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Climate change has been widely recognised as one of the most urgent and growing threats to natural and cultural heritage in the twenty-first century, and the indelible impact of humanity has led to the definition of a new geological epoch, the Anthropocene. Indigenous peoples are disproportionately affected by natural and human-induced changes to the environment. Their vulnerability is exacerbated by centuries of cultural and territorial disenfranchisement within settler-colonial nations. This dissertation aims at understanding Indigenous perceptions of heritage in the face of climate change and its intersection with the impacts of settler- colonialism. It analyses how these on-the-ground perceptions can, in turn, inform heritage organisations and contribute to safeguarding the many facets of tangible and intangible Indigenous heritage for future generations in the Anthropocene. This is accomplished through a comparative, transnational case study of two communities each from the Dehcho First Nations in the Northwest Territories, Canada, and the Aymara and Quechua peoples in northern Chile. I use a multi-method approach consisting of semi-structured interviews, oral histories and participant observation. The data is complemented by environmental and heritage legislation and grey literature at multiple organisational scales for both case studies. Three lines of enquiry are explored through an applied comparative thematic analysis: i) the perceptions of climate change and associated land loss/change among Indigenous groups and how this impacts each group’s notions of challenges to its cultural identity; ii) the intersection of the effects of post- colonialism, ongoing industrial activities and climate change on the intergenerational transmission of ancestral knowledge and notions of place attachment; and iii) how international, national and regional political and sociocultural rhetoric on environmental and heritage conservation affect local, grassroots considerations for safeguarding heritage. The similarities and contrasts of the Dehcho First Nations, Aymara and Quechua experiences of climate change across the North-South divide are related from the grassroots to arrive at redefining heritage practices in the Anthropocene. The results demonstrate that decolonising heritage is not only necessary, but that this decolonisation depends on building and actively engaging in intercultural empathy through the global threat of climate change. In order to understand how Indigenous practices, places, and items are valorised—attributed value—as heritage in the face of climate change, one must empathise with the cultural loss that exists in the temporal and cognitive spaces between Indigenous individuals’ moments of nostalgic reference and today.

Achievement of sustainable development in light of ongoing climate change and biodiversity pressures benefits from the deployment of innovations that foster engagement and uptake across all levels, mobilises finance flows commencement to the scale of the challenge, and enables the dissemination of transition solutions that support the low carbon economy. This research investigates the relationship between the legal architecture of market mechanisms under international law and the role of private actors, and how this contributes to sustainable development. Through an exploration of how market mechanisms under the climate change and biodiversity regimes have achieved environmentally sound outcomes, been advanced in sectoral approaches, and facilitated via bilateral and multilateral trade and investment relationships, important insights are identified regarding the composition of effective law and governance architectural approaches. Leveraging experiences derived from treaty practice viewed through an interactional account of international law, this assessment elucidates the important role played by alignment of legal regimes, robust transparency measures, and complementary schemes such as stakeholder-endorsed certifications in buttressing the established measures to ensure sustainable development outcomes and contributes to understanding the role of private actors in the operationalisation of environmental agreements. Research findings suggest it is the interaction of norms across the international legal architecture, informed by relationships within and across relevant treaty systems and the general corpus of international law, and actualised through engagement with private actors as a component of market mechanisms that provides the opportunity for congruence of practice, forging of shared understandings, and normative internalisation and ownership among communities of practice that stimulates both innovative solutions and ambitious action.

