Various physical mechanisms that affect radiowave propagation at millimetre wavelengths are considered. Current modelling weaknesses are highlighted and new improved models or more appropriate modelling approaches are suggested. Interference and resonance phenomena in the scattering of spherical ice and water particles are reviewed. The long standing problem of the numerous resonances observed in the scattering diagrams of dielectric spheres is answered. The spatial structure and the physical characteristics of non-precipitable ice and water clouds are reviewed. Extinction and back scattering calculations for a wide variety of cloud models over the entire millimetre frequency spectrum are given. Multiple scattering and the effects of super-large drops in clouds are also dealt with. The potential of a spaceborne instrument in deducing information about the vertical structure of various cloud types is examined. Attenuation and reflectivity profiles resulting from various cloud types are calculated for a nadir pointing fixed beam millimetre wave radar operating at 94 GHz. The physics and application of the equation of radiative transfer to millimetre wave propagation in the earth's atmosphere are given and also is the solution of this equation for a typical millimetre wave remote sensing application. The theory of gaseous absorption at millimetre wavelengths is presented and an improved modelling approach is proposed for the calculation of the absorption and dispersion spectra of atmospheric gases. The effects of trace gases on communication systems operating at high altitudes are for the first time reported. Finally the use of the 60 GHz oxygen absorption band for top-side air traffic control/navigation and broadband transmission purposes is studied.

Technological limitations have prevented interrogation and manipulation of many signaling pathways in model and living systems required for the development of diagnostic and therapeutic modalities in diseases, such as cancer. Liposome-supported plasmon resonant gold nanoshells are biologically inspired composite structures, in which the liposome allows for the encapsulation of substances, and the plasmon resonant structure facilitates rapid release of encapsulated contents upon laser light illumination. As shown in this work, we overcome current limitations in cellular manipulation using plasmon resonant gold-coated liposomes in conjunction with light-activated release to achieve accurate probing of complex cellular responses. Development toward this goal was demonstrated with four specific aims. The first specific aim was to develop a computational model of heat diffusion to investigate the light-induced heating of gold-coated liposomes. This model was used to optimize the photothermal process for release of an encapsulated payload. The second aim was to demonstrate encapsulation and on-demand release of molecules in a spectrally-controlled manner, where plasmon resonant nanoparticles only release content upon illumination with a wavelength of light matching their plasmon resonance band. The third specific aim was to demonstrate that this release mechanism can be used in a biological setting to deliver a peptide and extracellularly activate surface membrane receptors with single-cell spatial and high temporal resolution. The fourth specific aim further refined the level of spatial and temporal control of payload release using gold-coated liposomes with optical trapping to demonstrate mirco-manipulation of liposome movement and rapid content release to enable accurate perturbation of cellular functions in response to released compounds. Through this work, we have developed an experimental system with the potential for the delivery and localized release of an encapsulated agent with high spatial and temporal resolution. This on-demand release system is compatible with a broad range of molecules and uses biologically safe near-infrared light. In combination with the spectral tunability of these plasmon resonant nanoshells and spectrally-selective release, this technology may allow for interrogation of complex and diverse signaling pathways in living tissues or their models with unprecedented spatial and temporal control.

In this thesis results of x-ray scattering and neutron scattering experiments on several strongly correlated transition metal oxides are presented. The prototypical charge ordered cuprate La1.48Nd0.4Sr0.12CuO4 was investigated using polarised neutron scattering. The results show that several proposed schemes for the magnetic order in this class of materials may be ruled out, however the data are consistent with one-dimensional stripe-like magnetic order. X-ray diffraction was used to show that the charge order is insensitive to an applied magnetic field, but might be affected by the existence of superconductivity. The magnetic excitations were also studied, and at low energies a gap in the magnetic fluctuations was observed and there is tentative evidence that this is related to magnetic anisotropy. The spin state transition in LaCoO3 was investigated using neutron inelastic scattering, and excitations reminiscent of those observed in ferromagnets above their critical temperatures were observed. The debate surrounding the nature of the excited spin state, S=1 or S=2, could not be resolved, however. The nature of the spin excitations in La0.82Sr0.18CoO3 was investigated using polarised neutrons and it was found that at low energies the excitations take the form of spin-waves. At higher energies this mode becomes heavily damped, and several possible damping mechanisms for this are discussed. Finally, the multiferroic material DyMn2O5 was studied using x-ray resonant scattering. A complex, temperature dependent, magnetic structure was found using a Dy resonance, which reflects an underlying order of the Mn ions. The measurements were in agreement with a theory of multiferroics based on acentric spin-density waves.

