The industrial mass production of machines and devices relies on the assembly of different components in a specific order in the most rapid and efficient way. However what is routine at everyday length scales is infinitely more difficult and time consuming when we consider linking components to create nano-devices. This is particularly the case when one wishes to create a specific molecule-nanostructure construct. The individual component molecules and complex nanostructure architectures can be mass produced using tools of synthetic chemistry and nanofabrication techniques (e.g. nano-imprint and injection moulding). However, established technologies for combining these individual elements in a specific way are slow (e.g. dip pen nanolithography takes tens of hours to functionalise cm2 samples) and hence low throughput (i.e. incompatible with mass production). Therfore, creating relative complex hybrid molecular-nanofabricated materials is comparable to handcrafting a Bentley rather than the assembly line mass production of Volkswagen Golfs. We propose an innovative approach for nanoscale spatial control of chemical functionalisation of (plasmonic) nanostructures which has both nanoscale resolution ca. 20 nm and is simple and rapid. The concept, which we call "Meta-chemistry", involves using a pulsed laser to locally heat the solvent in specific regions surrounding a nanostructure. These nanoscale thermal gradients can then be exploited to drive chemistry in a spatially selective manner. In the proposal we will develop a fundamental understanding of how heat is generated and transported in a liquid surrounding a nanostructure, thus providing the foundation for optimal spatial control. Also crucially, we will synthesise thermally responsive polymers which will be transformed in the locally heated solvent, creating nano-domains which can be subsequently chemically functionalised. Using the meta-chemistry concept cm2 of a nanostructured substrate can be both spatially and selectively chemically modified, in preparation for subsequent chemical functionalisation, in less than 60 seconds. The proposal is at the cusp of chemistry physics and engineering, it will discover novel fundamental science which in the longer term could be the foundation of a powerful flexible technology for the nanoscience toolbox.

Ferroics are a class of materials that, below a certain ordering temperature, display either a long range ordering of microscopic +/- dipoles or of magnetic north-south (N/S) poles. These orderings on the microscopic atomic length scale give rise to macroscopic measurable physical properties. The +/- dipoles or N/S poles can be read and manipulated on the nanoscale by applying electronic and magnetic stimuli. In this manner existing technologies use materials like this in data storage devices where the "storage bits", the 1's and 0's correspond to the different state of either +/- or N/S. However, for next generation storage devices to improve energy consumption, increase speeds and data density, it will be desirable to have a new class of "multiferroic materials" in which these two phenomena of +/- charge dipoles and N/S magnetic state, not only coexist with one another, but are strongly coupled and depend on each other. This has significant advantages in that the data written by applying an electric field to switch a +/- state can now be read back quickly and non-destructively using a magnetic field to sense the flipping of the N/S pole. However, as yet it is still a substantial challenge to identify new materials that display this desired coupling between these two ferroic properties at or near room temperature, which would make such a device possible. The present work uses a novel approach to enumerate the possible types of materials exhibiting these properties, leading to a systematic strategy for attempting to make and test these materials for the desired physical properties. The work will contribute both new fundamental mechanistic insight into how multiferroic materials work, and can be rationally designed, as well as providing new materials that may be tested for application in next generation storage technologies.

