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• Speaker: Iddo Tzamaret (Imperial)
• Tuesday 11 March 2025, 14:00-15:00
• Venue: Computer Laboratory, William Gates Building, Room SS03.
• Series: Algorithms and Complexity Seminar; organiser: Tom Gur.

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Ice shelves buttress the grounded ice sheet, restraining its flow into the ocean. Mass loss from these ice shelves occurs primarily through ocean-induced basal melting, with the highest melt rates occurring in regions that host basal channels – elongated, kilometre-wide zones of relatively thin ice. While some models suggest that basal channels could mitigate overall ice shelf melt rates, channels have also been linked to basal and surface crevassing, leaving their cumulative impact on ice-shelf stability uncertain. Due to their relatively small spatial scale and the limitations of previous satellite datasets, our understanding of how channelised melting evolves over time remains limited. In this study, we present a novel approach that uses CryoSat-2 radar altimetry data to calculate ice shelf basal melt rates, demonstrated here as a case study over Pine Island Glacier (PIG) ice shelf. Our method generates monthly Digital Elevation Models (DEMs) and melt maps with a 250 m spatial resolution. The data show that near the grounding line, basal melting preferentially melts a channel’s western flank 50% more than its eastern flank. Additionally, we find that the main channelised geometries on PIG are inherited upstream of the grounding line and play a role in forming ice shelf pinning points. These observations highlight the importance of channels under ice shelves, emphasising the need to investigate them further and consider their impacts on observations and models that do not resolve them.

• Speaker: Katie Lowry, British Antarctic Survey
• Wednesday 12 March 2025, 14:00-15:00
• Venue: BAS Seminar Room 2.
• Series: British Antarctic Survey - Polar Oceans seminar series; organiser: Dr Birgit Rogalla.

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Causal set theory is an approach to quantum gravity in which spacetime is fundamentally discrete at the Planck scale. In this theory, spacetime takes the form of a random Lorentzian lattice known as a “causal set”. In this talk, I will describe recent developments in defining interacting scalar quantum field theories on this novel background. I will present diagrammatic rules for computing in-in correlators; these rules are manifestly causal thanks to the appearance of the retarded propagator. This framework is a step towards new quantum gravity phenomenology, since it enables the computation of early universe observables under the assumption that spacetime is fundamentally discrete.

• Speaker: Stav Zalel, University of Cambridge
• Friday 28 February 2025, 13:00-14:00
• Venue: Potter room/Zoom: https://cam-ac-uk.zoom.us/j/83177386172?pwd=WMMBb4K7LVPuZZZKAWyvDkKoQp711S.1.
• Series: DAMTP Friday GR Seminar; organiser: Xi Tong.

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Abstract not available

• Speaker: Sam Clarke, IEEF
• Thursday 06 March 2025, 11:30-12:30
• Venue: Open Plan Area, Institute for Energy and Environmental Flows, Madingley Rise CB3 0EZ.
• Series: Institute for Energy and Environmental Flows (IEEF); organiser: Catherine Pearson.

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Reducing reliance on fossil carbon is central to the concepts of sustainable development and material stewardship. Whereas decarbonization of the energy sector is feasible through the development of renewable energy, the chemicals sector needs carbon as a building block. The lasting and growing demand for this embedded carbon, especially for production of polymers, must be met in the future through utilization of renewable feedstocks such as biomass, CO2 and recycling of carbon-containing waste. In this context, the transition from fossil to renewable polymers provides a major challenge. Advances in renewable polymers will be exemplified through case studies of two of the most promising bio-based platforms for plastics: lactic acid (LA) and hydroxymethylfurfural (HMF).

• Speaker: Professor Matthew Davidson, Bath Institute of Sustainability and Climate Change
• Thursday 27 February 2025, 11:30-12:30
• Venue: Open Plan Area, Institute for Energy and Environmental Flows, Madingley Rise CB3 0EZ.
• Series: Institute for Energy and Environmental Flows (IEEF); organiser: Catherine Pearson.

