This thesis investigates the carrier and gain dynamics of semiconductor quantum dots in the strong quantum confinement regime (i.e. the dot radius is smaller than the bulk excitonic Bohr radius). The materials under investigation are InP and CdSe. We can summarize our findings as follows: For the first time, the quantum confined ground state in InP quantum dots has been observed at room temperature by femtosecond spectral holeburning. This is the first confirmation of the observation of a strongly confined quantum dot made of III-V semiconductor materials. In CdSe quantum dots with a radius of half the bulk exciton Bohr radius, the carrier and gain dynamics have been investigated. The predicted phonon bottleneck, which should slow down carrier relaxation up to nanoseconds, has not been found. The carrier relaxation rates are rather on the order of 1 eV/ps. Gain has been found for the first time in strongly confined quantum dots. The existence of gain was proven by spectral holeburning in the gain region. The gain buildup and decay dynamics have been studied on a femtosecond and picosecond timescale. A multi-level model including biexcitons accounts for the gain formation. The model has been confirmed by three-beam spectral holeburning experiments and femtosecond pump-probe experiments with circularly polarized light. Some quantum dots did not show gain under high optical excitation but instead exhibited photodarkening. The carrier separation and localization dynamics of this photodarkening process has been studied on a femtosecond timescale. For the first time, the shift of the bleaching towards lower energy during the localization process could be observed on a femtosecond timescale. Finally, pulse propagation in bulk CdSe at multiple Pi-pulses has been studied. For the first time, strong evidence for the observation of self induced transparency in semiconductors has been found. Also, optical precursors, probably of nonlinear nature, have been found.

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This thesis presents the results of muon-spin relaxation (µ⁺<abbr>SR</abbr>) studies into magnetic materials, and demonstrates how these results can be exploited to quantify the materials’ low moments and reduced dimensionality. Dipole-field simulations, traditionally used to estimate likely muon sites within a crystal structure, are described. A novel Bayesian approach is introduced which allows bounds to be extracted on magnetic moment sizes and magnetic structures—previously very difficult using µ⁺<abbr>SR</abbr>—based on reasonable assumptions about positions in which muons are likely to stop. The simulations are introduced along with relevant theory, and MµCalc, a platform-independent program which I have developed for performing the calculations is described. The magnetic ground states of the isostructural double perovskites Ba₂NaOsO₆ and Ba₂LiOsO₆ are investigated with µ⁺<abbr>SR</abbr>. In Ba₂NaOsO₆ long-range magnetic order is detected via the onset of a spontaneous muon-spin precession signal below <var>T</var>_c = 7.2(2) K, while in Ba₂LiOsO₆ a static but spatially-disordered internal field is found below 8 K. Bayesian analysis is used to show that the magnetic ground state in Ba₂NaOsO₆ is most likely to be low-moment (˜ 0.2<var>µ</var>_B) ferromagnetism and not canted antiferromagnetism. Ba₂LiOsO₆ is antiferromagnetic and a spin-flop transition is found at 5.5 T. A reduced osmium moment is common to both compounds, probably arising from a combination of spin–orbit coupling and frustration. Results are also presented from µ⁺<abbr>SR</abbr> investigations concerning magnetic ordering in several families of layered, quasi–two-dimensional molecular antiferromagnets based on transition metal ions such as <var>S</var> = ½ Cu²⁺ bridged with organic ligands such as pyrazine. µ⁺<abbr>SR</abbr> allows us to identify ordering temperatures and study the critical behaviour close to <var>T</var>_N , which is difficult using conventional probes. Combining this with measurements of in-plane magnetic exchange <var>J</var> and predictions from quantum Monte Carlo simulations allows assessment of the degree of isolation of the 2D layers through estimates of the effective inter-layer exchange coupling and in-layer correlation lengths at <var>T</var>_N. Likely metal-ion moment sizes and muon stopping sites in these materials are identified, based on probabilistic analysis of dipole-fields and of muon–fluorine dipole–dipole coupling in fluorinated materials.

The twin questions of how and why protein molecules fold into the specific topologies which enable them to fulfill their biological function have been the subject of continuous scientific investigation since the early twentieth century. Interactions between biological macromolecules and water are obviously crucial to both folding and function but attempts to gain understanding are impeded by the size and complexity of these systems. A useful approach is to consider much simpler model systems which capture some essential element of real biological systems but are experimentally and theoretically tractable. N-methylacetamide (NMA) is a minimal model of the peptide linkage which forms the backbone of protein molecules. Its behaviour in aqueous solution therefore captures the important competition between peptide - peptide and peptide - water hydrogen bonds which arises in protein hydration. In this thesis aqueous NMA solutions are studied across the full concentration range using classical molecular dynamics simulation. This gives access to the complete spectrum of behaviour between the two important limiting cases of dilute NMA in water and, conversely, dilute water in NMA. Water is now known to be an active player in biological interactions and the simple system studied here displays significant disruption of the structure and dynamics of pure water with the addition of only a small proportion of peptide groups. At dilute NMA concentrations water molecules continue to form system-size hydrogen bonded networks. Water molecules appear to optimise their local tetrahedral order by forming hydrogen bonds with a combination of NMA and water neighbours, rather than solely with members of their own species. NMA molecules hydrogen bond through the amide and carbonyl groups to form linear and branched chains in both the pure liquid and in the aqueous solutions. In the NMA rich region water molecules preferentially donate both hydrogens to chain-end or midchain carbonyl oxygens, forming bridges between NMA chains which resemble buried water configurations found in protein cavities. These bridge structures are thought to contribute to the observed slowing of the system dynamics at these concentrations. The investigation of dynamics by classical simulation is complemented by a quasielastic neutron scattering study of NMA in its liquid and aqueous phases.

<p> Micro- and nano-mechanical resonators with low mass and high vibrational frequency are often studied for applications in mass and force detection where they can offer unparalleled precision. They are also excellent systems with which to study nonlinear phenomena and fundamental physics due to the numerous routes through which they can couple to each other or to external systems. </p><p> In this work we study the structural, thermal, and nonlinear properties of various micro-mechanical systems. First, we present a study of graphene-coated silicon nitride membranes; the resulting devices demonstrate the high quality factors of silicon nitride as well as the useful electrical and optical properties of graphene. We then study nonlinear mechanics in pure graphene membranes, where all vibrational eigenmodes are coupled to one another through the membrane tension. This effect enables coherent energy transfer from one mechanical mode to another, in effect creating a graphene mechanics-based frequency mixer. In another experiment, we measure the resonant frequency of a graphene membrane over a wide temperature range, 80K - 550K, to determine whether or not it demonstrates the negative thermal expansion coefficient predicted by prevailing theories; our results indicate that this coefficient is positive at low temperatures &ndash; possibly due to polymer contaminants on the graphene surface &ndash; and negative above room temperature. Lastly, we study optically-induced self-oscillation in metal-coated silicon nitride nanowires. These structures exhibit self-oscillation at extremely low laser powers (~1&mu;W incident on the nanowire), and we use this photo-thermal effect to counteract the viscous air-damping that normally inhibits micro-mechanical motion.</p>