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Metal-assisted chemical etching (MaCE) enables silicon nanostructure fabrication but suffers from isotropic undercutting. This study highlights the critical role of catalyst morphology in etching directionality. High-aspect-ratio catalysts induce lateral etching, while thermal treatment at 450 °C stabilizes catalyst geometry, promoting vertical etching. These findings offer a strategy for precise silicon nanostructure control, advancing semiconductor and nanofabrication applications.

Metal-assisted chemical etching (MaCE) has emerged as a promising technique for fabricating silicon nanostructures, yet the presence of anomalous isotropic etching poses significant challenges for precise dimensional control. Here, it is demonstrated that catalyst morphology, particularly its aspect ratio, plays a crucial role in determining etching directionality. Through systematic investigation of the initial stages of MaCE, it is revealed that significant undercutting occurs within seconds of etching initiation, persisting across all solution compositions. This phenomenon is quantitatively analyzed using the Degree of Undercutting (DoU) and Degree of Anisotropy (DoA) metrics, establishing that conventional solution chemistry control alone cannot suppress lateral etching. These findings reveal that high-aspect-ratio dendrite catalysts, formed at elevated AgNO3 concentrations, undergo physical separation during etching, leading to residual catalysts that promote localized isotropic etching. To address this, a thermal treatment approach is developed that effectively transforms these problematic structures into stable, low-aspect-ratio catalysts. A critical transition at 450 °C, where enhanced silver atom mobility coincides with surface defect formation, enables nearly perfect vertical etching. This work not only provides fundamental insights into the relationship between catalyst geometry and etching behavior but also presents a practical solution for achieving precise control over silicon nanostructure fabrication.

A machine learning framework is harnessed to scrutinize the thermodynamically induced crystal phase transition behavior of medium-entropy Prussian blue analogs (ME-PBA). This study provides a unified framework for understanding the crystal phase transformation in ME-PBA and is poised to lay the groundwork for the development of other polymetallic coordination polymer derivatives.

Prussian blue analogs (PBAs) are exemplary precursors for the synthesis of a diverse array of derivatives.Yet, the intricate mechanisms underlying phase transitions in these multifaceted frameworks remain a formidable challenge. In this study, a machine learning-guided analysis of phase transitions in a medium-entropy PBA system is delineated, utilizing an array of descriptors that encompass crystallographic phases, structural subtleties, and fluctuations in multimetal valence states. By integrating multimodal simulations with experimental validation, a thermodynamics-driven phase transformation model for medium-entropy PBA is established and accurately predicted the critical synthesis parameters. A constellation of advanced techniques—including atomic force microscopy coupled with Kelvin probe force microscopy for individual nanoparticles, X-ray absorption spectroscopy, operando ultraviolet-visible spectroscopy, in situ X-ray diffraction, theoretical calculations, and multiphysics simulations—substantiated that the iron oxide@NiCoZnFe-PBA exhibits both exceptional stability and remarkable electrochemical activity. This investigation provides profound insights into the phase transition dynamics of polymetallic complexes and propels the rational design of other thermally-induced derivatives.

The reactive oxygen species (ROS)-responsive ordered assembly of magnetic nanoparticles (RMNAs) achieve a ROS-dependent off/on MPI signal regulation through the ordered assembly/disassembly-mediated MPI tuning strategy. Remarkably, the activatable MPI probe, RMNA, demonstrates a 3.98-fold recovery of MPI signals in response to ROS conditions, enabling ultra-sensitive monitoring of acute liver injury at a low dosage of 0.05 mg kg−1, with a 27-fold increase in MPI signals compared to the non-responsive group.

Magnetic particle imaging (MPI) has emerged as a versatile biomedical imaging modality, yet a significant challenge persists in the absence of activatable MPI probes for targeted imaging of disease biomarkers. In this study, a reactive oxygen species (ROS)-responsive ordered assembly of magnetic nanoparticles (MNPs) is reported, engineered through the meticulous design of magnetic nanoparticle building blocks and ROS-responsive polymeric ligands, enabling precise control over the assembly structure. This ordered configuration amplifies magnetic dipole-dipole interactions, raising the energy barrier during nonequilibrium dynamic magnetization and effectively quenching the MPI signal. By modulating the assembly and disassembly of these ordered structures in response to ROS, this nanoprobe achieves ROS-dependent off/on MPI signal regulation. Consequently, the probe enables the monitoring of early pathological ROS change in a mice model of early acute liver injury, facilitating highly sensitive monitoring of the ROS level-dependent severity of the disease. This work represents the inaugural application of microenvironment-responsive MPI probes for the early diagnosis of ROS-associated diseases. The introduction of ordered assembly structures for MPI signal tuning offers a promising translational approach in the development of next-generation activatable MPI probes.

