Physics

High Resolution Image Download MS PowerPoint Slide Full control over excitons in 2D materials is an important step toward their exploitation for applications. Strain modulation is one method that can be used to effectively control the movement of the excitons. Unfortunately, the effects of nonuniform strain in 2D materials are not yet well understood theoretically. However, these strain fields can be present in experiments in the form of wrinkles, bubbles, and folds, or even explicitly applied to 2D materials through prepatterned surfaces. The effects of these nonuniform strain fields on multilayers are even less studied because of the sheer size of these systems. In the present investigation, we study wrinkles that form in homo- and heterobilayers of 2D transition-metal dichalcogenides using density functional theory. We show that nonuniform strain could lead to the formation of spatially localized, momentum-direct, bright interlayer excitons IX KK in homobilayers of transition-metal dichalcogenides such as WSe 2 and WS 2 and to exciton localization in transition-metal dichalcogenide heterobilayers. Our results also reveal that the spin angular momentum is changed due to the mixing of in- and out-of-plane states, which can explain the brightening of the formerly dark excitonic states under strain. Our results provide insights into a better understanding of the strain control of excitons in 2D materials.

Positive nanoparticles have often a higher uptake than neutral and negative nanoparticles. This is usually attributed to electrostatic interactions with negatively charged proteoglycans on the cell membrane. However, upon contact with serum, nanoparticles adsorb a biomolecule corona and tend toward neutrality, suggesting that electrostatic interactions alone cannot explain the different uptake. Here, we used oppositely charged liposomes as an example to explore at a fundamental level why positive nanoparticles usually show a higher uptake than the negative ones. Two proteomic-based approaches were combined to compare their protein coronas and the cell surface proteins involved in their internalization. The results showed that the higher uptake of the positive liposomes used for this study could not be simply explained by the involvement of specific corona proteins and dominating cell surface proteins. Instead, small differences in the abundances of a large number of corona proteins and cell surface proteins were observed, including multiple low-abundance proteins. Importantly, the positive liposomes had higher uptake than the negative liposomes only when added to cells in the presence of serum, suggesting that the higher uptake likely resulted from the observed subtle differences in their corona and the collective contribution and interactions with multiple cell surface proteins.

Dipolar excitons typically emerge in weakly coupled van der Waals heterostructures (vdWHs), where electrons and holes are confined in different layers. However, the tunability of these extrinsic interlayer dipolar excitons under external out-of-plane electric fields is constrained by built-in interfacial electric fields and significant nonradiative processes. Here, we propose a dipolar exciton in monolayer Hf 2 SiCO 2, where vertically separated electrons and holes reside in a single layer of several atoms’ thickness. The dipolar excitons in the two X valleys, connected by rotoreflection symmetry, possess alternating antiparallel out-of-plane electric dipole moments, which are termed an alterexciton . These dipolar excitons exhibit electrically tunable polarization in a single valley, which further leads to a single-valley excitonic insulator under an increasing electric field. Because of the optical selection rules, the layer-locked valley excitons exhibit linear dichroism and valley-dependent electrical tunability. Furthermore, under linearly polarized light, the Coulomb-bound electrons and holes of the excitons are simultaneously deflected by the Berry curvature in each layer-locked valley, giving rise to the exciton Hall effect. These results not only contribute to the valley-polarized manipulation of dipolar excitons but also facilitate the exploration of single-valley single-photon emitters.

