This thesis would not have been possible without the support of my supervisor Prof Marty Gregg, who was an endless source of optimism and good advice. Marty was always happy for me to drop by and chat about results or even just to talk when things were difficult. I chose my PhD project partly on the basis that he would be my supervisor after enjoying his undergraduate lectures so much, and I definitely think it paid off! During my PhD I had the opportunity to work with a large number of people both in QUB and elsewhere who provided so much support and knowledge, without which this project could not have gone ahead. In QUB, special thanks goes to the technical staff of ANSIN and the Electron Microscopy Unit; Bill Hendren for all his help with the Lesker, VSM and basically keeping the entire ANSIN lab running singlehandedly, Stephen McFarland and Alina Schilling for always being there for help with the FIBs and TEMs (and we all know how much trouble they can be!). Thanks to Amit Kumar for advice on PFM and for being a great examiner -my viva was much less stressful than it could have been thanks to you. Special thanks also must go to my fellow PhD students and postdocs at QUB for all their help with learning how to use equipment and how to keep going when you lose your 100 th lamella...Kristina, Paddy, Jimmy, Charlotte, Jade, Joseph and many others who really taught me what I needed to know to get the results.To my fellow first-cohort CDT crew, we finally made it! It was a tough road sometimes, but we all got through it. Hannah, Jade, Emma, and Matt have been with me through the whole project and I feel like we've bonded through the battles! Thanks also to all my wonderful friends, some of whom have been with me since the first day of undergrad physics 8 years ago -Aaron, Kathy, Steve, Chris, Hannah, Rachael, and too many others too mention. This PhD wouldn't have been the same without Friday Parlour Pints and I can't wait to get back out with you! My wonderful family have been so supportive through this whole process, Mum, Dad, Bridget, Christopher and my favourite little lady in the whole world, my niece Lily, who never fails to brighten up my day.Lastly and most importantly, the most special thanks go to my wonderful fiancé Gavin. I don't know how you put up with me for all this time, but I'm very grateful that you have. I'd never have got this PhD without you, so really, they should be giving you the title as well. And of course, thanks to my cat Pabu, for all the cuddles and walking across my keyboard at key moments.