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Foundation Model and Generative AI are among the most promising topics nowadays. However, their rapid developments also raise a series of critical challenges on responsibility such as privacy, security and Intellectual property (IP). In this talk, I will touch on the relevant risks and how we are championing the responsible development of Foundation Model and Generative AI, including using Federated Learning to empower the training/fine-tuning/adaptation of foundation models without touching on the original data; training models on public and synthetic data only; strategies to detect and address the unauthorized data usage, training data memorization, and IP infringements, ensuring compliance and trust.

Bio: Dr. Lingjuan Lyu is currently leading the privacy-preserving machine learning and vision foundation model team in Sony Research. Her main research interests include the low-cost foundation model and generative AI model development, responsible AI, and federated learning. She has won a series of awards, including AI 10 to Watch, IJCAI Early Career Spotlight, IEEE Outstanding Leadership Award, IBM Ph.D. Fellowship, National Scholarship, and Best/Outstanding/Oral/Spotlight paper awards or recognitions from top venues like ICML , ACL, CIKM , NeurIPS, AAAI , IJCAI, WWW , and KDD . She also served as a chair, committee member, or organizer of top conferences including her recent role as a chair for NeurIPS’24 Datasets and Benchmarks.

• Speaker: Dr. Lingjuan Lyu
• Tuesday 25 February 2025, 16:05-17:00
• Venue: Computer Lab, LT2.
• Series: Cambridge ML Systems Seminar Series; organiser: Sally Matthews.

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A facile and general strategy is developed to prepare conjugated coordination polymer aerogels (denoted as M-CCPA, M = Ni, Cu, Zn, etc.) that can markedly increase the accessibility of their well-defined single-atom metal sites within their hierarchically porous structures with mesopores and nanopores, which can provide a wide space for the design of high-performance catalysts toward various energy-conversion systems.

Developing high-performance single-atom catalysts (SACs) with maximum metal utilization efficiency is of significance, which presents enormous potentials to be extensively applied. It is desired yet challenging to elaborately tailor the coordination structures of active sites in SACs and simultaneously enable sufficient accessibility of these active sites to reactants. Here, a facile and general strategy to prepare conjugated coordination polymer aerogels (CCPA) with porous architectures that can markedly increase the accessibility of their elaborately-tailored active sites, which as a new electrocatalyst paradigm can fully present both the structural advantages of SACs and aerogel materials, is reported. Taking nickel (Ni) as an example, Ni-based CCPA (Ni-CCPA) and its counterpart Ni-CCP with non-aerogel feature are studied as a proof-of-concept case. Electrochemical measurements show that, relative to Ni-CCP, Ni-CCPA exhibits appreciably higher performance toward alkaline oxygen evolution reaction (OER). Both the experimental results and theoretical simulations unravel that the improved OER performance of Ni-CCPA arises from the accelerated OH− diffusion within its porous architecture and enhanced OH− concentration near its highly exposed active sites at its high-curvature surfaces with localized electric fields. Importantly, as evidenced by the Cu-CCPA and Zn-CCPA examples, such strategy can be promisingly applied to prepare high-performance CCPA targeted toward various catalytic reactions and beyond.

GO naturally adsorbs onto the surface of LMPs via electrostatic interactions, self-assembles into a core–shell structure, and subsequently reduces to RGO in an acidic solution. The presence of RGO in the hierarchical structural composites significantly improves the electrode-electrolyte interface, suppressing and accommodating the irregular deformation of LMPs during the electrochemical reaction process and promoting the formation of a stable SEI film.