Piezoelectric dynamic therapy utilizes the acoustic-electric conversion of piezoelectric materials under ultrasound (US) to generate abundant reactive oxygen species (ROS) to kill tumor cells, offering an attractive protocol for tumor therapy. However, traditional piezoelectric sonosensitizers generally exhibit wide band gaps, resulting in suboptimal charge separation, low ROS generation efficiency, and insufficient induction of immunogenic cell death (ICD), which limits their therapeutic efficacy. In this study, we report a narrow-band gap piezoelectric nanoplatform engineered from porphyrin-osmapentalyne hybrids (P-OsPT). By strategically coupling anti-Hückel carbolong electron acceptor (A) with a Hückel-compliant porphyrin electron donor (D), a pronounced A-D-A architecture is established. The incorporation of osmium within the carbolong framework facilitates a d π - p π conjugation system, which not only significantly narrows the band gap and provides efficient channels for intraparticle charge transport but also imparts piezoelectric properties to the material. Under US irradiation, P-OsPT nanoparticles (NPs) achieve efficient acoustic-electric conversion, resulting in high ROS generation efficiency. In vitro and in vivo studies demonstrate that P-OsPT NPs-mediated piezoelectric immunotherapy can effectively kill tumor cells while inducing ICD, resulting in activation of immune response and inhibition of tumor metastasis. This study highlights the potential of carbolong complexes as a versatile platform for piezoelectric immunotherapy.

The low tumor retention of nanomedicines severely limits the specificity of diagnostic imaging and the efficacy of subsequent therapies. Herein, we report a targeted zwitterionic fluoropolymer probe (PTFBPA-RGD) engineered for exceptional intratumoral retention through tumor microenvironment (TME)-triggered in situ assembly. The probe incorporates stealthy zwitterionic brushes to minimize protein adsorption and prolong systemic circulation. Upon reaching the acidic TME, hydrogen bonding between the trifluoroborate and carboxylic acid moieties acts as an adhesive, driving the self-assembly of the probe into large aggregates, thereby prolonging intratumoral retention. Leveraging its intrinsic high fluorine content, zero-background 19 F magnetic resonance imaging ( 19 F MRI) demonstrated the precise localization of deep-seated tumors across subcutaneous, orthotopic (bladder/liver), and metastatic lung models. After loading with 177 Lu, tumor accumulation peaked at 48 h and remarkably retained 82% of this peak value even 96 h postinjection, leading to robust antitumor efficacy. This work provides an effective strategy to fabricate nanoprobes with high intratumoral retention for the specific multimodal imaging and therapy of deep-seated tumors.

High Resolution Image Download MS PowerPoint Slide Oxide semiconductors such as indium oxide (In 2 O 3 ) offer high-electron mobility and low-temperature processability, making them promising candidates for back-end-of-line (BEOL)-compatible logic-in-memory applications. However, direct deposition of high-κ ferroelectric dielectrics (Hf 0.5 Zr 0.5 O 2; HZO) on oxide channels typically degrades interfacial quality, leading to threshold voltage shifts and unstable polarization due to depolarization fields and defect states. In this work, we leverage advanced membrane transfer techniques to demonstrate a transferable ferroelectric HZO layer for interface-layer-free integration with In 2 O 3 . This approach forms a van der Waals-like junction, evidenced by an ∼0.8 nm interfacial gap, which avoids the chemical incompatibilities of conventional gate stack processing while preserving the pristine stoichiometry of the In 2 O 3 channel. The transferred HZO exhibits a dielectric constant of 26 and low leakage current (<10 –7 A cm –2 at 1 MV cm –1 ) while maintaining robust ferroelectric switching. Dual-gate ferroelectric In 2 O 3 transistors achieve a large memory window and stable endurance over 10 9 cycles. We further integrate these devices into reconfigurable inverter circuits that dynamically switch between NOR and NAND logic functions with tunable voltage transfer characteristics. The ferroelectric thin-film transfer process is fully compatible with silicon back-end-of-line thermal budgets and scalable to wafer-level integration, offering a viable route toward high-density, multifunctional logic-in-memory architectures.

Chiral quasi-bound states in the continuum (q-BICs) have recently emerged in metaphotonics as resonances that combine ultra-high-quality factors with near-unity circular polarization in the far field. However, these states are typically confined to the Γ-point (normal incidence) due to their symmetry-protected origins. We propose a new mechanism for realizing light-cone-proximal chiral q-BICs at large oblique angles, enabled by the divergence of the radiative density of states near the light cone. Using dielectric metasurfaces with a monoclinic lattice and broken in-plane mirror symmetry, we demonstrate that tuning the lattice angle allows for robust control of these resonances. The resulting chiral q-BICs exhibit near-unity circular dichroism in transmission and fully circularly polarized emission at angles exceeding 50° from normal. Our results establish a general route to off-normal and grazing-angle chiral q-BICs, enabling directional chiral lasing and providing a versatile platform for quantum and nonlinear photonics.

