Abstract: Nanoplasmonics has provided a way to control light with extremely high precision, into nanoscale volumes. In many circumstances, the nanoplasmonic devices which can be realised are fabricated using processing techniques which rely on planar technologies. This thesis provides a general method to make nanoplasmonic devices on a flexible membrane structure, which can be free standing, extremely thin (less than the wavelength of visible light), but retains the ability to be manipulated without loss of optical function. These devices are very pliant and conformable. Flexibility allows the integration of nanoplasmonic devices into many new applications where curved surfaces or the ability to conform to another object is required, as well as providing a route for post-fabrication tunability. Two specific applications are considered: lab-on-fibre technology and surface enhanced Raman spectroscopy. Lab-on-fibre technologies have been advancing the ability to miniaturise experiments which would normally require a whole laboratory. Fabricating a membrane and then later applying it to the fibre decouples the choice of fibre from the design of the device. Surface enhanced Raman spectroscopy is a powerful diagnostic tool which can uniquely identify an optical fingerprint of different molecules. The technique has been held back from widespread clinical adoption because of the difficulty of reproducibility of the substrates used. A repeatable and reliable rigid substrate is demonstrated, which can identify the concentration of a three component mixture of physiologically relevant biomolecules. This same design is then shown in a flexible form factor, which is applied to a non-planar landscape where it can identify the locations where a molecule of interest has been deposited. This thesis details the development of the fabrication protocol, the construction of experimental apparatus for characterisation, and the use of numerical modelling to advance the flexible nanoplasmonic membrane platform. Candidate’s declarations: I, Peter Reader-Harris, hereby certify that this thesis, which is approximately 40,000 words in length, has been written by me, and that it is the record of work carried out by me, or principally by myself in collaboration with others as acknowledged, and that it has not been submitted in any previous application for a higher degree. I was admitted as a research student in September 2011 and as a candidate for the degree of Doctor of Philosophy in September 2011; the higher study for which this is a record was carried out in the University of St Andrews between 2011 and 2015. Date Signature of candidate Supervisor’s declaration: I hereby certify that the candidate has fulfilled the conditions of the Resolution and Regulations appropriate for the degree of Doctor of Philosophy in the University of St Andrews and that the candidate is qualified to submit this thesis in application for that degree. Date Signature of supervisor Permission for publication: In submitting this thesis to the University of St Andrews I understand that I am giving permission for it to be made available for use in accordance with the regulations of the University Library for the time being in force, subject to any copyright vested in the work not being affected thereby. I also understand that the title and the abstract will be published, and that a copy of the work may be made and supplied to any bona fide library or research worker, that my thesis will be electronically accessible for personal or research use unless exempt by award of an embargo as requested below, and that the library has the right to migrate my thesis into new electronic forms as required to ensure continued access to the thesis. I have obtained any third-party copyright permissions that may be required in order to allow such access and migration, or have requested the appropriate embargo below. The following is an agreed request by candidate and supervisor regarding the publication of this thesis: PRINTED COPY No embargo on print copy ELECTRONIC COPY No embargo on electronic copy Date Signature of candidate Signature of supervisor