Halide perovskites are the leading candidates for next-generation, low-cost optoelectronics with power conversion efficiencies well above 25%. However, operational stability remains a key challenge. Although there is an understanding that the microscale and nanoscale play a consequential role in determining the macroscopic performance and stability, significant gaps remain in the mechanistic understanding of degradation processes at the nanoscale and the mechanisms for stability in cation-alloyed systems. Nanoscale hexagonal phase impurities have been identified as problematic for operational stability, leading to both performance losses and morphological degradation. However, it is still unclear at what stage these phase impurities originate. Understanding this better is critical in order to mitigate the harmful effects of these phase impurities on performance and operational stability. Cation alloying is a commonly used technique in the field to mitigate these hexagonal phase impurities, although not without its challenges. In this thesis study, the nanoscale structural landscape of key halide perovskite compositions is studied. By taking snapshots of the perovskite at different states of the annealing process, the impact of phase impurities on device performance is characterised. Thereon, the mechanism by which composition dictates photostability in FA-rich perovskite absorber layers is studied. It is demonstrated that the composition impacts the degree of octahedral tilt, which is essential to restricting the transition to hexagonal phase impurities. Additionally, it is demonstrated that while a judicious mix of A-site cations can be used to stabilise the photoactive black phase of halide perovskites, it is challenging to achieve this homogeneously over large areas, necessitating a search for alternative or complementary approaches to stabilise perovskite via octahedral tilt. Using scanning electron diffraction (SED) studies, the spacegroup of additive-stabilised-CsPbI3 is demonstrated to be a low symmetry tilted γ-phase. Furthermore, using SED, the nanoscale structural landscape of mixed-phase CsPbI3 absorber layers is studied and it is demonstrated that both narrow-bandgap γ-phase and wide-bandgap δ-phase co-exist at the nanoscale, enabling stable and bright white-light emission. Overall, this thesis provides insights into the role of nanoscale structure in dictating the properties and behaviour of halide perovskites and offers rational guidelines for their optimisation and use in optoelectronic devices. Additionally, it is demonstrated that SED is a powerful tool for studying these materials at the atomic scale, allowing for the detailed characterisation of their structures and properties.

Formate production via both CO2 reduction and cellulose oxidation in a solar-driven process is achieved by a semiartificial biohybrid photocatalyst consisting of immobilized formate dehydrogenase on titanium dioxide (TiO2|FDH) producing up to 1.16±0.04 mmolformate gTiO2-1 in 24 hours. Isotopic labelling experiments with 13C-labelled substrates support the mechanism of stoichiometric formate formation through both redox half-reactions. TiO2|FDH was further immobilized on hollow glass microspheres to perform more practical floating photoreforming allowing vertical solar light illumination with optimal light exposure of the photocatalyst to real sunlight. Enzymatic cellulose depolymerization coupled to the floating photoreforming catalyst generates 0.36±0.04 mmolformate mirr-2 after 24 h. This work thus presents simultaneous solar-driven valorization of waste streams, demonstrates the advantages of biohybrid photocatalysts in photoreforming for the first time and will provide inspiration for the development of future semi-artificial waste-to-chemical conversion strategies.

To meet the increasing demand for sustainable products, one can look to nature to scout new functional materials. For instance, the most brilliant and striking colours in plants are obtained using cellulose nanofibrils organised in helicoidal architectures. Interestingly, similar helicoidal architectures with analogous optical response can be obtained in vitro by self-assembly of cellulose nanocrystals (CNCs). CNCs are rod-like colloids capable of arranging into a liquid crystalline phase above a critical concentration in suspension. So far, the process that governs the self-assembly of CNCs into photonic structures was studied only at small scale. This neglects the limitations and challenges posed by large-scale and continuous processes which are prevalent in industrial contexts. In this thesis, I demonstrate how the self-assembly of CNCs can be precisely controlled to produce meters-long films using a roll-to-roll (R2R) equipment. Starting with commercially available material, the preparation of CNC suspension was optimised for R2R deposition to produce films with vibrant photonic colour across the visible range. Particularly, I discuss how the suspension properties, the casting parameters and drying time relate to the optical properties of the produced films. To validate the use of such materials for pigment preparation, I develop a protocol to produce a series of coloured microparticles from R2R-cast CNC films. The optical properties of the CNC microparticles were then assessed in various environment and finally benchmarked against other commercial effect pigments and glitters.