I n the original publication, in Figure 3B, the model mouse corresponding to day 13 in the CMCS/Arg@MNs group was inadvertently selected from the GL@MNs group.The affected two-dimensional wound model image of the CMCS/Arg@MNs group and Figure 3C have therefore been corrected accordingly.The corrected Figure 3 is shown below.Also, the changed portion of the Supporting Information file is attached here.The authors apologize for the inconvenience caused by this mistake.This error occurred during image archiving, cropping, and figure assembly.The affected images and corresponding quantitative analysis have been corrected based on the appropriate original data.These corrections do not affect the overall interpretation of the results or the main conclusions of the article.

Unidirectional liquid transport is critical for diverse applications, e.g., atmospheric water harvesting, integrated microfluidics, and high-efficiency heat transfer. However, existing strategies are mostly limited to narrow surface-tension ranges. Here, we designed bioinspired asymmetric cilia arrays (BACAs) mimicking the 45° inclined cilia of Alchemilla mollis, achieving unidirectional liquid transport over an ultrabroad surface-tension range of 22.2–72.8 mN m –1 . Systematic studies show that transport modes depend on surface tension, solid surface energy, and cilia spacing. For 0.6 mm-spaced BACAs (∼16.4 mJ m –2 ), ethanol/water mixtures exhibit reverse transport above 32.1 mN m –1, forward transport below 28.0 mN m –1, and bidirectional flow in between. These phenomena arise from the dynamic equilibrium between gravity and capillarity. We further established a theoretical predictive framework based on the bidirectional transport contact angle to quantify transport modes, which contributed to achieve programmable liquid routing and precise spatiotemporal control over liquid transport.

The atomic architecture of apomyoglobin amyloid fibrils, despite the protein's dual distinction as the first structurally resolved protein and the paradigmatic nondisease amyloid, has remained a decades-long puzzle. Here, we identify electrostatic screening as the critical switch that enables the formation of highly ordered apomyoglobin fibrils, allowing us to determine the cryo-electron microscopy structures of three distinct polymorphs (PM1, PM2, and PM3) at 2.7 Å resolution. The structures reveal a conserved "hydrophobic-in, positively charged-out" architecture, where a charged surface surrounds a tightly packed core, providing a structural explanation for salt-dependent assembly. Structural comparisons reveal a hierarchical principle of amyloid organization, in which short sequence segments retain conserved local conformations dictated by their intrinsic folding propensities, while variations in supramolecular packing give rise to polymorphic diversity. These findings establish a molecular framework for understanding electrostatically controlled self-assembly and the structural basis of amyloid polymorphism.

The shuttle effect of intermediate lithium polysulfides (LiPSs) and sluggish redox kinetics limit the practical application of lithium–sulfur (Li–S) batteries. Herein, RuCo alloy nanoparticles supported on N-doped mesoporous carbon spheres (RuCo/NMCS) are developed as efficient catalytic sulfur hosts. Electron transfer from Co to Ru optimizes the adsorption and catalytic conversion of LiPSs, accelerating sulfur redox reactions. Meanwhile, the dynamic changes of Ru and Co species in the RuCo/NMCS electrode demonstrate the strong Ru–S and Co–S interactions between metals and LiPSs during the discharge–charge process, corresponding to the accelerated conversions of Li 2 S 2 /Li 2 S to LiPSs and LiPSs to S 8 . Consequently, the RuCo/NMCS electrode showcases improved electrochemical performance with enhanced cycling capacity and stable reversible capacity. This work provides a feasible and rational route to construct alloy electrocatalyst-supported cathode materials with bidirectional catalysis on LiPS conversion, promoting the application of alloy electrocatalysts as kinetic regulators for high-performance Li–S batteries.

