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NanoManufacturing

Michael De Volder, Engineering Department - IfM
 
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Table of Contents for Advanced Materials. List of articles from both the latest and EarlyView issues.
Updated: 33 min 33 sec ago

Unlocking Grotthuss Proton Energy Storage in Pyrochlore‐Type Tungsten Oxide

Mon, 04/08/2025 - 14:22

A novel trace-Ni2+-implanted pyrochlore-type tungsten oxide is developed to showcase unique Grotthuss proton conduction abilities based on hydrogen-bonding topochemistry, which has realized ultrafast and stable electrochemical proton storage performance in aqueous proton batteries up to 500C.


Abstract

It is of momentous significance to identify suitable proton-storage electrode materials inherent with Grotthuss topochemistry toward high-power aqueous proton batteries. However, currently reported oxide electrode materials have seldom conformed to the Grotthuss mechanism. Here Grotthuss mechanism-dominated proton storage is showcased in a novel 3D-tunnel-structured pyrochlore-type WO3·0.5H2O (WOH), together with a reliable and effective approach to amplifying its Grotthuss conduction effect. Different from other phases of tungsten oxide (e.g., orthorhombic, monoclinic, and hexagonal), the zeolitic-water-enriched cubic pyrochlore WOH favors proton-hopping akin to “Newton's cradle” instead of traditional “vehicle-like” transport. Interestingly, introducing trace Ni(II) ions into the WOH (NWOH) is find to notably increase the content of structural water in lattice, thereby reframing the hydrogen-bonding network along with enhanced proton transfer capability as a consequence of its largely reduced activation energy as low as 0.08 eV. Hence, NWOH shows boosted reversible capacity of 71 mAh g−1 at 100C, ultrafast charging capability up to 500C, and ultralong cycling life over 30,000 cycles. Once coupled with Prussian blue analogue cathodes with identical Grotthuss conduction mechanism, the resultant high-output-voltage full-cells (≈1.1 V) sustain high-rate cycling with high energy/power density and operate at a wide working temperature from −20 to 50 °C.

Sacrificial‐Agent‐Triggered Mass Transfer Gating in Covalent Organic Framework for Hydrogen Peroxide Photocatalysis

Mon, 04/08/2025 - 14:21

A sacrificial-agent-triggered mass transfer gating (MTG) strategy reconfigures interfacial reactions for photocatalytic H2O2 generation in COFs. This enables precise switching of the dominant photocatalytic mechanism between surface-confined directional charge transfer pathways and diffusion-dominated redox processes. Mechanistic studies elucidate the ternary role of sacrificial agents as MTG regulators, effectively addressing inherent reaction constraints.


Abstract

Covalent organic framework (COF) photocatalysts for H2O2 production remain challenging by mass transport limitations and poor charge separation efficiency. Herein, a sacrificial agent-triggered mass-transfer gating (MTG) strategy is developed to reconfigure interfacial reaction for photocatalytic H2O2 generation via synthesized benzothiazole-COFs. This enables precise switching of the dominant photocatalytic mechanism between surface-confined directional charge transfer pathways and diffusion-dominated redox processes. Notably, benzyl alcohol (BA) enhances the mass transport and the catalytic site accessibility, scavenges photogenerated holes, and supplies protons for coupling reactions, thereby increasing the H2O2 yield of Tp-BTz COF to 100.9 mmol g−1 h−1 and achieving the outstanding photocatalytic performance reported to date. Both Tp-BTz COF and Tp-TTz COF demonstrate durably high H2O2 production efficiency even in the high-salinity seawater and municipal tap water systems. The generated H2O2 effectively degrades organic pollutants such as methyl orange (MO) and rhodamine B (RhB), demonstrating practical potential for wastewater treatment. The proposed gating strategy by introducing BA enables three synergistic functions: i) modulating interfacial reactions, ii) acting as a sacrificial agent to scavenge holes, and iii) supplying abundant protons (H+) for the oxygen reduction reaction (ORR) to facilitate the proton-coupled electron transfer. This approach establishes a generalizable paradigm for designing high-performance photocatalytic systems toward sustainable energy and environmental applications.

Electric Field‐Guided Ion Orchestration for Multi‐Chemistry Zinc Metal Batteries

Mon, 04/08/2025 - 14:21

An electric field-guided ion orchestration (EF-IO) strategy is developed to stabilize zinc metal batteries. By leveraging cation interfacial modifiers to reconfigure electric double layers and solvation configurations, the EF-IO design enables ultra-long cyclability and wide temperature adaptability. It also unlocks new reversible anion storage in high-voltage organic cathodes, advancing multi-chemistry zinc battery designs.