Experimental studies presented in this thesis have shown the first realisation of resonant tunnelling transport through two impurities in a vertical double-barrier tunnelling diode; have proved the chiral nature of charge carriers in graphene by studying ballistic transport through graphene $p$-$n$ junctions; have demonstrated significant differences of $1/f$ noise in graphene compared with conventional two-dimensional systems. Magnetic field parallel to the current has been used to investigate resonant tunnelling through a double impurity in a vertical double-barrier resonant tunnelling diode, by measuring the current-voltage and differential conductance-voltage characteristics of the structure. It is shown that such experiments allow one to obtain the energy levels, the effective electron mass and spatial positions of the impurities. The chiral nature of the carriers in graphene has been demonstrated by comparing measurements of the conductance of a graphene $p$-$n$-$p$ structure with the predictions of diffusive models. This allowed us to find, unambiguously, the contribution of ballistic resistance of graphene $p$-$n$ junctions to the total resistance of the $p$-$n$-$p$ structure. In order to do this, the band profile of the $p$-$n$-$p$ structure has been calculated using the realistic density of states in graphene. It has been shown that the developed models of diffusive transport can be applied to explain the main features of the magnetoresistance of $p$-$n$-$p$ structures. It was shown that $1/f$ noise in graphene has much more complicated concentration and temperature dependences near the Dirac point than in usual metallic systems, possibly due to the existence of the electron-hole puddles in the electro-neutrality region. In the regions of high carrier concentration where no inhomogeneity is expected, the noise has an inverse square root dependence on the concentration, which is also in contradiction with the Hooge relation.

A resonant cavity operating in TE011 mode was used to study the adsorption response of single walled carbon nanotubes (SWCNTs) and other nanomaterials for different types of gas molecules. The range of the frequency signal as a probe was chosen as geometry dependent range between 9.1 -9.8 GHz. A highly specific range can be studied for further experiments dependent on the type of molecule being investigated. It was found that for different pressures of gases and for different types of nanomaterials, there was a different response in the shifts of the probe signal for each cycle of gassing and degassing of the cavity. This dissertation suggests that microwave spectroscopy of a complex medium of gases and carbon nanotubes can be used as a highly sensitive technique to determine the complex dielectric response of different polar as well as non-polar gases when subjected to intense electromagnetic fields within the cavity. Also, as part of the experimental work, a range of other micro-porous materials was tested using the residual gas analysis (RGA) technique to determine their intrinsic absorption/adsorption characteristics when under an ultra-high vacuum environment. The scientific results obtained from this investigation, led to the development of a chemical biological sensor prototype. The method proposed is to develop operational sensors to detect toxin gases for homeland security applications and also develop sniffers to detect toxin drugs for law enforcement agency personnel.

The energy levels of a hydrogen Rydberg atom approaching a metallic structure are perturbed by the image-charge interaction with the surface. At small atom-surface separations surface ionisation of the Rydberg electron can occur, whereby the electron is transferred to a metal-localised state. In previous studies investigating surface ionisation at bulk metallic surfaces, this state has been part of a conduction band; however this thesis focuses on metallic and structured surfaces where the Rydberg electron transfers into a discrete image-state or hybrid 'well-image state'. The surface ionisation of hydrogen Rydberg atoms at a Cu(100) projected band-gap surface is investigated experimentally and theoretically. Experimentally, the surface ionisation of an incident beam of hydrogen Rydberg atoms is measured by extraction of the resulting ions. Resonance-enhanced charge transfer is seen for hydrogen Rydberg states that are degenerate with copper-localised image-states. A wavepacket propagation study shows that for on-resonance states the maximum in the surface-ionisation probability is shifted away from the surface by decreasing the collisional velocity. The discrete hybrid 'well-image states' localised along the surface normal of a thin-film change energy with thin-film thickness. The interaction of hydrogen Rydberg atoms with iron thin films deposited on an insulating substrate is investigated. The preference for electron penetration along the surface normal is seen by the resonance-enhancement of charge transfer at energies where the Rydberg state and well-image state are degenerate. By changing the thickness of the thin film, by in situ depositions, the energies of the well-image state are altered and the Rydberg n-values at which resonances occur, change. At a thickness of 30-monolayer the energetic spacings between the well-image states and the Rydberg states become comparable, and the single well-image state resolution is lost. A wavepacket-propagation study investigates the interaction of a nanoparticle and low-n hydrogen Rydberg atoms. The nanoparticle has a fully confined potential which at small radii yields well-spaced, fully discrete well-image states. Resonance-enhanced charge transfer occurs when the Rydberg state and the nanoparticle well-image state energy levels are degenerate. However, when there is poor energy matching between the nanoparticle well-image state and the Rydberg atom, no charge transfer is seen i.e. surface ionisation does not occur. Overall, the work presented here demonstrates the capability of Rydberg-surface studies to identify discrete, high-lying energy levels at specific surfaces.

