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The design of superconducting materials in order to achieve higher transition temperatures (Tc) to the zero-resistance state has been recognised by recent international and national reviews as at the extreme forefront of current challenges in condensed matter science with potential for transforming existing and enabling new technologies of tremendous economic and societal benefits in energy and healthcare. Achieving the zero-resistance state requires close control of the interactions of electrons with each other (known as electron correlation) and with lattice vibrations (phonons). This project addresses these challenges by building on EPSRC-supported collaborative work by the project team, which has shown that high Tc superconductivity, defined both in terms of transition temperature and the key role played by electronic correlations, is accessible in molecular systems. In the fullerene-based molecular superconductors, superconductivity occurs in competition with electronic ground states resulting from a fine balance between electron correlations and electron-phonon coupling in an electronic phase diagram strikingly similar to that of the atom-based copper oxide high Tc superconductors, where correlation plays a key role. A second molecular superconductor family with transition temperatures over 30 K, based on metal intercalation into aromatic hydrocarbons, has also been reported. It is therefore timely to optimise and understand superconducting materials made from molecules arranged in regular solid structures. The scope of synthetic chemistry to tailor molecular electronic and geometric structure makes the development of molecular superconducting systems important, because this chemical control of the fundamental building units of a superconductor is not possible in atom-based systems. The molecular systems are the only current candidates for the important target of isotropic correlated electron superconductivity. We will exploit these opportunities by integration of new chemistry with new physical understanding, exemplified by revealing how changes in molecular-level orbital degeneracy driven by chemical control of molecular charge and overlap direct the electronic structure of an extended solid. We will develop the new chemistry of the molecular solid state that will be needed for this level of electronic structure control, in particular mastering the chemistry of metal intercalation into hydrocarbons. This new materials chemistry will include the use of new building blocks (such as endohedral metallofullerenes) and will harness the assimilation of defects to access new molecular packings, motivated by our discovery that different packings of the same molecular unit give different Tc and distinct electronic properties. Further structural control will be exercised by binding small molecules to the cations intercalated into the molecular lattices. The synthesis of metal-intercalated solids based on multiple molecular components will be undertaken to permit detailed optimisation of the electronic structure. We will thus specifically exploit the molecular system advantages of isotropy, packing and molecular-level electronic structure control by developing the new chemistry of the molecular solid state needed to establish the new electronic ground states. Physical understanding of the structural and chemical origins of the new electronic states is essential to identify the factors controlling the electron pairing in the superconductors. This understanding will emerge from an integrated investigation of the insulator-metal-superconductor competition, spanning thermodynamic, spectroscopic and electronic property measurements closely linked to comprehensive structural work in order to produce the structure-composition-property relationships required for the design of next generation systems. The project benefits from an international multidisciplinary collaborative team to ensure all relevant techniques are deployed.

This is a long-range basic research project that targets the synthesis of a new crystalline materials family whose chemical, electronic and magnetic properties will create opportunities in fundamental science. To date, such advances have mainly been made in inorganic materials. This project will extend that opportunity to materials where the electronically active component is an organic anion. Our understanding of materials such as silicon and copper relies on a description of the electrons in which they do not interact strongly with each other. The electronic behaviour of materials in which the electrons do interact strongly, known as correlated materials, differs from such classical free electron materials. Correlated materials have been a fruitful source of new electronic and magnetic ground states and properties. This behaviour has overwhelmingly been observed in inorganic systems, because of the capability offered by inorganic solid state materials chemistry to position multiple distinct metal cations and thus predictably arrange spins, orbitals and charges. We have no such synthetic capability or crystal chemical understanding for organic correlated electron materials. The one example of success is the fulleride superconductors such as K3C60, where the underlying crystal chemistry is based on sphere packing that is directly analogous to well-studied inorganic systems, enabling extensive synthetic control and property design. While currently offering an outstanding range of properties, all-inorganic systems are restricted to the atoms provided by the periodic table, whose crystal and electronic structures are controlled by the ionic size and orbital characteristics of those elements. If we could achieve similar general control of structures based on electronically active organic species, such as anions derived by reduction of unsaturated molecules studied here, the resulting structural and electronic properties would be determined by the molecular size, shape and electronic structure. In contrast to the inorganic ionic systems, these steric and electronic structures of the organic molecules that would be the building blocks of such materials are controllable by synthetic chemistry. In two recent papers in Nature Chemistry, we have reported chemical synthesis approaches that produce crystalline salts of reduced unsaturated aromatic molecules and access new electronic states, including a candidate for the quantum spin liquid ground state in a three-dimensional pi-electron based material. This advance demonstrates the potential to create a family of tuneable crystalline organic electronic materials beyond the fullerides. The project will establish this family, allowing the positioning of electronically and sterically tuneable building blocks to control electronic, magnetic, optical and charge storage properties. This will be achieved by developing the synthetic chemistry capability to produce crystalline materials from a broad range of unsaturated organic molecules. To generate materials of comparable compositional and structural complexity to the inorganic systems, we will apply and expand this chemistry to materials with multiple metal sites and with more than one molecular component. This will allow us to control extended electronic structure by positioning of and charge transfer between the molecular units to target geometrically frustrated magnetic lattices and mobile charges in quantum spin liquids as examples of the new electronic ground states this chemistry will enable. The compositions, charge states and structures of the resulting hydrocarbon salts will reveal the charge storage potential of this family of materials. We will use informatics techniques to guide efficient exploration of the chemical space, and apply a range of structural, thermodynamic, spectroscopic, electronic and magnetic measurement techniques with our international collaborators to identify the new electronic states that arise.