Abstract

While nonaqueous cosolvents alleviate hydrogen evolution reaction and dendritic growth in aqueous zinc (Zn) metal batteries (ZMBs), persistent H2O activity at Zn|electrolyte interfaces originating from unregulated ion distribution leads to premature failure. Here, an electric field-guided ion orchestration (EF-IO) strategy is proposed, leveraging cation interfacial modifiers to reconfigure electric double layers (EDLs) and solvation configurations. Interfacial simulations combined with experimental investigations verify that the ion-orchestrated-EDL synergistically diversifies Zn2+/Na+ solvation configurations and homogenizes localized electric fields, thereby forming an organic–inorganic gradient solid electrolyte interphase (SEI) that suppresses parasitic reactions. This enables dendrite-free Zn plating with 3400 h cyclability in Zn||Zn symmetric cells, while Zn||V10O24·12H2O full cells exhibit exceptional durability along with wide temperature adaptability (−45 to 55 °C). Crucially, this EF-IO strategy unlocks ClO4 −-based reversible anion storage in high-voltage organic cathodes. By bridging interfacial dynamics and multi-chemistry compatibility, this work establishes a promising paradigm for robust and versatile ZMBs.

Nonreciprocal Spin Waves in Nanoscale Hybrid Néel–Bloch–Néel Domain Walls Detected by Scanning X‐Ray Microscopy in Perpendicular Magnetic Anisotropic Fe/Gd Multilayers

Mon, 04/08/2025 - 14:20

Using scanning transmission X-ray microscopy, nonreciprocal spin-wave behavior is revealed in real space in Fe/Gd multilayers with perpendicular magnetic anisotropy, highlighting their functionality for magnonic logic circuits operating at GHz frequencies. Topological defects disrupt phase continuity while preserving nonreciprocity, demonstrating the potential of these domain walls as programmable magnonic waveguides for directed information flow.


Abstract

Spin wave nonreciprocity is crucial for signal processing in magnonic circuits. Domain walls (DWs) have been suggested as channels for nonreciprocal spin waves (magnons) with directional-dependent properties. However, the experimental investigations are challenging due to the low-damping magnetic material with DWs demanded and the nanoscale length scales involved. In this study, scanning transmission X-ray microscopy (STXM) is used to examine coherently-excited magnons when propagating in hybrid Néel-Bloch-Néel DWs in amorphous Fe/Gd multilayers with perpendicular magnetic anisotropy (PMA). Well-ordered lattices of stripe domains and DWs are created through the integration of Cobalt nanowire arrays. Their width is measured to be δDW = (60 ± 13) nm. Near 1 GHz magnons are detected with short wavelengths down to λ = (281 ± 44) nm which were channeled in the DWs. Consistent with micromagnetic simulations, the STXM data revealed a nonreciprocal magnon band structure inside the DWs. Bloch points are identified which disrupted the phase evolution of magnons and induced different λ adjacent to these topological defects. These observations provide direct evidence of nonreciprocal spin waves within hybrid Néel–Bloch–Néel DWs in PMA materials, serving as programmable waveguides in magnonic devices with directed information flow.

Selective Crystallization Delay in Wide‐Bandgap Perovskites Enables Initial Homogeneous Phase for Square Centimeter Perovskite/Organic Tandem Solar Cells

Mon, 04/08/2025 - 14:20

A mixed-halide perovskite film with initially homogeneous phase distribution is obtained by using 3-amino-5-fluorobenzamide additive, which selectively suppresses bromide precipitation during crystallization to mitigate halide phase segregation while demonstrating weak size dependence. The resulting 1.004-cm2 perovskite/organic tandem solar cells achieved a remarkable 25.21% power conversion efficiency, coupled with impressive operational stability maintaining ≈90% initial performance over 1500 h.


Abstract

Mixed halide wide-bandgap (WBG) perovskites, used in high-performance perovskite/organic tandem solar cells (TSCs), are prone to phase segregation under light irradiation. Particularly, the initial inhomogeneous halide phase distribution in WBG perovskites can accelerate the phase segregation under operational stressors, thus hindering scaling of TSCs that require high phase homogeneity. Here, a selective delayed crystallization strategy is proposed in which a functional agent (3-amino-5-fluorobenzamide; AFBA) is used to regulate the initial halide phase distribution. The -NH2 of AFBA, with a low electron-cloud density, shows a higher binding affinity with bromide than with iodide, thus selectively delaying the rapid crystallization of bromide; this phenomenon induces a homogeneous halide distribution across the film. The initial homogeneous film is phase-stable under operational stressors. As a result, the square-centimeter WBG perovskite front cell achieves a high efficiency of 18.61%. When stacked with organic subcells, the square-centimeter perovskite/organic TSC exhibits a remarkable efficiency of 25.21%, showing a weak-dependence of efficiency on size from 0.062 to 2.000 cm2, as well as a prolonged operational lifetime with a T 90 of 1500 h. Perovskite/organic TSCs are also connected in series with electrochromic devices to dynamically monitor the TSC performance via the color variation, providing insights for their future applications.