Gallium-based liquid metal (LM) has emerged as a promising candidate anode material for lithium-ion batteries (LIBs), exhibiting high theoretical capacity, excellent electrode kinetics, and unique self-healing ability. However, the liquid-solid-liquid transition during the electrochemical reactions can disrupt the solid electrolyte interphase (SEI) and damage the structural integrity, ultimately limiting the cycling stability. Here, hierarchical-structured reduced graphene oxide coated eutectic gallium-indium liquid metal particles (RGO@EGaIn LMPs) are synthesized using a facile self-assembly strategy. The customized RGO@EGaIn electrode demonstrated impressive performance in both half-cell and full-cell configurations for LIBs. The morphological and phase transitions of RGO@EGaIn LMPs during the lithiation/delithiation processes are uncovered by real-time in situ transmission electron microscopy tests. It is clarified that the presence of RGO in the hierarchical structure buffers the volume expansion of LMPs from ≈160% to 125% and provides a fast pathway for the rapid transfer of ions and electrons during the electrochemical reaction, which effectively enhances the electrochemical performance of the electrode. This work introduces a straightforward and effective method for preparing high-performance room-temperature liquid metal electrodes, representing a significant step forward toward the commercial application of liquid metal batteries.

Ni3S4/ZnCdS heterojunction is prepared for the efficient production of H2 and high-selectivity value-added chemicals from waste plastic. The catalyst exhibits high H2 production rates of 27.9 and 17.4 mmol g−1 h−1, along with selectivities of 94.2% and 78.3% in the liquid product toward pyruvate and acetate production from PLA and PET, respectively.

The oxidative degradation of plastics in conjunction with the production of clean hydrogen (H2) represents a significant challenge. Herein, a Ni3S4/ZnCdS heterojunction is rationally synthesized and employed for the efficient production of H2 and high-selectivity value-added chemicals from waste plastic. By integrating spectroscopic analysis techniques with density functional theory (DFT) calculations, a solely electron transfer-mediated reaction mechanism is confirmed, wherein Ni3S4 extracts electrons from ZnCdS (ZCS) to promote the spatial segregation of photogenerated electrons and holes, which not only facilitates H2 production but also maintains the high oxidation potential of holes on the ZCS surface, favoring hole-dominated plastic oxidation. Notably, the catalyst exhibited efficient H2 production rates as high as 27.9 and 17.4 mmol g−1 h−1, along with a selectivity of 94.2% and 78.3% in the liquid product toward pyruvate and acetate production from polylactic acid (PLA) and polyethylene terephthalate (PET), respectively. Additionally, carbon yields of 26.5% for pyruvate and 2.2% for acetate are measured after 9 h of photoreforming, representing the highest values reported to date. Overall, this research presents a promising approach for converting plastic waste into H2 fuel and high-selectivity valuable chemical products, offering a potential solution to the growing issue of “White Pollution”.

2D polymeric C60 is an emerging all-carbon semiconductor possessing unique hierarchical electronic structures. A hydrogen-assisted electrochemical strategy has been developed to produce gram-scale large size (≈52.5 µm2) and monolayer thick 2D polymeric C60 with high exfoliation yield (≈83%). The thin-film photodetectors demonstrate broad spectral response from visible light to near-infrared region.

2D polymeric fullerene scaffolds, composed of covalently bonded superatomic C60 nanoclusters, are emerging semiconductors possessing unique hierarchical electronic structures. Hitherto their synthesis has relied on complex and time-consuming reactions, thereby hindering scalable production and limiting the technological relevance. Here, the study demonstrates a facile electrochemical exfoliation strategy based on the intercalation and expansion of a layered fullerene superlattice, to produce large size (≈52.5 µm2) and monolayer thick 2D polymeric C60 with high exfoliation yield (≈83%). In situ reduction of solvated protons (H+) weakens the interlayer interactions thereby promoting the rapid and uniform intercalation of tetra-n-butylammonium (TBA+), ensuring gram-scale throughput and high structural integrity of exfoliated 2D polymeric C60. As a proof of concept, the solution-processed 2D polymeric C60 nanosheets have been integrated into thin-film photodetectors, exhibiting a broad spectral photoresponse ranging from 405 to 1200 nm, with a peak photocurrent at 850 nm and a stable response time. This efficient and scalable exfoliation method holds great promise for the advancement of multifunctional composites and optoelectronic devices based on 2D polymeric C60.