Biofilms are groups of microorganisms that stick to each other on a surface, becoming an organised colony that is surrounded by a slimy substance to form a diverse and well protected community. A common example of a biofilm that everyone can relate to is the formation of plaque on teeth, which left untreated causes tooth decay. While biofilm formation in the mouth is mostly harmless, it has been estimated that up to 80 % of all infections worldwide are biofilm-related. In particular, biofilm colonisation of implanted devices such as Endotracheal tubes presents a particularly resilient reservoir of infection, shielded from systemic antibiotics, that often leads to the emergence of multidrug-resistant colonies. Patients contracting such infections have a particularly bleak outlook, with mortality rates for diseases such as Ventilator Associated Pneumonia (VAP) exceeding 50 % in certain patient groups. Quite simply, establishing a management strategy for these organisms is a global priority. Cold plasma technology has recently attracted global attention as it provides an effective means to destroy biofilm contamination, including biofilms containing multidrug resistant bacteria. A major barrier to the implementation of this promising technology is a lack of innovation in plasma source development. This award will tackle the challenge by developing novel power sources and systems that produce an output tailored specifically to manage biofilm contamination on implanted devices in situ; these efforts will be driven by a closely interacting team of specialists in microbiology and translational medicine, clinicians and patients. Key to this will be the unique methods and understanding uncovered on my previous EPSRC funded research which addressed the Physical Sciences grand challenge area of Emergence and Physics Far From Equilibrium (EP/J005894/1). My long term research vision is to establish a multidisciplinary centre of excellence focused on the development of novel plasma based physical interventions as part of my ambition to revolutionise technology driven approaches to global health challenges. The Centre will act as a hub to facilitate new thinking/methodologies/technology in this area driven by novel engineering and physical sciences research and will be a catalyst to explore new scientific horizons. Delivering this vision will demand a transformative approach that pushes the frontiers of plasma science and breaks-down traditional discipline boundaries. Success will require creativity, ambitious plans, high levels of flexibility and the necessary taking of risks balanced against the scope for reward. I will manage these aspects within the framework of a coherent research programme, and activities will be underpinned by a hand-picked team of research leaders. At the heart of my approach is the sustained and active involvement of end-users to inform research design and research goals. My approach will ensure priorities focus on clinical need, an essential factor to drive innovation and ensure successful translation. The average timeline for translation of new technologies in to the healthcare sector ('bench to bed') is 17 years; given the immediate clinical need for the proposed technology, accelerating the translational process will be a key priority of the Centre. Drawing on the wealth of expertise available in the project team and the unique innovation eco-system in Liverpool, which includes the North West Coast Academic Health Science Network (AHSN - www.nwcahsn.nhs.uk), a translational plan has been established to see the introduction of plasma decontamination technology in the healthcare sector within a 10 - 12 year timeframe. The introduction of this technology will have a significant impact in a market sector valued at $14 billion; directly contributing to the UK's strong life sciences industry, which employs an estimated 183,000 and generates a combined estimated turnover of £56bn.

Metals are used for electricity transmission, but energy is lost as heat because of electrical resistance. Superconductors have no electrical resistance and can carry electricity without losing energy, so finding superconductors which work at as high a temperature as possible is important. Most superconductors have simple structures built from atoms, but recently superconductors made from molecules arranged in regular solid structures have been found. Recent work by the proposing groups on molecular fulleride-based systems led to the discovery of the highest working temperature (at 38 K) for a molecular superconductor. We found that the electronic ground state which is in competition with superconductivity is magnetically ordered - this ordering also occurs at a very high temperature (46K) for a material where the active electrons are in orbitals of s/p parentage. We showed how the exact arrangement of the C60 molecules in the solid with stoichiometry Cs3C60 can be controlled to switch on the zero-resistance superconducting state from the insulating magnetically ordered state. In this project we will exploit the newly presented opportunities arising from these discoveries. We will identify the factors responsible for determining whether superconducting or magnetic ground states are adopted in new fulleride systems. We will develop new structural families of molecular, s/p electron-based superconductors and magnets with enhanced properties, controlled in an understandable manner by crystal symmetry, orbital degeneracy and lattice packing. In order to achieve this, we will use focussed solution-based synthetic protocols that we have pioneered, combined with structural and physical property measurements at ambient and high pressure and high-level electronic structure calculations. The project will explore unique aspects of the behavior of correlated electrons in solids i.e. electrons whose behavior is determined by their mutual Coulomb repulsion. This is one of the most important contemporary problems in condensed matter science. The high molecular and lattice symmetry of fullerene-based solids offers an opportunity to study strongly correlated electrons under conditions that are qualitatively different from previously studied materials, and therefore to take our understanding of molecular superconductivity and magnetism and the metal-insulator transition to an unprecedentedly advanced stage. The programme exploits the complementary expertise of the two principal investigators and will lead to a new generation of novel fullerene-based molecular materials with unpredictable and theoretically challenging properties.