Gate‐Tunable Highly Linear Bipolar Photoresponse in Se@SWCNT Adaptive Neurons for Dynamically Programmable Neuromorphic Computing

Mon, 04/08/2025 - 14:16

This work presents a dynamically programmable synaptic transistor with a Se@SWCNT 1D van der Waals heterojunction, enabling both positive and negative responses via gate-tunable modulation. The transistor achieves high symmetry and linearity (R 2 > 0.99) in weight variation, demonstrating excellent performance across complex tasks, offering promising applications in brain-inspired optical neuromorphic systems with high accuracy.


Abstract

The development of tunable and highly controllable photoconductive devices for brain-inspired optical neuromorphic systems remains challenging. Previous neuromorphic devices are limited by asymmetric and nonlinear conductive properties, which impose specific restrictions on training tasks and weight learning rules in dynamic and complex visual environments. A programmable synaptic transistor based on a Se@SWCNT 1D van der Waals heterojunction, enabling gate-controlled positive and negative responses is presented. This approach eliminates the need for multilayer heterojunctions or complex circuits, simplifying array integration and wafer-scale fabrication. This phototransistor shows improved symmetry and linearity (R 2 > 0.99) in weight variation following optical stimulation, and simultaneously achieves linear persistent photoconductivity and negative photoconductivity with over 128 memory states, which is not reported previously. By adjusting light intensity and wavelength range, consistent weight rule processing across three tasks of increasing complexity is demonstrated. Notably, different visual tasks require distinct neural structures and decay rates. The proposed transistor facilitates transitions between bio-inspired brain regions via optical hybrid programming, adapting to dynamic visual environments. This innovation contributes significantly to brain-like computing and bio-inspired vision, due to its exceptional accuracy and dynamic switch models.

Iodine‐Mediated Redox Strategy for Sustainable Lithium Extraction From Spent LiFePO4 Cathodes

Fri, 04/07/2025 - 09:18

An iodine-mediated electrochemical strategy recycles spent LiFePO4 cathodes, extracting lithium as carbonate and producing metallic zinc. Delithiated LiFePO4 is transformed into an efficient oxygen evolution catalyst. This scalable, sustainable approach reduces energy use and emissions while offering economic benefits for clean energy applications.


Abstract

With the widespread application of lithium-ion batteries, the recycling of spent batteries, especially those involving LiFePO4 (LFP) cathodes for their low-cost and high safety, has become an urgent environmental and resource challenge. Traditional recycling methods (hydrometallurgy and pyrometallurgy) struggle to achieve green and efficient recycling. Herein, this study proposes an iodine-mediated electrochemical strategy to utilize a recyclable I3 −/I− redox system and efficiently extract Li+ from spent LFP through liquid-phase reactions on one side (achieving a 93% leaching rate and recovery as lithium carbonate), while simultaneously producing metallic zinc through electrodeposition, which can be directly used in Zn-air batteries or hydrogen production. Furthermore, the delithiated LFP is upcycled into an oxygen evolution reaction (OER) catalyst, achieving an overpotential of only 250 mV at 10 mA cm−2, superior to commercial RuO2 catalysts. Eventually, this system reduces energy consumption by 32% (9.2 MJ kg−1) compared to traditional hydrometallurgical processes, decreases greenhouse gas emissions by 35% compared to traditional pyrometallurgical processes, while achieving a net profit of ≈$0.44 per kg. This work establishes a novel, scalable recycling system, providing a robust sustainable solution for spent LFP cathodes recycling and clean energy storage.

Active‐Site‐Switching in Medium‐Entropy Metal Sulfides for Wide‐Temperature High‐Power Zn‐Air Pouch Cells

Fri, 04/07/2025 - 09:18

Flexible QZPCs formulated by the MES@CNT/CC air cathode and IL-PANa hydrogel electrolyte demonstrate a high cell-level energy density of 105 Wh kgcell −1, and an ultra-long cycle life of 4000 cycles at 5 mA cm−2 even at low temperature of −30 °C. The electronic synergy within the bifunctional MES@CNT/CC air cathode, initiates an intriguing adaptive active-site-switching catalytic mechanism during the reciprocating ORR and OER processes, thereby sustaining the high performance of the QZPCs.