Full-color tunable time-dependent room-temperature phosphorescence (RTP) from self-protective carbonized polymer dots (CPDs) is achieved via a self-doping strategy for simultaneous modulation of their carbon core N-related and surface oxygen-related emissive centers. The broad emission color, long lifetime, and excellent luminescence stability of these dynamic afterglow materials promote their practical applications in multimodal anti-counterfeiting and advanced dynamic information encryption, as well as time-delay light-emitting diodes (LEDs).

Achieving full-color time-dependent tunable phosphorescence (TDTP) in pure organic materials remains a significant challenge due to the nonradiative transition and modulation puzzle of triplet states. Herein, full-color TDTP has been realized in self-protective carbonized polymer dots (CPDs) under ambient conditions using a self-doping strategy. These CPDs are generated with dual emission centers of the high-energy N-related triplet state and the low-energy surface oxide triplet state, which are responsible for the slow-decaying blue afterglow (453 nm) and the fast-decaying green to red afterglow (513–609 nm), respectively. These luminescent centers can be activated simultaneously upon CPD aggregation due to the generated rigid networks by intra/intermolecular hydrogen-band interactions. The detailed experimental characterization and theoretical calculation confirm that the red-shifted afterglow color is attributed to a gradual reduction of their energy levels with the increasing surface C═O content and aggregation degree of CPDs. Thus, these matrix-free CPDs exhibit dynamic TDTP colors over the entire visible spectrum in the solid state after turning off 365 nm UV light. Based on their unusual phosphorescent properties and excellent photostability, these CPDs have been tested for various applications such as multidimensional dynamic information encryption and anti-counterfeiting, as well as time-delayed light-emitting diodes (LEDs).

This review provides a comprehensive overview of the recent advances in the single-atom site electrocatalysts (SACs) stability/durability, encompassing both deactivation mechanism at the atomic-, meso-, and nanoscale, and mitigation strategies by controlling the catalyst composition, structure, morphology and surface. Moreover, the challenges and prospects of efficient SACs for long-term use are proposed. This review can provide a unique perspective as well as rational guidelines, with emphasis on stability/durability issues, for future large-scale applications of SACs and beyond.

Single-atom site electrocatalysts (SACs), with maximum atom efficiency, fine-tuned coordination structure, and exceptional reactivity toward catalysis, energy, and environmental purification, have become the emerging frontier in recent decade. Along with significant breakthroughs in activity and selectivity, the limited stability and durability of SACs are often underemphasized, posing a grand challenge in meeting the practical requirements. One pivotal obstacle to the construction of highly stable SACs is the heavy reliance on empirical rather than rational design methods. A comprehensive review is urgently needed to offer a concise overview of the recent progress in SACs stability/durability, encompassing both deactivation mechanism and mitigation strategies. Herein, this review first critically summarizes the SACs degradation mechanism and induction factors at the atomic-, meso- and nanoscale, mainly based on but not limited to oxygen reduction reaction. Subsequently, potential stability/durability improvement strategies by tuning catalyst composition, structure, morphology and surface are delineated, including construction of robust substrate and metal-support interaction, optimization of active site stability, fabrication of porosity and surface modification. Finally, the challenges and prospects for robust SACs are discussed. This review facilitates the fundamental understanding of catalyst degradation mechanism and provides efficient design principles aimed at overcoming deactivation difficulties for SACs and beyond.

The study developed GAZn-PEG nanoparticles (GAZn-PEG NPs) that synergize with HIFU to enhance anti-tumor immunity. GAZn-PEG NPs reduce HSP-90 expression, promote dendritic cell maturation, and activate the cGAS-STING pathway, amplifying immune stimulation. Combined with HIFU, GAZn-PEG NPs eradicated local tumors and induced durable systemic immunity, effectively suppressing metastasis and recurrence.