High Resolution Image Download MS PowerPoint Slide Mechanically induced conformational switching at the single-molecule level represents a fundamental mechanism for molecular functionality, yet quantitative characterization of the underlying force and energy landscape remains limited. Here, we study individual TBrPP-Co(II) molecules on Au(111) using qPlus atomic force microscopy. By reconstructing interaction potentials from 3D Δ f ( x, y, z ) data, we determine a threshold force of ∼96 ± 8 pN and a tip-induced switching interaction energy of ∼38 ± 4 meV associate with the conformational transition. The isolated tip-molecule force follows a power law (exponent ∼6), indicating dominance of long-range van der Waals interactions. At closer distances, deviations reveal force-induced deformation preceding the transition. Validation via the inflection point test confirms measurement reliability. These findings show that long-range dispersive interactions can mechanically deform a molecule and facilitate conformational switching through a deformation-assisted pathway, providing a quantitative framework for controlling mechanically driven functionality at the single-molecule scale.

ABSTRACT Flexoelectricity, a universal electromechanical coupling effect in all dielectric materials, offers a broader range of material selection for fabricating smart and functional devices. Inspired by the serpentine structures found in muscle fibers, this work proposes a metamaterial‐inspired flexoelectric sports monitoring (MFSM) sensor based on polydimethylsiloxane (PDMS), by integrating the concept of microstructural design from metamaterials into sensor engineering. The flexoelectric polarization response can be modulated by both the structural characters of the initial serpentine microstructure and the application of hierarchical lattice design strategies. Experiments demonstrate that, under specific geometric and loading conditions, the proposed MFSM sensor achieves a 44.5‐fold enhancement in the effective transverse piezoelectric coefficient at the macroscopic device level compared to AlN. Furthermore, the structural design can be tailored to match the nonlinear J‐shaped stress‐strain curves of different skin regions, enabling a conformal fit. Finally, by integrating a Wi‐Fi module for real‐time signal monitoring and utilizing deep learning for motion posture identification, the proposed MFSM sensor achieves 100% classification accuracy across seven human motion categories in a single‐subject proof‐of‐concept study. Subject to further validation across broader demographics, this work is anticipated to offer novel solutions for postoperative rehabilitation and athletic posture correction.

ABSTRACT Efficient on‐chip generation and control of chiral incoherent light emission are essential for emerging applications in integrated nanophotonics. Although previous on‐chip light‐emitting metasurfaces have achieved various forms of guided photoluminescence (PL) manipulation, high circular dichroism (CD) emission and chiral phase manipulation remain largely unexplored owing to the absence of robust design paradigms for on‐chip excitation and coupling mechanisms. Here, we propose and experimentally demonstrate an on‐chip chiral emission metasurface (OCEM) platform that enables high‐CD unidirectional PL emission and chiral focusing. By breaking the in‐plane mirror and two‐fold rotational symmetries of on‐chip meta‐atoms, we achieve circular‐polarization‐selective emission of guided PL, experimentally yielding a high CD of ∼0.86 in unidirectional PL emission, with a narrow divergence angle of less than 4° and a large diffraction angle of ∼30°. Furthermore, by incorporating a detour‐phase mechanism via spatial displacement of meta‐atoms, chiral focusing of incoherent guided PL is experimentally demonstrated. By unifying spatial coherence engineering, spin‐selectivity, and chiral wavefront control within a single architecture, the OCEM platform substantially expands the functional repertoire of integrated light sources. We envision that this platform will advance integrated chiral photonic devices, offering a versatile and scalable route toward compact circularly polarized light sources and on‐chip chiroptical sensing.