An in situ polymerizable radical molecule (ATEMPO) preferentially interacting with the {111}c facets, is employed as an additive to promote perovskite crystal growth. During annealing, ATEMPO polymerizes, forming a network-buffer that mitigates lattice strain and suppresses intragrain planar defects. This strategy yields high-quality perovskite films, achieving a champion PCE of 25.28% with a remarkably high V OC of 1.203 V, minimizing photovoltage loss in FAPbI₃ perovskite solar cells.

Formamidinium lead iodide (FAPbI₃) perovskite solar cells (PSCs) hold immense potential for high-efficiency photovoltaics, but maximizing their open-circuit voltage (V OC) remains challenging. Targeting the inherently stable {111}c-dominant facets is a promising approach for enhancing stability, but their formation typically suffers from high defect densities and disordered growth. This study introduces a novel approach using an in situ polymerizable radical molecule, ATEMPO, as an additive to address these issues. ATEMPO preferentially interacts with the {111}c perovskite facets, guiding their growth and forming a “radical molecular network-buffer” upon polymerization. The network effectively mitigates lattice strain, suppresses defect formation, enhances charge transport via redox-mediated hopping, and provides a hydrophobic barrier, significantly improving moisture resistance. This strategy yields high-quality, {111}c -oriented FAPbI₃ films, leading to a champion PCE of 25.28% with a remarkably high V OC of 1.203 V, corresponding to an energy loss (E loss) of only 0.297 eV, among the highest V OC reported for FAPbI₃-based PSCs. Furthermore, a mini-module fabricate with an active area of 12.5 cm2 achieve a high PCE of 21.39%. the work paves the way for developing high-performance, stable PSCs with minimized photovoltage loss. Furthermore, it offers a promising strategy to enhance device longevity and address environmental concerns.

Induced pluripotent stem cell membrane is coated onto adjuvant-loaded nanoparticle cores to create a universal cancer vaccine. The formulation utilizes oncofetal antigens present on the cell membrane to elicit broadly protective immune responses in vivo. The enhanced immunity generated by the nanovaccine enables robust prophylactic efficacy against multiple murine tumor models.

Cancer vaccines are a promising immunotherapeutic modality that function by training the immune system to recognize and destroy malignant cells. As tumor-specific and tumor-associated antigens generally cannot be identified until after a tumor has already been established, these vaccines must be applied therapeutically when strong immunosuppressive mechanisms are already in place. Building upon previous work using cell membrane coating nanotechnology, the development of a broad-spectrum prophylactic cancer nanovaccine that consists of induced pluripotent stem cell (iPSC) membrane coated around an adjuvant-loaded nanoparticle core is shown. The resulting nanostructure is capable of presenting iPSC-derived oncofetal antigens, which are oftentimes re-expressed on cancer cells but lowly present on normal adult tissues. When administered in vivo, the iPSC membrane-coated nanoparticles are highly immunostimulatory and elicit strong antitumor immunity that can successfully inhibit the growth of multiple tumor types, including five different murine tumor models and in a bilaterial heterogeneous tumor model. Overall, this work demonstrates an effective approach for engineering iPSC-based nanovaccines that can be applied broadly to prevent cancer before it occurs.

A novel single-atom Ru anchor on BaCe0.125Fe0.875O3−δ (BCF) perovskite, develope via a scalable solid-state approach, forms a distinctive 4-coordinate Ru–O–Fe configuration that induces reverse hydrogen spillover and promotes proton-involved oxygen reduction. The optimized 2Ru-BCF (2 wt.% Ru) cathode based fuel cell delivers an excellent peak power density of 1.78 W cm−2 at 700 °C with stable operation for 200 h.