High-intensity focused ultrasound (HIFU) is emerging as a promising non-invasive treatment for solid tumors. Nevertheless, HIFU may also induce the upregulation of Heat Shock Protein 90 (HSP-90), potentially resulting in resistance to HIFU. Besides, although it is effective against in situ tumors, challenges remain with tumor metastasis and recurrence. Herein, the innovative design of gambogic acid (GA) based coordination polymer—GAZn-PEG nanoparticles (GAZn-PEG NPs) are synthesized through the coordination of GA with zinc ions (Zn2+), and subsequently functionalized with lipid bilayer incorporating polyethylene glycol (PEG), sensitizing HIFU for the treatment of cervical and ovarian cancers. Briefly, under HIFU exposure, GA markedly suppresses the expression of HSP-90, thereby increasing the tumor's sensitivity to HIFU therapy. Furthermore, Zn2+ not only overcome the issue of GA's poor water solubility but also synergistically stimulate immune responses in conjunction with GA. More intriguingly, it has been discovered that GAZn-PEG can effectively activate the cyclic GMP-AMP synthase-stimulator of the interferon genes (cGAS-STING) pathway, thereby enhancing the immune responses provoked by HIFU. Specifically, GAZn-PEG NPs show a remarkable increase in dendritic cell activation and the effective stimulation of the cGAS-STING pathway, crucial for long-term protection against tumor recurrence and metastasis.

Quasi-periodic metamaterials combine stiffness and large-strain deformability, overcoming limitations of traditional stretching-dominated periodic designs that are prone to global buckling instabilities and catastrophic layer collapses. By leveraging non-uniform force chains, they achieve high isotropic stiffness, stable deformation, and remarkable failure resistance. Supported by numerical and experimental results, these advances open pathways for low-density applications in impact resistance and energy absorption.

Architected materials achieve unique mechanical properties through precisely engineered microstructures that minimize material usage. However, a key challenge of low-density materials is balancing high stiffness with stable deformability up to large strains. Current microstructures, which employ slender elements such as thin beams and plates arranged in periodic patterns to optimize stiffness, are largely prone to instabilities, including buckling and brittle collapse at low strains. This challenge is here addressed by introducing a new class of aperiodic architected materials inspired by quasicrystalline lattices. Beam networks derived from canonical quasicrystalline patterns, such as the Penrose tiling in two dimensions and icosahedral quasicrystals (IQCs) in three dimensions, are shown to create stiff, stretching-dominated topologies with non-uniform force chain distributions, effectively mitigating the global instabilities observed in periodic designs through distributed localized buckling instabilities. Numerical and experimental results confirm the effectiveness of these designs in combining stiffness and stable deformability at large strains, representing a significant advancement in the development of low-density metamaterials for applications requiring high impact resistance and energy absorption. These results demonstrate the potential of deterministic quasi-periodic topologies to bridge the gap between periodic and random structures, while branching toward uncharted territory in the property space of architected materials.

A broadband polycrystalline lithium niobate platform is developed for highly versatile and scalable fabrication of nonlinear metasurfaces. This work demonstrates simultaneous second harmonic generation and wavefront-shaping via a metalens on this platform. The high effective optical nonlinearity enables broadband frequency doubled light focusing for power density enhancement from near-ultraviolet to near-infrared spectral range.

Miniaturizing nonlinear optical components is essential for integrating advanced light manipulation into compact photonic devices, enabling scalable and cost-effective applications. While monocrystalline lithium niobate thin films advance nonlinear nanophotonics, their high inertness limits the design of top-down fabricated nanostructures. A versatile bottom-up fabrication method based on nanoimprint lithography is presented for achieving polycrystalline lithium niobate nanostructures and demonstrate its significant potential for nonlinear metasurfaces. The fabrication enables nearly vertical features and aspect ratios of up to 6 combined, which we combine with a novel solution-derived material with high effective second-order nonlinearity d eff of 5 pm V−1. On this platform, second-harmonic focusing is demonstrated over a broad spectral range from near-ultraviolet to near-infrared, increasing the nonlinear signal intensity by up to 34 times. This method enables the first lithium niobate metalens and expands the field of nonlinear metasurfaces by providing a low-cost, highly scalable fabrication method for engineered nonlinear nanostructures.

Cancer metastasis begins with intravasation, a complex process involving cancer-endothelial interactions. INVADE (Intravasation-on-µDevice), a biomimetic microfluidic platform enables high-throughput analysis of intravasation under controlled conditions. This system reveals distinct invasion modes, an epithelial-mesenchymal transition (EMT) - mesenchymal-epithelial transition (MET) switch, and endothelial suppression of mesenchymal traits. It also uncovers bilateral signaling, highlighting dynamic cancer-endothelial crosstalk with implications for metastasis research. .