Abstract

Quasi-solid-state Zn-air pouch cells (QZPCs) promise a high energy-to-cost ratio while ensuring inherent safety. However, addressing the challenges associated with exploring superior energy-wise cathode catalysts along with their activity origin, and the super-ionic electrolytes remains a fundamental task. Herein, the realistic high-performance QZPCs are contrived, underpinned by a robust NiVFeCo medium-entropy metal sulfides (MESs) bifunctional air cathode with a record-low potential polarization of 0.523 V, paired with a sodium polyacrylate-ionic liquid hydrogel exhibiting exceptional conductivity (234 mS cm−1) and water retention (93.8% at 7 days) at room temperature as the super-ionic conductor electrolyte. Through combined studies of in situ Raman, ex situ X-ray absorption fine structure analysis, and theoretic calculations, an intriguing adaptive active-sites-switching mechanism of the MESs cathode during discharging/charging processes is unveiled, revealing a dynamic role transition of Co and Ni active sites in the reversible oxygen electrocatalysis. Consequently, the persistent low cathode polarization and super ion-conductive electrolyte endorse QZPCs an excellent rate performance from 1 to 100 mA cm−2 at room temperature. Moreover, an impressively high cell-level energy density of 105 Wh kgcell −1 with an ultra-long cycle lifespan of 4000 cycles at 5 mA cm−2 and a low temperature of −30 °C is achieved.

Interfacial Energetics Reversal Strategy for Efficient Perovskite Solar Cells

Fri, 04/07/2025 - 09:18

A general strategy- “interfacial energetics reversal” to reconstruct perovskite energetics that matches well with the upper hole transport layer has been successfully developed, enabling efficient n–i–p perovskite solar cells with nonradiative recombination induced qVoc loss of only 57 meV from the radiative limit.


Abstract

Reducing heterointerface nonradiative recombination is a key challenge for realizing highly efficient perovskite solar cells (PSCs). Motivated by this, a facile strategy is developed via interfacial energetics reversal to functionalize perovskite heterointerface. A surfactant molecule, trichloro[3-(pentafluorophenyl)propyl]silane (TPFS) reverses perovskite surface energetics from intrinsic n-type to p-type, evidently demonstrated by ultraviolet and inverse photoelectron spectroscopies. The reconstructed perovskite surface energetics match well with the upper deposited hole transport layer, realizing an exquisite energy level alignment for accelerating hole extraction across the heterointerface. Meanwhile, TPFS further diminishes surface defect density. As a result, this cooperative strategy leads to greatly minimized nonradiative recombination. PSCs achieve an impressive power conversion efficiency of 25.9% with excellent reproducibility, and a nonradiative recombination-induced qV oc loss of only 57 meV, which is the smallest reported to date in n-i-p structured PSCs.

Key Role of Bridge Adsorbed Hydrogen Intermediate on Pt–Ru Pair for Efficient Acidic Hydrogen Production

Fri, 04/07/2025 - 09:18

The designed Pt atomic chain modified fcc-type Ru nanocrystal with co-crystalline structure possesses an efficient bridge adsorbed hydrogen configuration (*Hbridge) at the Pt–Ru(fcc) interface. The *Hbridge dominates HER and exhibits superior intrinsic activity, ≈10.6 times higher than that of Pt. The designed Pt–Ru(fcc) with *Hbridge demonstrates excellent catalytic activity and stability for both laboratory and industrial levels.


Abstract

Atop and multiple adsorbed hydrogen are considered as key intermediates on Pt-group metal for acidic hydrogen evolution reaction (HER), yet the role of bridge hydrogen intermediate (*Hbridge) is consistently overlooked experimentally. Herein, a Pt atomic chain modified fcc-Ru nanocrystal (Pt–Ru(fcc)) is developed with a co-crystalline structure, featuring *Hbridge intermediate bonded on the Pt–Ru pair site. Electrons leap from the pair site to *Hbridge facilitate hydrogen desorption, thus accelerating the Tafel kinetics and ensuring outstanding electrocatalytic performance, with a low overpotential (4.0 mV at 10 mA  cm−2) and high turnover frequency (56.4 H2 s−1 at 50 mV). Notably, the proton exchange membrane water electrolyzer PEMWE with ultra-low loading of 10 ugPt cm−2 shows excellent activity (1.61 V at 1.0 A cm−2) and low average degradation rate (4.0 µV h−1 over 1000 h), significantly outperforming the benchmark Pt/C. Furthermore, the PEMWE-based 80 µm Gore membrane under identical operating conditions requires only 1.54 and 1.58 V to achieve 1.0 and 1.5 A cm−2. This finding highlights the key role of *Hbridge at the Pt–Ru interface in obtaining high HER intrinsic activity and underscores the transformative potential in designing next-generation bimetallic catalysts for clean hydrogen energy.