Resonant ionization laser ion sources are applied worldwide to increase purity and intensity of rare isotopes at radioactive ion beam facilities. Especially for heavy elements the laser wavelengths required for efficient resonant laser ionization are not only element dependent, but also vary to small degrees from isotope to isotope. Since the first operation of an actinide target at ISAC-TRIUMF in 2008, the demand for neutron-rich isotopes far away from stability has steadily increased. Those isotopes often have very low production rates so that often only a few ions per second are released. In order to study isotope shifts and hyperfine structure of silver, actinium and astatine, in-source resonant ionization spectroscopy in combination with radioactive decay detection has been applied. Despite the Doppler limited resolution, it has the advantage that it is ultra-sensitive and the atomic spectrum for the nuclear ground and isomeric states can be investigated individually. An isobaric separation has been demonstrated for 115-119Ag, where the hyperfine structure of one state showed a splitting of 22 GHz to 38 GHz while for the other state only a single peak spectrum can be resolved. For astatine and actinium, the main interest is to measure and study the optical isotope shift, which is for the first excitation step for neutron-rich isotopes in the order of IS_FES≈±3.7GHz/u for both elements, as these observables give insight into nuclear moments and shape. In addition, also the isotope shift of the second excitation step for astatine has been measured to IS_SES,At≈-1.7GHz/u. Laser spectroscopy on astatine has mainly been performed on the neutron-deficient isotopes 199,205At due to high count rates and low isobaric contamination. With the results obtained it is possible to extrapolate the required wavelength for ionizing and delivering the isotopes 221-225At which are of interest to e.g. electric dipole moment studies. / October 2017

This thesis presents three investigations of the magnetic and electronic proper- ties of manganese oxide materials. The investigations are performed using a variety of neutron scattering and x-ray scattering techniques. The electronic ground-state of Pr(Sr_0.1 Ca_0.9)₂ Mn₂O₇ an antiferromagnet with CE-type ordering, is determined using neutron spectroscopy, as opposed to the more usual approach of using diffraction. The Zener polaron model of the elec- tronic ground state of the CE-type magnetic phase is shown to be unsuitable for this material. The ground-state is shown to agree well with the electronic ground state proposed by Goodenough in the 1950’s, but without significant Mn^3+/Mn^4+ disproportionation. The distribution of the magnetisation density within the unit cell of the CE-type antiferromagnet La_0.5Sr_1.5MnO₄ is determined from a polarised neutron diffraction experiment by analysing the results with the maximum entropy method. The majority of the magnetisation density is found to be located at the Mn site. The investigation shows tentative evidence of a small magnetic moment on the in-plane O site. However, a larger moment is observed at both the La/Sr site and the out-of-plane O site. The magnetic structure of the magnetoelectric multiferroic DyMn₂O₅ is inves- tigated using resonant magnetic x-ray scattering. The magnetic structure is shown to be similar to other members of the RMn₂O₅ series of multiferroics, but with the key difference that the magnetic moments are closely aligned parallel with the crystallographic b-axis, in contrast to the usual observation of the moments being close to parallel with the a-axis. This study also shows evidence that the electrical polarisation has a significant contribution from the valence electrons of the O ions, agreeing with previous work.

The frequency shifts and Q changes of a resonant microwave cavity were utilized as a basis for determining microwave properties of solids and liquids. The method employed consisted of varying the depth of penetration of a cylindrical sample of the material into a cavity operating in the TM0 1 0 Mode. The liquid samples were contained in a thin-walled quartz tube. The perturbation of the cavity was achieved by advancing the sample into the cavity along the symmetry axis by employing a micrometer drive appropriately calibrated for depth of penetration of the sample. A differentiation method was used to obtain the half-power points of the cavity resonance profile at each depth of penetration. The perturbation techniques for resonant cavities were used to reduce the experimental data obtained to physical parameters for the samples. The probing frequency employed was near 9 gHz.

This thesis represents one phase of a joint effort of research on the properties of liquids and solids. This work is concerned primarily with the microwave properties of solids. In this investigation the properties exhibited by conductor and semiconductor materials when they are subjected to electromagnetic radiation of microwave frequency are studied. The method utilized in this experiment is the perturbation of a resonant cavity produced by introduction of a cylindrically shaped sample into it.