Over the past decade, lead-halide perovskites (LHPs) have demonstrated significant potential in terms of their performance across a wide range of optoelectronic devices, including solar cells, photodetectors and light-emitting diodes. However, the toxicity of lead and instability issue of LHPs are still concerns for their widespread implementation. These successes, but also the challenges of LHPs have motivated great efforts across multiple disciplines to search for lead-free and stable alternatives that can have similar optoelectronic properties to LHPs, namely ‘perovskite-inspired materials (PIMs)’. With the deeper understanding of defect tolerance displayed in LHPs, a large number of PIMs have been identified until now. Among all the identified PIMs, ternary chalcogenides or ABZ2 materials, are believed to be one of the most promising alternatives so far, owing to their simple fabrication protocols, strong absorption and high stability in air. Particularly, AgBiS2 solar cells have demonstrated the highest efficiency (9.17%) among all bismuth-based solar cells. Nevertheless, studies into ternary chalcogenides are mostly limited to AgBiS2 photovoltaics, and the investigations into other potential ABZ2 materials or broader applications are rare so far. Therefore, this thesis will aim to investigate the optoelectronic properties of another promising while rarely investigated ABZ2 material – NaBiS2, and also the potential of AgBiS2 as near-infrared (NIR) photodetectors. In the first project of this thesis, NaBiS2 nanocrystals (NCs) have been shown to exhibit extremely strong absorption, along with a comparatively sharp absorption onset. However, optical-pump-terahertz-probe (OPTP) measurements indicated that most free charge-carriers in NaBiS2 NCs will be localised within a few picoseconds. These localised charge-carriers only exhibited low mobility of around 0.03 cm2 V-1 s-1 and could not transport effectively even though they might be rather long-lived in NaBiS2 and unaffected by intentionally-introduced defects. With help from density functional theory (DFT) calculations, all of these unusual characteristics in NaBiS2 have been shown to closely associate with intrinsic cation disorder, which was also observed in AgBiS2. Although post-annealing is effective for improving cation inhomogeneity and enhancing absorption in AgBiS2, its effect on NaBiS2 was found to be rather minor, which also indicated that the charge-carrier localisation process in NaBiS2 could not be significantly mitigated after annealing. Based on the fundamental insights acquired in the first project, the possibility of further improving charge-carrier transport in NaBiS2 NCs through ligand exchange treatment was investigated in my second project. Using a variety of correlated spectroscopic characterisation techniques, I found that NaBiS2 NCs treated by inorganic iodide ligands had enhanced sum mobility and surface photovoltage (SPV) signals, which implies an improvement in the macroscopic charge-carrier transport. However, the ultrafast localisation process was still observed in these iodide-treated NaBiS2 NCs, suggesting that their cation disorder was not greatly changed. At the same time, the defect capture rates were also found to be lower in the iodide-treated NaBiS2 NCs based on my two proposed models for describing charge-carrier dynamics. As a result, solar cells based on these iodide-treated NaBiS2 NCs could exhibit a peak external quantum efficiency (EQE) value over 50%, along with a power conversion efficiency exceeding 0.7%. Although this is an order of magnitude larger than previous reports, I found ion migration to be a limiting factor for NaBiS2 devices from temperature-dependent transient current measurements, where a low activation energy of only 88 meV was extracted. In my third project, AgBiS2 photodetectors were fabricated and characterised in depth. Aside from the broadband photo-response across from ultra-violet (UV) to near-infrared (NIR) region, AgBiS2 photodetectors have demonstrated an extremely high cut-off frequency (f-3dB) on MHz order, indicating their great potential in applications requiring fast device response such as optical communications. The mechanism behind this fast response was studied, and a relatively long drift length compared to the AgBiS2 film thickness is believed to be the key reason. Similar to NaBiS2 devices, ion migration was also found easy in AgBiS2 devices with an activation energy of 124 meV, which could lead to their increasing noise currents with time. Importantly, these noise currents could be also effectively suppressed when optimising the AgBiS2 film thickness, in which a balance between large shunt resistant and cumulative quantity of defects should be reached. Finally, owing to the small bandgap of AgBiS2 NCs (~1.2 eV), AgBiS2 photodetectors could effectively monitor the heartbeat rates by probing the transmission change of blood vessels illuminated by NIR light, which has been widely used in the medical field owing to its deeper penetration in tissues. These three projects not only uncovered several remarkable optoelectronic characteristics of ABZ2 materials, but also investigated possible methods to further alter these characteristics. Although ABZ2 materials have shown great potential as light harvesters, it can be seen that both cation disorder (or charge-carrier localisation) and ion migration are still limiting the performance. More studies on the root causes of both phenomena, and how to effectively suppress their effects on the materials, would be hence crucial in the future work. With more understandings on this material class, we could expect more efficient, stable, and cleaner optoelectronic devices to be realised in the future.

AbstractMountain treelines are thought to be sensitive to climate change. However, how climate impacts mountain treelines is not yet fully understood as treelines may also be affected by other human activities. Here, we focus on “closed‐loop” mountain treelines (CLMT) that completely encircle a mountain and are less likely to have been influenced by human land‐use change. We detect a total length of ~916,425 km of CLMT across 243 mountain ranges globally and reveal a bimodal latitudinal distribution of treeline elevations with higher treeline elevations occurring at greater distances from the coast. Spatially, we find that temperature is the main climatic driver of treeline elevation in boreal and tropical regions, whereas precipitation drives CLMT position in temperate zones. Temporally, we show that 70% of CLMT have moved upward, with a mean shift rate of 1.2 m/year over the first decade of the 21st century. CLMT are shifting fastest in the tropics (mean of 3.1 m/year), but with greater variability. Our work provides a new mountain treeline database that isolates climate impacts from other anthropogenic pressures, and has important implications for biodiversity, natural resources, and ecosystem adaptation in a changing climate.

