In this thesis, we assess various climatic impacts of stratospheric aerosol injection (SAI), a geoengineering proposal that aims to cool Earth by enhancing the sunlight-reflecting aerosol layer in the lower stratosphere. To this end, we employ simpleradiative transfer models, a detailed radiative transfer code (SOCRATES), and two Hadley Centre general circulation models (HadGEM2-CCS and HadGEM2-ES). We find that the use of a light-absorbing aerosol (black carbon) for SAI would result in significant stratospheric warming and an unprecedented weakening of the hydrological cycle. Conversely, we find that SAI with sulphate or titania aerosol could counteract many of the extreme climate changes exhibited by a business-as-usual scenario (RCP8.5) by the end of this century. In a separate investigation, we show that volcanic aerosol dispersion following low-altitude volcanic eruptions can exhibit high sensitivity to the ambient weather state. Volcanic aerosol may get 'trapped' in a single hemisphere or transported to the opposite hemisphere depending simply on the meteorological conditions on the day of the eruption. In a final study, we investigate the impacts of SAI on North Atlantic tropical storm frequency. We find that SAI exclusively promoted in the southern hemisphere would increase North Atlantic storm frequency, and vice versa for northern hemisphere SAI. The results of this thesis should promote further research into SAI, which could conceivably be deployed to maintain global-mean temperature below the COP21 target of +1.5 K above pre-industrial levels, whilst society transitions onto a sustainable energy pathway. Conversely, the possibility of SAI being weaponised, for instance, to specifically increase North Atlantic tropical storm frequency, should motivate policymakers to implement effective regulation and governance to deter unilateral SAI deployments.

This paper aims to study how varying crossflow burning temperatures from 1100 C to 1800 C affect the liquid droplet breakup, size distribution, and atomization of a liquid water jet injected into a vitiated crossflow. The LJIC injection mechanism was implemented using the high-pressure axially staged combustion facility at the University of Central Florida. The measurement devices used to gather particle data from the exhaust plume were the TSI Aerodynamic Particle Sizer (APS), which measures particles between 0.523 µm and 20 µm, and the Sensirion SPS30 (SPS30), which measures particles between 0.3 µm and 10 µm. Both measurement devices were placed 3 ft away from the choked exit. Table 3 shows that the 1800 C crossflow temperature behaved as predicted by having the largest particle distribution of 67.97% and the largest particle count of 19,301 at 0.523 µm. The 1100 C crossflow produced the second-largest normalized particle count of 66.69% and raw particle count of 20,209 at 0.523 µm. This result is contrary to the original hypothesis because it shows that the relationship between temperature and particle count is non-linear and that many other factors must be at play in the atomization process, such as the droplet distribution at the nano level. The SPS30 was used to compare the particle size distributions between a 1500 C and 1800 C crossflow. Acquiring number concentration data for particles up to 10 µm in size, the 1800 C crossflow had a distribution peak at 802.76416 N/cm3, and the 1500 C crossflow had a peak of 867.28272 N/cm3. For the 0.5 µm peak, The 1800 C had a 10 µm particle size distribution peak at 674.27.76416 N/cm3, and the 1500C crossflow had a peak of 730.501 N/cm3. The decreased number concentration from 1500 C to 1800 C case grants the water particles in the 1800 C crossflow increased surface area, which allows for increased heat exposure from the vitiated crossflow [7]. Despite some nonlinear particle count results, the highest crossflow temperature of 1800 C produces the best atomization results by reducing the total particle count and having the largest collection of particles at the lowest detectable particle size of 0.523 µm.

Coherent diffractive imaging (CDI) has become a very popular technique over the past two decades. CDI is a "lensless" imaging method which replaces the objective lens of a conventional microscope by a computational image reconstruction procedure. Its increase in popularity came together with the development of X-ray free-electron lasers (XFELs) which produce extremely bright and coherent X-rays. By facilitating these unique properties, CDI enables structure determination of non-crystalline samples at nanometre resolution and has many applications in structural biology, material science and X-ray optics among others. This work focuses on two specific CDI techniques, flash X-ray diffractive imaging (FXI) on biological samples and X-ray ptychography. While the first FXI demonstrations using soft X-rays have been quite promising, they also revealed remaining technical challenges. FXI becomes even more demanding when approaching shorter wavelengths to allow subnanometre resolution imaging. We described one of the first FXI experiments using hard X-rays and characterized the most critical components of such an experiment, namely the properties of X-ray focus, sample delivery and detectors. Based on our findings, we discussed experimental and computational strategies for FXI to overcome its current difficulties and reach its full potential. We deposited the data in the Coherent X-ray Database (CXIDB) and made our data analysis code available in a public repository. We developed algorithms targeted towards the needs of FXI experiments and implemented a software package which enables the analysis of diffraction data in real time. X-ray ptychography has developed into a very useful tool for quantitative imaging of complex materials and has found applications in many areas. However, it involves a computational reconstruction step which can be slow. Therefore, we developed a fast GPU-based ptychographic solver and combined it with a framework for real-time data processing which already starts the ptychographic reconstruction process while data is still being collected. This provides immediate feedback to the user and allows high-throughput ptychographic imaging. Finally, we have used ptychographic imaging as a method to study the wavefront of a focused XFEL beam under typical FXI conditions.  We are convinced that this work on developing strategies and algorithms for FXI and ptychography is a valuable contribution to the development of coherent diffractive imaging.

The newly emerging technology of X-ray free-electron lasers (XFELs) has the potential to revolutionise molecular imaging. XFELs generate very intense X-ray pulses and predictions suggest that they may be used for structure determination to atomic resolution even for single molecules. XFELs produce femtosecond pulses that outrun processes of radiation damage and permit the study of structures at room temperature and of structural dynamics. While the first demonstrations of flash X-ray diffractive imaging (FXI) on biological particles were encouraging, they also revealed technical challenges. In this work we demonstrated how some of these challenges can be overcome. We exemplified, with heterogeneous cell organelles, how tens of thousands of FXI diffraction patterns can be collected, sorted, and analysed in an automatic data processing pipeline. We improved  image resolution and reduced problems with missing data. We validated, described, and deposited the experimental data in the Coherent X-ray Imaging Data Bank. We demonstrated that aerosol injection can be used to collect FXI data at high hit ratios and with low background. We reduced problems with non-volatile sample contaminants by decreasing aerosol droplet sizes from ~1000 nm to ~150 nm. We achieved this by adapting an electrospray aerosoliser to the Uppsala sample injector. Mie scattering imaging was used as a diagnostic tool to measure positions, sizes, and velocities of individual injected particles. XFEL experiments generate large amounts of data at high rates. Preparation, execution, and data analysis of these experiments benefits from specialised software. In this work we present new open-source software tools that facilitates prediction, online-monitoring, display, and pre-processing of XFEL diffraction data. We hope that this work is a valuable contribution in the quest of transitioning FXI from its first experimental demonstration into a technique that fulfills its potentials.