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 $>$ 10$\mathrm{<mrow\; data-mjx-texclass="ORD">5</mrow>}$ 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 $\pm$ 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 $|\Psi =12(|\uparrow |\downarrow +ei\varphi |\downarrow |\uparrow )$. This is a proof of principle experiment, and sets a fidelity benchmark upon which gains can be made by mitigation of environmental dynamics.