Over the past several years, online disinformation and misinformation concerning climate change have gained substantive attention within the scientific community. However, while the dynamics that drive the circulation of false online information have been analysed extensively, it remains unclear whether (and how) this phenomenon can be counteracted. This research project analyses the emerging role of bottom-up mobilisations as a form of noise-reduction, thereby examining how social movements may deploy peer-produced communication narra- tives to counteract the circulation of online disinformation and misinformation relating to climate change. To investigate this communication dynamic, this research applies techniques from computational social sciences to an original dataset of ≈ 250k Facebook posts produced by two movements that best embody this novel and innovative generation of radical envi- ronmental activism: Extinction Rebellion and Fridays for Future. The central thesis of this project forwards two original contributions to the fields of climate change communication and social movement studies. First, it analyses the emergence of a new generation of radical climate change movements and the significance of this new development in climate activism (Chapter II). Second, it offers interdisciplinary empirical evidence on how radical climate movements can act as a bottom-up force for what I term ‘epistemic activism’. It presents a theoretical framework where activist-led, peer-produced communication can provide a coun- tering force to both vertical disinformation and horizontal misinformation. It quantitatively analyses two channels through which these forms of false information can be opposed. For reducing vertical disinformation, this work assesses the use of naming and shaming against information polluters (Chapter III), while for horizontal misinformation, it evaluates the dissemination of scientific counter-narratives (Chapter IV). Ultimately, this thesis shows that the two movements under analysis engage extensively in epistemic activism, with great potential to influence the online climate change debate positively.

In recent decades, many societal changes have unfolded, including population ageing, reconfigurations of household structures, labour market transformation, and a secular deceleration of economic growth. These shifts pose considerable challenges to preexisting welfare states, particularly to the efficacy of countries’ pension systems. This dissertation examines the context and trajectory of pension reforms in Mexico, the United Kingdom, and the United States. Its contribution is to ascertain the viability and political feasibility of reforms that enhance the financial sustainability of their pension systems, while maintaining adequate income and coverage levels. The dissertation builds on political economy approaches and on the institutionalist literature, which highlight how the role of interest groups and structure of institutions and political systems shape policy outcomes. The frameworks of blame avoidance and credit-claiming are also considered, to provide a comprehensive analysis of the complex dynamics surrounding pension systems and reform efforts. This dissertation uses a mixed-methods approach – including public opinion surveys of 3,000+ individuals, semi-structured elite interviews, historical document analyses, and specialized fiscal and actuarial projections of selected pension reforms in the three selected countries. It addresses three core research questions: 1) What is the current context for pension reform in Mexico, the United Kingdom, and the United States given their histories? 2) Is the necessary (for achieving specific minimum levels of sustainability, adequacy, and coverage) pension reform politically feasible? 3) How do the characteristics of each reform affect its political feasibility? Corollary: The modification of which channel (benefits, contributions, retirement age) is perceived as more politically feasible for diverse stakeholders? The methodology chosen provides a timely picture of the context surrounding potential pension reforms in the three case studies. In Mexico, credit-claiming and the interests of private stakeholders explain the success of recent pension reforms, and partisan politics are the key determinants for future fiscal changes. For the United Kingdom, the institutionalist literature helps explain the reasons for the relatively easier reform avenues; the most politically feasible reforms are those in the private sector, while the housing market is of key importance for pensions. In the United States, the institutionalist literature and the framework of blame avoidance also help explain the current legislative gridlock and the reasons why no major reform has been enacted for decades. For Mexico and the United Kingdom there exist politically feasible reforms, notably a modification of the retirement age channel, that can increase the system’s sustainability while maintaining income adequacy and coverage; whereas based on the current context of extreme polarisation and legislative gridlock, there do not seem to exist politically feasible pension reforms that preserve the structure of Social Security in the United States. The dissertation brings the lens of political feasibility to bear on a previously technical literature on the structure of the pension systems in the three countries, and thus on the feasibility of reform to deliver financial sustainability, adequacy of retirement incomes, and adequate coverage of the old age population. It identifies the feasible routes for reform in Mexico and the United Kingdom, but concludes that the political economy context the United States has reached rules out feasible reforms of its current pension structures.