Cancer metastasis begins with intravasation, where cancer cells enter blood vessels through complex interactions with the endothelial barrier. Understanding this process remains challenging due to the lack of physiologically relevant models. Here, INVADE (Intravasation-on-µDevice), a biomimetic microfluidic platform, is presented, enabling high-throughput analysis of cancer cell intravasation under controlled conditions. This engineered platform integrates 23 parallel niche chambers with an endothelialized channel, providing both precise microenvironmental control and optical accessibility for real-time visualization. Using this platform, distinct intravasation mechanisms are uncovered: MCF-7 cells exhibit collective invasion, while MDA-MB-231 cells demonstrate an interactive mode with three functionally distinct subpopulations. A previously unknown epithelial-mesenchymal transition (EMT) and mesenchymal-epithelial transition (MET) switch is We discovered during intravasation, where MDA-MB-231 cells initially increase Vimentin expression before undergoing a 2.3 fold decrease over 96 h alongside a 1.5 fold increase in epithelial cell adhesion molecule (EpCAM). Remarkably, endothelial cells directly suppress cancer cell mesenchymal properties, as evidenced by a 4.6 fold reduction in Vimentin expression compared to mono-cultures. Additionally, bilateral cancer-endothelial interactions are revealed, aggressive cancer cells induce significant intercellular adhesion molecule-1 (ICAM-1) upregulation in endothelium. The INVADE platform represents an engineering advancement for studying complex cell–cell interactions with implications for understanding metastatic mechanisms.

A recent article by Barnes and co-workers reported an experimental re-evaluation of earlier work on photoisomerization reactions inside optical cavities under conditions of strong light-matter coupling. They correctly highlight the importance of controlling irradiation conditions from sample to sample where optical cavities are involved. This comment aims to emphasize the great lengths the original study went to ensure exactly this.

Recently, an article by Barnes and co-workers reported an in-depth experimental re-evaluation of the earlier work on photoisomerization reactions inside optical cavities under conditions of strong light-matter coupling. That earlier work, which constituted the first demonstration of ‘polaritonic chemistry’, associated cavity-induced modifications of photoisomerization rates with the emergence of strong light-matter coupling (and the formation of polaritonic states). Barnes and co-workers instead found that cavity-induced changes in light absorption can account for changes in the photochemical reaction rates. While Barnes and co-workers correctly highlight the importance of controlling irradiation conditions from sample to sample where optical cavities are involved, this comment aims to emphasize the great length the original study went to ensure exactly this. The original experimental methods are summarized to point out the significant differences between them and those conducted by Barnes and co-workers. Furthermore, the importance of monochromatic photoexcitation at an isosbestic point rather than using broadband (UV through to IR) irradiation, as well as the careful control for photon flux reaching the molecular layer in all samples, as per the original work, is discussed. Further examination of important issues facing this new and developing domain of Physical Chemistry, is anticipated.

A time-division multiplexing physical unclonable function (TDM-PUF) label based on multicolor phosphorescent carbon dots (CDs) is proposed, which leverages the variations in wavelengths and lifetimes of the phosphorescent CDs to construct time-resolved multidimensional cryptographic protocols. This study provides a competitive anti-counterfeiting label and inspires the development of novel anti-counterfeiting strategies.

Phosphorescent materials offer a promising approach to information encryption due to their long luminescence lifetimes and high signal-to-noise ratios. However, fixed phosphorescent patterns are vulnerable to imitation over time, limiting their effectiveness in advanced encryption. Here, a time-division multiplexing physical unclonable function (TDM-PUF) label utilizing multicolor phosphorescent carbon dots (CDs) is proposed that leverages variations in wavelength and lifetime to construct time-resolved, multidimensional cryptographic protocols. Efficient multi-color phosphorescence in CDs is achieved by enhancing intersystem crossing, suppressing non-radiative transitions through confinement effects, and regulating emission spectra via energy transfer. The random spatial distribution and unpredictable emissions of phosphorescent CDs significantly enhance the complexity of the PUF system, thereby fortifying its defenses against mimicry attacks. Furthermore, this PUF system exhibits multiple optical responses over time, allowing correct information recognition only at specified time nodes, achieving time-resolved anti-counterfeiting. Finally, by segmenting PUF labels based on emission color and time channels, non-overlapping multicolor and multi-time segments are achieved, enabling highly secure time-division multiplexed encryption. The study provides a competitive anti-counterfeiting label and inspires the development of novel anti-counterfeiting strategies.