The mid-infrared band of the electromagnetic spectrum has huge potential in healthcare technologies. Many biological molecules exhibit very strong absorption of radiation (light) in this region. This absorption depends strongly on matching the wavelength (colour) of the light to the stretching of the molecular bonds, unique to each molecule. For example, water absorbs radiation at a mid-infrared wavelength of 2.94 um nearly 100,000 times more strongly than a near-infrared wavelength of 1 um. A laser is an intense, highly directional, and monochromatic beam of radiation. The potential of mid-infrared lasers at 2.94 um as medical tools was recognised early on, due to the high-water content of biological tissue (>70%). Focussing a 2.94 um laser on tissue results in highly efficient absorption of the radiation in a very localised area. The subsequent rapid heating in this area causes the tissue to vaporise into a gas (ablation), resulting in an ultra-precise method of removing tissue, e.g. for use as laser scalpels or biopsy replacements. There are, however, a lack of ultrafast mid-infrared lasers with pulse durations shorter than 1 nanosecond (a billionth of a second) suitable for tissue ablation. Existing ultrafast mid-infrared commercial lasers do not have enough energy to initiate ablation, are often too large and complex to be deployed outside of specialist laser laboratories, or have poor beam qualities leading to large beam sizes on the sample (poor spatial resolution). As a result, the standard approach to 2.94 um tissue ablation is to use more widely available lasers (Er:YAG/Nd:YAG OPO) with longer pulses. However, the effect of these longer pulses on tissue can be highly problematic, causing tissue carbonisation (burning) and necrosis (cell-death) in surrounding cells, which can be avoided when using picosecond (ultrafast) pulses. In this project, I will create a compact, robust, fibre-integrated picosecond mid-infrared laser (fPIRL) platform. The platform will be based on a novel cascaded nonlinear wavelength conversion scheme, employing a combination of advanced fibre optic technology and new mid-infrared materials to create a completely fibre-integrated source suitable for wide deployment in non-specialist laboratories and clinics. The fPIRL platform will be employed as an ultra-precise laser scalpel, removing minute volumes of tissue for subsequent analysis with mass spectrometry. The tool will be much less destructive and much more precise than existing techniques. The team assembled crosses industry and academia, including materials scientists, laser physicists, analytical chemists, and systems medicine specialists. Together, we will enable significant advances in various biomolecular analysis techniques. The proposed single-cell resolution molecular mapping setup will help drive improvements in cancer tumour removal surgeries. Our fibre-delivered source will underpin future robotic surgical interventions in hard-to-reach surgical sites. With our long-wavelength source (6 um) we aim to reveal different biological fingerprints, improving diagnoses for certain diseases, than with existing ablation techniques. This project will create a new photonics-based healthcare technologies tool. The tool will enable significant advances in disease diagnosis and intervention, through advances in biomolecular analysis techniques suitable for both research and in-vivo applications. These advances will ultimately improve patient outcomes in the UK for the NHS, leading to a healthier, happier, and more productive society. Beyond this project, the fPIRL could be used for any precision surgical intervention, cultural preservation in ancient art, and polymer processing for biological implants.

Clouds formed by aircraft (contrails) are the most easily visible human forcing of the climate system. Trapping energy in the Earth system, they contribute more than half of the total climate impact of aviation. This makes reducing contrails an important goal to achieve the UK's climate commitments. Theoretical considerations indicate two pathways for reducing contrails. First, improving engine design to emit fewer particulates may reduce contrail lifetimes and so their climate impact. Second, rerouting aircraft to avoid contrail forming regions. Assessing these pathways requires accurate models of contrail formation, evaluated at the level of an individual aircraft. This evaluation requires observations of contrails across their lifetime, coupled to details of the generating aircraft. Even where they are matched to specific aircraft, existing observations typically view a contrail once, (limiting their use for measuring contrail lifecycles) or cannot provide the detail on the contrail microphysical properties (such as ice crystal number or shape) necessary to assess the efficacy of different pathways to contrail reduction. Improving confidence in our contrail models urgently requires novel observations of contrail properties and lifecycles from individual aircraft. The impact of aircraft on clouds is not limited to contrails forming in clear air. Over half of contrails form embedded in existing clouds and the particulates emitted by aircraft can affect cloud formation several days after they were released. These effects produce a cooling, potentially large enough to offset all other warming effects of aviation, but are not represented in aircraft-level models used for planning contrail avoidance strategies. There are few observational constraints of these effects, targeted observations of the impact of individual aircraft on cloud microphysics are required to assess them and to improve future model simulations. To address these uncertainties and around contrail formation, persistance and climate impact as well as aerosol-cloud interactions, COBALT has three core components: 1. A measurement campaign in the southern UK, combining an array of ground-based cameras with a steerable cloud radar, to make high resolution observations of contrail formation from individual aircraft. Guided by aircraft transponder information, these observations will be focused on contrails and clouds modified by aircraft, characterising contrail formation and perturbed cloud properties within the first few hours of their lifecycle. 2. Counterpart satellite observations, using novel techniques to characterise contrail and cloud development from an hour to several days behind the aircraft. Building on techniques for studying natural cirrus, this will produce a complete characterisation of the contrail lifecycle, along with the first estimate of the aviation aerosol impact on existing cirrus clouds at a global scale. 3. The complete lifecycle characterisation will be combined with flight data from aircraft operators to produce a unique dataset designed specifically for the evaluation of aircraft-level models of contrail formation. An initial focus will be placed on evaluating aircraft-scale models, as these are currently being used to plan aircraft diversions. A comparison of climate model parametrisations of contrail formation will assess the ability of the parametrisations to reproduce the wide-area (>1000km2) contrail observations taken by the camera array. Led by an inter-disciplinary team of scientists and engineers, with partners in key international research centres and industry groups, COBALT will provide the tools necessary to evaluate our current models and ability to avoid contrails, guiding future modelling and operational trials of sustainable fuels and contrail avoidance.

