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The question of how statistical physics can be seen to emerge from unitary quantum dynamics goes back to Schrödinger and von Neumann, however has been reaffirmed as a topic of importance due to recent advances in experimental capabilities, allowing the observation of the unitary evolution of many-particle systems over long periods of time. Understanding why such a system evolves to the specific thermal equilibrium state, effectively described by a relevant thermodynamic ensemble, has thus seen significantly more interest in recent years. Furthermore, observations of the dynamics of such systems open questions on the route to equilibrium, and subsequent fluctuations. In this thesis I will develop an approach to this problem, taking as a starting point the non-integrability of the system under study, which leads to a generic model in terms of random matrix theory (RMT), and more generally, chaotic wavefunctions. In the formulation of these methods, special attention is paid to the form of local observables of quantum systems, and an approach to their description is developed in terms of correlation functions of chaotic wavefunctions. From this approach a key conjecture in the understanding of thermalization, the eigenstate thermalization hypothesis (ETH), is derived in full, and the dynamical behaviour of such observables is obtained analytically. Further, I will show that emergent classical behaviour can be observed in the form of a fluctuation-dissipation theorem (FDT) of Brownian processes. This is exploited to develop an experimental proposal to measure the ‘complexity' of a quantum device, by experimentally obtaining its effective Hilbert space dimension in terms of a fully connected system. Finally, quantum jump trajectories, describing stroboscopic projective measurements of local observables are studied, and shown to display classical Brownian dynamics in the form of a Markov process. Throughout this thesis, exact diagonalization calculations of realistic quantum spin systems are used to confirm analytical results.