Protonic ceramic fuel cells (PCFCs) offer a promising avenue for sustainable energy conversion, however, their commercial potential is hindered by sluggish proton-involved oxygen reduction reaction (P-ORR) kinetics and inadequate durability of cathode materials. Here, a novel single-atom Ru anchor on BaCe0.125Fe0.875O3−δ (BCF) perovskite, synthesized by a facile and scalable solid-state approach, as a potential cathode for PCFCs is reported. Theoretical and experimental analyses demonstrate that the single-atom Ru on BCF, characterized by a unique 4-coordinate Ru-O-Fe configuration, not only induces reverse hydrogen spillover but also acts as an active site for P-ORR. The application of the optimized 2Ru-BCF (2 wt.% Ru) cathode in a single cell delivers an exceptional peak power density of 1.78 W cm−2 at 700 °C, along with excellent operational stability over 200 h. These findings provide new insights into single-atom engineering, advancing the commercial viability of PCFCs.

This review explores how in situ and operando spectroscopic techniques reveal the real-time behavior of reticular materials, including MOFs and COFs. These methods track material formation and functionalization, structural changes, defect formation, dynamic responses to external triggers, and catalytic processes. Key findings and future opportunities are highlighted, offering pathways to enhance the design and functionality of these materials.

The application of in situ and operando spectroscopic techniques has significantly advanced the understanding of reticular materials, particularly metal–organic frameworks (MOFs) and covalent organic frameworks (COFs). These techniques offer real-time insights into the dynamic structural, electronic, and chemical changes that occur within these materials during various processes, such as catalysis, sorption, and material synthesis. This review offers a comprehensive overview of key in situ and operando techniques used to investigate the formation, functionalization, and catalytic behavior of reticular materials. How these techniques have elucidated the roles of active sites, reaction intermediates, and structural transformations under reaction conditions, especially in single-site catalysis, electrocatalysis, and photocatalysis, is highlighted. The review also discusses the challenges and opportunities that lie ahead in integrating advanced spectroscopic methods with reticular materials, aiming to foster further innovation in the design and application of these versatile materials.

An organic gradient homojunction design via rational donor–acceptor engineering is proposed to establish a new class of full-spectrum responsive polymer homojunction photoelectrode for solar-coupled seawater-electrolyte-based metal-air flow batteries with improved solar utilization and device energy efficiency even at lower temperatures, by exploring photoelectric/photothermal dual-assisted bidirectional oxygen catalysis.

Coupling solar into metal-air batteries represents an appealing paradigm for storing intermittent solar energy and boosting device energy efficiency. Current solar-coupled metal-air systems rely on UV or visible light harvesting and suffer from inferior charge separation ability and limited solar utilization. Additionally, sunlight action behavior/mechanism in some useful scenarios (seawater electrolytes, low-temperature) is underexplored. Herein, through gradient homojunction design via donor-acceptor (D-A) engineering, it exploits a novel full-spectrum-responsive polymer homojunction photoelectrode (PGH) for sunlight-coupled seawater-electrolyte-based Zn/Na-air batteries (Zn-SWAB/Na-SWAB) with boosted sunlight utilization and energy efficiency at lower temperatures. By stacking three pre-designed analogous [A1-D1]m-[A1-D2]n copolymers with gradient energy-levels and rich heterocycles, PGH integrates separate metal-free active sites for oxygen reduction/evolution reaction (ORR/OER), efficient photothermal effect with full-spectrum-absorption, and superior photoelectric effect with high charge-separation efficiency. Thus, PGH under simulated-sunlight produces remarkably-enhanced photocurrent up to 3.2 and 21.4 times during ORR/OER in near-neutral electrolytes. This endows sunlight-coupled PGH-enabled Zn-SWAB and Na-SWAB with low voltage gaps of 0.08/0.25 V at room temperature, and 0.21/0.43 V at 0 °C – both of which surpass most reported room-temperature results. Their energy efficiencies (84.6%/86.8%) at 0 °C even approach their room-temperature counterparts (93.9%/92.3%). Mechanistic studies reveal photoelectric/photothermal dual-promoted bidirectional oxygen catalysis responsible for intriguing performance.