Understanding the complex interplay between local structure and physical properties is a key challenge in high entropy oxide (HEO) research, particularly concerning electronic transport. This work demonstrates the profound influence of local chemical inhomogeneity and underlying epitaxial strain on the electronic transport properties of HEO thin film with perovskite structure, paving pathways to tailor electronic properties in high-entropy regime.

Understanding the electronic transport properties of thin films of high-entropy oxide (HEO), having multiple elements at the same crystallographic site, is crucial for their potential electronic applications. However, very little is known about the metallic phase of HEOs even in bulk form. This work delves into the interplay between global and local structural distortion and electronic properties of single crystalline thin films of (La0.2Pr0.2Nd0.2Sm0.2Eu0.2)NiO3, which exhibit metal-insulator transition under tensile strain. Employing electron microscopy and elemental resolved electron energy loss spectroscopy, we provide direct evidence of nanoscale chemical inhomogeneities at the rare-earth site, leading to a broad distribution of Ni–O–Ni bond angles. However, the octahedral rotation pattern remains the same throughout. The metallic phase consists of insulating patches with more distorted Ni–O–Ni bond angles, responsible for higher resistance exponents with increased compositional complexity. Moreover, a rare, fully metallic state of HEO thin film is achieved under compressive strain. We further demonstrate a direct correlation between the suppression of the insulating behavior and increased electronic hopping. Our findings provide a foundation for exploring Mott-Anderson electron localization physics in the high-entropy regime.

A core-shell perovskite composite with a highly durable electrochemical activity for oxygen catalysis is developed as an air electrode for reversible protonic ceramic cells (RPCCs) via a unique solid-state reaction. This work also demonstrates a new pathway to developing highly durable air electrode materials for RPCCs technology, accelerating RPCCs’ commercialization.

Reversible protonic ceramic cells (RPCCs) offer a promising pathway to efficient and reversible energy conversion, accelerating the global shift to renewables. However, the RPCCs’ commercialization faces limitations in air electrode materials. Traditional cobalt-based perovskite air electrodes, while effective, suffer from high cost and environmental concerns. Alternative materials, such as SrFeO3-δ (SF)-based perovskites, offer potential, yet durability issues, including thermal-expansion mismatch and mechanical instability, hinder their practical application. Here, a unique solid-state reaction between SF and negative-thermal-expansion (NTE) material is demonstrated to yield a core-shell perovskite composite as a highly durable RPCCs air electrode. Specifically, by calcining a mixture of SF and an NTE material, ZrW2O8 (ZWO), the in situ incorporation of ZWO into the SF lattice is achieved, resulting in a non-closed core-shell composite, comprising single perovskite SraFebZrcWdO3-δ (SP-SFZW) core and B-site cation ordered double perovskite SrxFeyZrmWnO6-δ (DP-SFZW) shell. Both SP-SFZW and DP-SFZW serve as oxygen catalysts, while DP-SFZW shell additionally acts as a thermal expansion suppressor and mechanical support structure, effectively mitigating electrode cracking and delamination from other cell components during RPCC operation. Consequently, the composite electrode demonstrates comparable catalytic activity to SF, coupled with significantly enhanced durability. This work illustrates a novel approach for developing robust RPCCs air electrode.

An AEM-derived proton acceptor-electron donor mechanism is proposed in RuO2 by constructing an interstitial-substitutional mixed solid solution structure (C,Ta-RuO2), in which the interstitial C as the proton acceptor decreases the deprotonation energy barrier, while the substitutional Ta as the electron donor weakens the Ru─O bond covalency, thereby breaking the activity-stability trade-off of RuO2 in acidic OER.