ABSTRACT Syringe injections inherently accompany burst inoculation of a defined volume to cover a sustained period of effect. Considering the combinative need for both release patterns, a user‐specified switch between burst and sustained release is required, depending on each therapeutic strategy. Ovarian hyperstimulation syndrome (OHSS) is a representative risk of syringe injections used to stimulate ovulation. Follicle‐stimulating hormone (FSH) is injected repeatedly for sustained effects, followed by a last shot of human chorionic gonadotropin (hCG) for burst effects, which accompanies OHSS risks. Hence, a shape memory microneedle (SMN) is developed by enabling recovery from X to O shape by mild heating, switching from sustained to burst release under a single transdermal insertion. The X shape provides sufficient loading spaces for double hormone layers in gelatin gel from outer FSH to inner hCG onto the SMN. After the 3‐day sustained release of FSH by controlling gelatin degradation in the X shape, the recovery to the O shape pushes out hCG for a 24‐hour burst release with sufficient gelatin breakage in a clinic‐mimetic rabbit model. Despite overdose loading with a single shot, the SMN preserves the injection level of ovulation by suppressing OHSS risks, indicating the SMN's potential to address syringe injection issues.

ABSTRACT The cold start of proton exchange membrane fuel cells (PEMFCs) at subzero temperatures is hindered by ice formation during the process. We developed a hierarchical mesoporous carbon structure, denoted as TMC‐GC, showing strong suppression of heterogeneous ice nucleation. The water/TMC‐GC mixture exhibited a phase transition temperature 4.2°C lower than that of the mixture containing commercial carbon black (XC72). Low‐field nuclear magnetic resonance reveals that TMC‐GC can sustain a larger fraction of unfrozen water with higher molecular mobility compared to XC72 at −30°C, thereby favoring more effective removal of supercooled water during cold start. Adopting TMC‐GC as the carbon support, the Pt/TMC‐GC catalyst achieved an isothermal operational time of 25.3 min at −10°C, 3.7 times that of commercial Pt/C (6.8 min), in single‐cell PEMFC tests, demonstrating the state‐of‐the‐art cold‐start performance. Stack‐level theoretical projections indicate that replacing Pt/C with Pt/TMC‐GC enhances PEMFC robustness, enables faster startup, and reduces preheating energy demand (by 28.9% at −20°C) during cold starts. Owing to the superior mass‐transport characteristics of the hierarchical mesoporous carbon structure, the Pt/TMC‐GC delivers key performance metrics that surpass the U.S. Department of Energy targets and are competitive with leading catalysts under normal‐operation conditions.

ABSTRACT As emerging tumor therapies, cuproptosis and disulfidptosis exhibit unique potentials. However, high‐level glutathione (GSH) in the tumor microenvironment neutralizes cuproptosis‐essential copper ions, while pentose phosphate pathway‐mediated nicotinamide adenine dinucleotide phosphate (NADPH) regeneration alleviates disulfidptosis‐required disulfide bonds accumulation, substantially restricting their efficacy. Synergistically inducing these two death mechanisms faces challenges, including antioxidant defense systems, compensatory effects between metabolic pathways, and precise regulation difficulties. Since NADPH deficiency inhibits GSH synthesis, targeting the “glucose metabolism‐NADPH‐GSH” axis may provide a key strategy for synergistically enhancing the cuproptosis and disulfidoptosis effects. Herein, a biomimetic nanosystem LCM@CM was constructed, consisting of a proteolysis‐targeting chimera (PROTAC)‐armed lanthanum single‐atom‐doped multivalent copper heterojunction encapsulated within A549 cell membranes. The heterojunction acts as an “electron pump,” catalyzing the consumption of glucose, GSH, and NADPH while generating O 2 and releasing copper ions, effectively triggering cuproptosis and disulfidptosis. Meanwhile, PROTAC MZ1 can precisely inhibit the BRD4‐c‐MYC‐G6PD signaling pathway, systematically depleting NADPH and GSH from their metabolic sources to directly induce disulfidptosis and enhance the cuproptosis. Additionally, the homologous membrane coating enhances tumor‐specific targeting, and improves nanosystem enrichment in the tumor. By ingeniously integrating chemical catalysis and biological targeting, a strategy using PROTAC and nanoheterojunction to synergistically trigger cuproptosis and disulfidptosis is innovatively proposed, offering novel insights for lung cancer therapy.