A water-soluble Pt(II) pincer complex probe is proposed to achieve the direct recognition of anionic [UO2(CO3)3]4− using a new strategy where the overlapping of thick hydration shells drives an assembly. This hydration-shell-promoted assembly endows the probe with excellent specificity, a rapid response, and high sensitivity (14.89 fg). This study paves the way for exploring new approaches for the direct detection of highly hydrated ions.

It is still challenging to directly recognize the anionic species [UO2(CO3)3]4−, the dominant species in the environment (82%-93%), using current optical probes because of the adverse effects of its thick hydration shell on binding interactions. In this study, a water-soluble Pt(II) methylated terpyridine complex ([Pt(CH3-tpy)NCO]+) supramolecular probe is designed to directly target [UO2(CO3)3]4− by a new strategy of thick hydration shell overlapping arrangement. The optical response demonstrates excellent selectivity among ≈30 investigated interfering substances, along with rapid response (≈15 s), high sensitivity (64.1 nm) and dual-signals. It is confirmed both experimentally and theoretically that the superior detection performance is attributed to the formation of a unique supramolecular structure featuring biplane-like building block, bicolumnar stacking and water-bridged anionic networks, via the overlap of thick hydration shells of aligned [UO2(CO3)3]4− to boost a superentropic driving force, and the distinguishable dual-signals arises from the emergence of four types of Pt-Pt interactions, generating low-energy metal-to-metal charge transfer adsorption/emission. In addition, a [Pt(CH3-tpy)NCO]+-based hydrogel platform is constructed for detecting both anionic and cationic uranium, with a detection limit of 14.89 fg. This work unlocks not only a way to directly detect [UO2(CO3)3]4−, but also a new idea for sensing ions with extreme thick hydration layers.

Point defects typically reduce thermal conductivity (κ) by scattering heat-carrying phonons. However, introducing spiro interstitials through particle irradiation in graphite surprisingly increases cross-plane κ from 10.8 to 18.9 W m K−1 at room temperature. The scanning transmission electron microscope and first-principles calculations reveal that these defects bridge graphene planes, increasing group velocity while reducing phonon-phonon scattering, thereby enhancing cross-plane κ of graphite.

Point defects typically reduce the thermal conductivity (κ) of a crystal due to increased scattering of heat-carrying phonons, a mechanism that is well understood and widely used to enhance or impede heat transfer in the material for different applications. Here an opposite effect is reported where the introduction of point defects in graphite with energetic particle irradiation increases its cross-plane κ by nearly a factor of two, from 10.8 to 18.9 W m K−1 at room temperature. Integrated differential phase contrast imaging with scanning transmission electron microscopy revealed the creation of spiro interstitials in graphite by the irradiation. The enhancement in κ is attributed to a remarkable mechanism that works to the benefit of phonon propagation in both the harmonic and anharmonic terms: these spiro interstitial defects covalently bridge neighboring basal planes, simultaneously enhancing acoustic phonon group velocity and reducing phonon–phonon scattering in the graphite structure. The enhancement of κ reveals an unconventional role of lattice defects in heat conduction, i.e., easing the propagation of heat-carrying phonons rather than impeding them in layered materials, inspiring their applications for thermal management in heavily radiative environments.

This study explores the potential applications of antiphase ferroelectric boundaries (APFBs) in PbTiO3 films due to the sharp, straight morphology and the interlocking feature between antiphase boundaries and 180° conventional domain walls. AFPBs retain a high degree of similarity to conventional domain walls, which may serve as dividers of domains and be used in promising strategy for miniaturizing ferroelectric devices.

The ferroelectric domain wall, serving as the boundary between separate data carriers based on domains, has attracted widespread interest due to its distinctive physical properties. Although the domain walls in ferroelectric materials are narrower than those in magnetic materials due to their higher lattice anisotropy, they still account for a considerable proportion in ultrathin films, reducing storage efficiency to some extent. Here, ultrathin antiphase ferroelectric boundaries (APFBs) are presented and validated their feasibility as ferroelectric domain walls. The naturally formed APFB shows a sharp and straight morphology, with the characteristic of interlocking between the antiphase boundary (APB) and conventional 180° domain wall. The calculations from the density functional theory demonstrate that the APFBs undergo a significant but localized change in electronic structure. They largely retain the characteristics that are consistent with those of conventional domain walls, such as enhanced conductivity, irregular oxygen vacancy trapping energy, and vacancy-tunable physical properties. Finally, as techniques for precisely controlling the nucleation of APB developing, configurations with out-of-plane APFBs used as dividers may provide a promising strategy for miniaturizing ferroelectric devices.