The acidic oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane electrolyzer (PEMWE) often face a trade-off between activity and stability due to inherent linear relationship and overoxidation of metal atoms in highly oxidative environments, while following the conventional adsorbate evolution mechanism (AEM). Herein, a favorable AEM-derived proton acceptor-electron donor mechanism (PAEDM) is proposed in RuO2 by constructing interstitial-substitutional mixed solid solution structure (denoted as C,Ta-RuO2), which can effectively break the activity-stability trade-off of RuO2 in acidic OER. In situ spectroscopy experiments and theoretical calculations reveal that the interstitial C as the proton acceptor reduces the deprotonation energy barrier, enhancing catalytic activity, while the substitutional Ta as the electron donor donates electrons to the Ru sites via bridging oxygen, weakening the Ru─O bond covalency and preventing over-oxidation of surface Ru, thereby ensuring long-term stability. Under the guidance of this mechanism, the optimized C,Ta-RuO2 simultaneously achieves far low overpotential (η10 = 171 mV) and ultra-long stability (over 1300 h) for the acidic OER. More remarkably, a homemade PEMWE using C,Ta-RuO2 as the anode also shows high water splitting performance (1.63 V@1 A cm−2). This work supplies a novel strategy to guide future developments on efficient OER electrocatalysts toward water oxidation.

Breaking Quantum Confinement in Yb3⁺-Doped ZnSe QDs: Surface-energy engineering enables scalable growth beyond the exciton Bohr radius with high-purity blue emission (453 nm), narrow full width at half maximum (FWHM) of 46 nm, and exceptional photoluminescence quantum yield (PLQY) of 67.5%.

Large ZnSe quantum dots (QDs) with an emission peak ≈450 nm hold significant promise for display technologies. However, achieving efficient pure-blue emission through the enlargement of ZnSe nanocrystals remains a significant challenge. In this study, a breakthrough is reported in growing large-size ZnSe QDs well beyond the exciton Bohr radius through Yb3+ doping strategy. Yb3+ doping reduces the surface energy of the ZnSe (220) crystal plane and alleviates interface strain in the ZnSe/ZnS structure, enabling the QDs to grow larger while maintaining enhanced crystal stability. The resulting Yb: ZnSe/ZnS QDs exhibit pure-blue emission at 453 nm, with a full width at half maximum (FWHM) of 46 nm and a high photoluminescence quantum yield (PLQY) of 67.5%. When integrated into quantum dot light-emitting diodes (QLEDs), the devices display electroluminescence (EL) at 455 nm, with an external quantum efficiency (EQE) of 1.35%, and a maximum luminance of 1337.08 cd m−2.

A heterogeneous microgel–hydrogel hybrid is developed to construct a multiscale vascular network through embedded bioprinting and guided vascular morphogenesis. With a high density of hepatocytes, a bioengineered thick vascularized liver tissue model achieves a rapid and promising functional compensation in rats with 85% hepatectomy via direct vascular integration, providing a theraputi paradigm for physiological-related engineered tissue in animals with acute disease.

3D bioprinting of liver tissue with high cell density (HCD) shows great promise for restoring function in cases of acute liver failure, where a substantial number of functional cells are required to perform essential physiological tasks. Direct vascular anastomosis is critical for the successful implantation of these bioprinted vascularized tissues into the host vasculature, allowing for rapid functional compensation and addressing various acute conditions. However, conventional hydrogels used to encapsulate high-density cells often lack the mechanical properties needed to withstand the shear forces of physiological blood flow, often resulting in implantation failure. In this study, a heterogeneous microgel–hydrogel hybrid is developed to carry HCD hepatocytes and support the embedded bioprinting of hierarchical vascular structures. By optimizing the ratio of microgel to biomacromolecule, the covalently crosslinked network offers mechanical integrity and enables direct vascular anastomosis, ensuring efficient nutrient and oxygen exchange. The bioprinted thick, vascularized constructs, containing HCD hepatocytes, are successfully implanted in rats after 85% hepatectomy, leading to swift functional recovery and prolonged survival. This study presents a strategy to enhance regenerative therapy outcomes through advanced bioprinting and vascular integration techniques.

The α-FAPbI3 perovskite, ideal for high-efficiency solar cells, suffers from impurity phases causing defects and instability. Using FAI/MASCN vapors repairs impurities into α-FAPbI3, enhancing charge transport and morphology. This achieves 26.05% efficiency, with large-area devices (24.52% for 1 cm2, 22.35% for 17.1 cm2). Cyclic repair retains 94.3% efficiency after two cycles, significantly boosting device durability.