ABSTRACT To solve the drawbacks of low lithium‐ion transference number (t Li + ) and poor interface stability of poly(ethylene oxide) (PEO)‐based solid electrolytes, La 3+ ‐doped BiOCl nanosheets were developed as new functional fillers. Via a surfactant‐assisted microemulsion method, the stacking defects of nanosheets were suppressed, and the controllable synthesis of dispersed nanosheets was realized. These nanosheets ensure uniform dispersion in the PEO matrix, construct continuous ion transport channels, and reduce interfacial impedance. It is worth noting that La 3+ doping can accurately control the oxygen vacancy (O v ) concentration, and the optimal doping amount can increase t Li + to 0.47. The assembled Li||Li symmetrical cells deliver a long‐term cycle lifespan of over 2000 h, accompanied by outstanding cycling durability for lithium metal batteries. Theoretical calculations confirm that superior performance originates from lanthanum doping and O v , which facilitate electron delocalization and induced the formation of TFSI − ‐rich interface layer and a LiF‐dominated stable SEI film. Furthermore, the O v remarkably accelerates the redox reaction kinetics of polysulfides and simultaneously boosts the cycling stability of lithium‐sulfur batteries. The universality of the electrolyte design strategy was verified by multi‐scale electrochemical analysis and theoretical calculation, which provided a new idea for the development of high‐performance solid‐state batteries.

ABSTRACT Platinum‐based drugs remain the cornerstone of chemotherapy for various solid tumors. However, their clinical efficacy is limited by systemic toxicities, acquired resistance, and the inability to induce sufficient, durable antitumor immunity. In this context, targeting the cyclic GMP‐AMP synthase (cGAS)‐stimulator of interferon genes (STING) pathway has become a key strategy in modern cancer immunotherapy. Notably, platinum complexes inherently possess the ability to activate this innate immune signaling pathway, primarily through the induction of cytosolic double‐stranded DNA (dsDNA) accumulation. This activation promotes tumor cell apoptosis and enhances antitumor immunity by facilitating antigen presentation, promoting dendritic cell (DC) maturation, and boosting T cell activation. Herein, we review recent advances in platinum‐based STING activators for chemoimmunotherapy. First, mechanisms linking classical platinum cytotoxicity to cGAS‐STING signaling activation are summarized. Subsequently, emerging strategies are systematically categorized into molecular design and nanomedicine approaches. Molecular designs are grouped by the functional ligands attached to platinum scaffolds, while advanced nanoplatforms are arranged according to carrier materials and architectures. Finally, we highlight the remaining challenges in this field and outline potential directions for the development of next‐generation chemoimmunotherapy.

ABSTRACT Solid oxide electrolysis cells (SOECs) offer high‐efficiency conversion of renewable electricity into chemical fuels, but their long‐term durability is limited by impurity poisoning of the Ni‐YSZ fuel electrodes. To understand the impact of polarization on impurity poisoning and microstructural degradation, we employed a novel Pt‐SiO 2 ‐Ni/YSZ/Pt model cell. For direct comparison, the Pt‐SiO 2 ‐Ni electrode was investigated under both cathodic polarization (SOEC operation) and anodic polarization for solid oxide fuel cell (SOFC) operating conditions. Post‐mortem STEM‐EDS and HRTEM analyses firstly reveal Na‐Al‐Si‐O segregation as an amorphous phase instead of crystalline along Ni grain boundaries near gas‐exposed surfaces, accompanied by Zr/Y extraction from the YSZ electrolyte and reprecipitation as fluorite phases near the Ni/YSZ interface. These phenomena are suppressed in the SOFC reference despite identical thermal exposure. The results demonstrate that ultralow oxygen partial pressures generated by cathodic polarization promote reductive dissolution of Si, Na, Al, Y, and Zr into metallic Ni, followed by rapid migration and reoxidation at sites of higher oxygen activity. The polarization‐dependent impurity transport explains accelerated degradation in high‐current SOECs. This work provides direct nanoscale evidence of the dominant degradation mechanism and offers guidance for mitigation strategies toward robust, long‐duration SOEC systems for renewable energy conversion and storage.