A twisted guest acceptor BTP-4Cl is introduced to fine-tune the solubility of host components to address the excessive aggregation issue in blade-coated processing. It is found that the twisted molecular conformation profited in inducing longer intermolecular distance and dispersing molecular distribution in the solvent. Simultaneously, the guest acceptor positively influenced the crystalization kinetics by providing nuclei seeding sites. Finally, a fine phase separation is achieved in the open-air blade-coated organic solar cells with a state-of-the-art power conversion efficiency of 19.67%.

Blade coating is a promising tool for upscaling organic solar cells (OSCs). However, the performances of blade-coated OSCs still lag behind their spin-coated counterparts, limiting their competitive edge towards commercialization. One of the main reasons is that controlling the film aggregation kinetics and morphology becomes challenging during the transition from spin coating to blade coating, especially when using high boiling point solvents, which can result in excessive aggregation. Therefore, a deeper understanding and appraisal of film formation kinetics influenced by coating methods is crucial. In this work, it is demonstrated that ink solubility tuning by incorporating a twisted third component (BTP-4Cl) can induce rapid crystallization behavior and promote fine phase separation between the donor polymer (PM6) and the acceptor (BTP-eC9) in blade coating. As a result, a high power conversion efficiency (PCE) of 19.67% is obtained in OSCs (0.04 cm2), one of the state-of-the-art efficiencies among the reported blade-coated OSCs (19.76% for the spin-coated devices). In addition, it is found that the inhibited phase aggregation contributes to enhancing the light stability of the device. This strategy offered novel insights into the effectiveness of solubility-tuning approaches for achieving highly efficient and stable OSCs under open-air coating conditions.

This study presents the synthesis of mitochondrion-targeted nanodrugs containing a BODIPY-derived type I photosensitizer and a dual nanozyme for light-controlled mitochondrial stress-inducing and agonist-independent cGAS-STING pathway activation. Their tumor therapeutic ability, dual nanozyme activities, mitochondrion-targeted cGAS-STING pathway activation, and intratumoral and systemic immunositimulation capacity underscore their potential as a paradigm for efficient photoimmunotherapy.

CGAS-STING agonists generally lead to hyperimmunity and systemic toxicity, hindering their immunotherapeutic outcomes. Herein, a mitochondrion-targeted nanoagonist (termed HABH) containing boron dipyrromethene (BODIPY)-derived type I photosensitizer (BDP) and Au nanoparticle-engineered hollow mesoporous silica (HMSN/AuNPs) has been fabricated for light-controlled mitochondrial stress-inducing and agonist-independent cGAS-STING pathway activation. The HABH nanoagonist can actively target tumor tissues and release the mitochondrion-targeted BDP. Under light illumination, BDP achieves type I photodynamic therapy (PDT) in mitochondria, generating massive hydroxyl radicals (•OH) and inducing mitochondrial stress in an oxygen-independent manner, promoting the release of mitochondrial DNA (mtDNA). Simultaneously, the HMSN/AuNPs act as dual nanozymes to derive cascade reactions for •OH production, elevating the intracellular oxidative state, and together with the BDP-induced mitochondrial stress, finally evoking the cGAS-STING pathway and facilitating the release of type I interferon. In the orthotopic breast tumor models, the HABH nanoagonist achieved intratumoral and systemic immunoactivation for eradicating primary tumors and preventing metastasis tumors. Therefore, the constructed mitochondrion-targeted nanoagonist enabled light-controlled and agonist-independent cGAS-STING activation, providing a paradigm for photoimmunotherapy.