The photoactive α-phase of formamidinium lead iodide perovskite (α-FAPbI3) is regarded as one of the ideal materials for high-efficiency perovskite solar cells (PSCs) due to its superior optoelectronic properties. However, during the deposition of α-FAPbI3 perovskite films, the presence of impurity phases, such as PbI2 and δ-FAPbI3, can cause the formation of inherent defects, which leads to suboptimal charge transport and extraction properties, as well as inadequate long-term stability in the film's morphology and structure. To address these issues, an impurity phase repair strategy is employed using FAI/MASCN mixed vapors to convert the impurity phases into light-absorbing α-FAPbI3. Meanwhile, this recrystallization process also facilitates the recovery of its characteristic morphology, thereby improving efficiency and enhancing the durability of PSCs. This approach promotes the PSCs to obtain an efficiency of 26.05% (with a certified efficiency of 25.67%, and steady-state PCE of 25.41%). Additionally, this approach is suitable for the fabrication of large-area devices, obtaining a 1 cm2 device with a PCE of 24.52% and a mini-module (with an area of 17.1 cm2) with a PCE of 22.35%. Furthermore, it is found that this strategy enables cyclic repair of aged perovskite films, with the perovskite solar cells retaining ≈ 94.3% of their initial efficiency after two cycles of repair, significantly enhancing the lifetime of the perovskite solar cells.

A self-assembled interface orthogonal strategy is first applied to construct pseudo-planar heterojunction organic photovoltaics with controllable vertical gradient distribution morphology. Introducing low surface-energy N2200 to self-assemble molecular layer on PM6 surface overcomes erosion effect and modulates phase morphology, thus achieving the highest efficiency of 19.86% via air-printing process.

Precisely regulating vertically distributed morphology by blade-coating process is crucial to realize high-performance large-scale pseudo-planar heterojunction organic photovoltaics (OPVs). However, the thermodynamic motion and random diffusion of donor/acceptor (D/A) generated from the differences in surface energy and concentration during sequentially blade-coating process will cause great challenges for obtaining ideal active layer morphology. Herein, this study have proposed a self-assembled interface orthogonal strategy by introducing low surface energy guest (N2200) to form protective layer on PM6 surface, which counteracts erosion from orthogonal solution of acceptor to enhance continuity of D/A phases, thus promoting directional carrier migration and effectively suppressing energetic disorder. Finally, N2200-modified device achieves the highest power conversion efficiency (PCE) of 19.86%, and large-area module (16.94 cm2) exhibits exceptional PCE (16.43%). This investigation presents innovative insights into morphology issue triggered by molecular motion and provides an effective method for air-printing large-scale OPVs with precisely controlled morphology based on non-halogenated solvent.

A novel copper-sulfur-nitrogen cluster Cu8SN is synthesized by using a strong anchoring ability protective ligand (2-mercaptopyrimidine) and a relatively weak monodentate tert-butyl mercaptan ligand. Then, a precise thermal-resection strategy is applied to only peel the targeted weak ligands off, which induces a structural transformation of the initial Cu8SN cluster into a new and more stable Cu–S–N cluster (Cu8SN–T). Cu8SN–T exhibits greatly enhanced light-harvesting abilities and full-spectrum responsive overall CO2 photoreduction with ≈100% CO2-to-CO selectivity.

Atomically precise copper clusters are desirable as catalysts for elaborating the structure–activity relationships. The challenge, however, lies in their tendency to sinter when protective ligands are removed, resulting in the destruction of the structural integrity of the model system. Herein, a copper-sulfur-nitrogen cluster [Cu8(StBu)4(PymS)4] (denoted as Cu8SN) is synthesized by using a mixed ligand approach with strong chelating 2-mercaptopyrimidine (PymSH) ligands and relatively weak monodentate tert-butyl mercaptan ligands. A precise thermal-resection strategy is applied to selectively peel only the targeted weak ligands off, which induces a structural transformation of the initial Cu8 cluster into a new and more stable Cu–S–N cluster [Cu8(S)2(PymS)4] (denoted as Cu8SN-T). The residual bridging S2− within the metal core forms asymmetric Cu-S species with a near-infrared (NIR) response, which endows Cu8SN-T with the capability for full-spectrum responsive CO2 photoreduction, achieving a ≈100% CO2-to-CO selectivity. Especially for NIR-driven CO2 reduction, it has a CO evolution of 42.5 µmol g−1 under λ > 780 nm. Importantly, this work represents the first NIR light-responsive copper cluster for efficient CO2 photoreduction and opens an avenue for the precise manipulation of metal cluster structures via a novel thermolysis strategy to develop unprecedented functionalized metal cluster materials.