ABSTRACT Recurrent infections and persistent inflammation pose significant challenges in the clinical treatment of infected bone defects. Here, a porous scaffold of Zn‐0.8Li‐0.5Ag with a TPMS‐Gyroid structure was fabricated by laser powder bed fusion (LPBF) for the treatment of infected bone defects, integrating mechanical performance, anti‐infective properties, and osteogenic requirements. In vitro, Zn‐0.8Li‐0.5Ag scaffold exhibits potent bactericidal property against Staphylococcus aureus ( S. aureus ) and Escherichia coli ( E. coli ), excellent anti‐inflammatory property through immunomodulation, and acceptable osteogenesis property by enhancing the expression of osteogenesis‐related genes. In vivo, the Zn‐0.8Li‐0.5Ag scaffold significantly suppresses pathogenic bacteria, alleviates local inflammation, and promotes tissue regeneration. RNA sequencing further elucidated that the Zn‐0.8Li‐0.5Ag scaffold exerted anti‐inflammatory effects by releasing Zn 2 + , Li + , and Ag + , which downregulated Gbp2 expression, thereby inhibiting inflammatory pathways. Collectively, the Zn‐0.8Li‐0.5Ag scaffold with antibacterial, anti‐inflammatory, and osteogenic effects holds great promise as a promising biomaterial for repairing infectious bone defects.

ABSTRACT The band gap tunability of halide perovskites underpins their exceptional photovoltaic and optoelectronic performance. However, rational band gap engineering remains challenging due to the complex interplay between multiple structural degrees of freedom. Conventional empirical descriptors like the tolerance factor fail to capture this complexity. Here, we report a universal symmetry‐based methodology to decode structure‐property relationships in lead halide perovskites. Integrating group theory with high‐accuracy DFT calculations, we deconstruct the Pnma structure into symmetry‐adapted distortions and quantify their individual impacts on the band gap, revealing opposing effects of octahedral tilts (band gap increase) and lattice strains (band gap decrease). These insights yield a tilt‐based structural descriptor that exhibits universal correlation with experimental band gaps across the lead halide perovskite family spanning diverse A‐site cations (inorganic/organic), crystal phases (orthorhombic/tetragonal), and halide compositions (I, Br, Cl) under compositional and pressure variations. The framework's predictive power is demonstrated through accurate forecasting of band gap evolution in pressure‐tuned CsPbI 3 and compositionally engineered solid solutions using a physical model that explicitly incorporates both tilt and strain mode contributions. Our approach transcends the limitations of empirical descriptors by establishing a rigorous, symmetry‐based foundation for rational perovskite design, thereby accelerating the development of next‐generation functional materials.

ABSTRACT Solution processing of mixed‐halide perovskites inevitably leads to inferior crystallinity and introduces undesired defects, arising from inhomogeneous ion mixing in the precursor solution or rapid solvent evaporation and uncontrollable nucleation/growth, thereby impairing both the power conversion efficiency (PCE) and long‐term stability of perovskite solar cells (PSCs). Here, we report a synergistic dual‐additive strategy utilizing potassium thiocyanate (KSCN) and potassium iodide (KI) to tailor the solution chemistry of perovskite precursors. The synergistic incorporation of thiocyanate ion (SCN − ), potassium ion (K + ), and iodide ion (I − ) optimizes the crystallization process through kinetics modulation, achieving multi‐site passivation via ionic interactions, thereby enabling high‐quality perovskite films and enhancing the optoelectronic performance of the devices. Consequently, we demonstrate a champion PCE of 26.09% for formamidinium‐cesium‐based single‐junction PSC with a high open‐circuit voltage ( V OC ) of 1.205 V, along with maintaining 90.8% of its initial efficiency after 500 h of continuous operation at 65°C under 1 sun illumination in ambient air. Crucially, this strategy is fully compatible with the fabrication of all‐perovskite tandem solar cells, empowering a high PCE of 28.76%.