantum dots and a better understanding offers the potential for further improvement of the coherence time. The findings of this work present a complete study of the coherence of the charge carriers in self-assembled quantum dots and provide the knowledge needed to improve the implementation of a quantum-dot based quantum network. In particular, the combination of spin-spin entanglement and the hole coherence times enable further research towards multidimensional photonic cluster states.