Complex multicellular life first appeared on Earth some 800 million years ago and subsequently diversified through a bewilderingly complex pattern of species originations/extinctions. However, this was not a steady and uninterrupted process. On at least five occasions the biota of the planet was devastated by a catastrophe that eliminated a considerable proportion of total biodiversity--including entire groups of organisms (higher taxa). These so-called 'mass extinctions' fundamentally changed the nature of life on Earth by steering evolution into a completely different trajectory. Of the 'Big Five' mass extinctions by far the least understood is the Devonian mass extinction that occurred ca.370 million years ago. There is widespread debate regarding both the timing and nature of this event, which has led to a complete lack of consensus regarding its causes. This proposal seeks to investigate the Devonian mass extinction from a fresh perspective focussing on changes in carbon-cycling. The Earth currently has two carbon-cycles of similar magnitude: a marine one based on photosynthetic plankton and a terrestrial one based on photosynthetic land plants. Fundamental changes in carbon-cycling took place during the Devonian due to dramatic changes in the nature of terrestrial vegetation. At the start of the Devonian land plants were centimetres tall, rooted in very shallow soils and covered a limited area of the continents. By the end of the Devonian vast swathes of the continents were shrouded in forests of trees tens of metres tall that deep-rooted into mature soils. These major vegetation changes caused profound changes in the terrestrial carbon-cycle (due to carbon sequestration from chemical weathering and biomass burial). We hypothesise that it was dramatic changes to the terrestrial carbon-cycle that disrupted the Earth system and caused the Devonian mass extinction. However, we believe that it was not a single catastrophic event (such as the bolide impact that caused the end Cretaceous mass extinction) but rather it occurred sequentially as discrete morphological/anatomical innovations led to changes in plant size and coverage causing step-changes in the terrestrial carbon-cycle. The research project will focus on the Devonian sequences of northern Spain. These are ideal because they: (i) are remarkably complete and incorporate known extinction events at the Frasnian-Famennian and Devonian-Carboniferous boundaries; (ii) accumulated in isolation on a large microcontinent and as such are not influence by species immigration/emigration and habitat tracking; (iii) contain an excellent fossil record of both marine plankton (acritarchs and chitinozoans) and terrestrial vegetation (plant spores/pollen). We will study the evolutionary dynamics of both the marine plankton and terrestrial vegetation through a study of species origination/extinction patterns. This biodiversity profile will be integrated with geochemical analyses that will identify perturbations in the Earth's carbon-cycle (in addition to nutrient cycling, redox conditions and volcanic activity). These data will be fed into an Earth Systems model for the Devonian carbon-cycle that we generate using inverse modelling techniques. The model will also incorporate data on the appearance of major plant groups and novelties (e.g. first forests). Together these data will shed light on the nature and timing of Devonian extinction events among primary producers and link them to changes in the carbon-cycle. Our research will clarify many aspects of the Devonian mass extinction (nature and timing) and link it to the monumental changes in carbon-cycling brought about by the dramatic evolution of terrestrial vegetation. This will also serve as a warning for the present day regarding consequences of human induced changes to the Earth's carbon-cycle bought about by deforestation, soil erosion and other detrimental activities.