Soft Extrudable Dendritic Particles with Nanostructured Tendrils for Local Adhesion and Drug Release to Bladder Cancers

Fri, 04/07/2025 - 08:56

Soft dendritic particles (SDPs) made of biodegradable polymers and small-molecule drugs are manufactured using a fluid flow templating method. In alginate gels, extruded SDPs sustainably adhere on tumor sites and selectively kill cancer cells. Intravesical instillation of SDPs in tumor-bearing mouse bladders triggers a CD45+ immune response with minimal toxicity, highlighting their potential for targeted cancer therapy.


Abstract

Bladder cancer is a leading cause of cancer-related mortality, yet current intravesical drug delivery methods often suffer from poor retention times in the bladder. Gecko feet-like nanomaterials offer the potential to overcome this challenge, however, conventional methods to fabricate high surface area nanomaterials for drug delivery involve complex and expensive manufacturing processes. In this work, a simple fluid flow templating method is reported for manufacturing soft dendritic particles (SDPs) composed of poly(lactic-co-glycolic acid) (PLGA) with a chitosan coating for enhanced adhesion to epithelial tissues via van der Waals interactions. The biodegradable SDPs encapsulate chemotherapeutic agents and are administered using an alginate hydrogel, enabling precise deposition by extrusion for sustained drug release. The results demonstrate that SDPs adhere to mouse and human cancer cells for several days. The SDPs effectively encapsulate and release several clinically utilized chemotherapeutic drugs such as gemcitabine, docetaxel, and methotrexate, exhibiting superior cancer cell killing in vitro. In murine models, gemcitabine-loaded SDPs instilled into tumor-bearing bladders elicited stronger CD45+ immune cell responses than control groups while maintaining minimal toxicity. This work presents a simple, biomimetic drug delivery platform with prolonged retention and controlled drug release, offering a versatile approach for enhancing therapeutic delivery in epithelial cancer models.

Valence and Site Engineering Enable Efficient Broadband Near‐Infrared Emission at 960 nm in Cr3+‐Activated Forsterite

Fri, 04/07/2025 - 08:56

This study reports a near-infrared (NIR) luminescent material (Mg2SiO4:1.5%Cr,5%Li) with efficient (EQE = 48%) ultra-broadband (FWHM ≈ 2413 cm−1 (226 nm)) NIR emission at 960 nm upon blue-light excitation. This innovation addresses the low efficiency of long-wavelength (λmax > 900 nm) NIR-emitting materials due to the radiationless de-activation and the low absorption efficiency of Cr3+ activators.


Abstract

Near-infrared (NIR) light sources hold great potential for applications in night vision illumination, bio-imaging, and non-destructive testing. However, radiationless de-activation and low absorption restrict the development of high-efficiency blue light excitable NIR phosphors, especially for emissions beyond 900 nm. Herein we report a high-performance Cr3+-activated forsterite (Mg2SiO4:1.5%Cr3+, 5%Li+) phosphor exhibiting broadband NIR emission peaking at 960 nm with a record external quantum efficiency (EQE) up to 48%. The introduction of Li+ as a charge compensator and symmetry distorter not only suppresses Cr4+ formation but also enhances the cross section of Cr3+ d-d forbidden transitions in Mg2SiO4. More importantly, Li+ promotes excited-state energy transfer between Cr3+ emitters, yielding exceptional thermal stability and external quantum efficiency. A fabricated NIR phosphor-converted light-emitting diode (LED) achieved a NIR radiated power of 356 mW (at a driving current of 700 mA) and an electro-optical conversion efficiency up to 12.9% (at 100 mA). This work unlocks new possibilities for smart spectroscopy applications, from non-destructive testing to human angiography and biometric recognition.

Engineering a Lipid Nanoparticle with Atypical Calcium Crystal Structure for Enhanced IFNβ‐Mediated Immunotherapy

Thu, 03/07/2025 - 09:24

The engineered lipid nanoparticles (NanoCa) demonstrate potent anti-tumor effects by activating type I interferons, promoting the maturation of dendritic cells, and enhancing antigen presentation.


Abstract

Immune checkpoint inhibitors have revolutionized cancer therapy; however, many patients exhibit suboptimal responses, which is due to inadequate T cell priming by the innate immune response. Metal ions play a critical role in modulating the innate immune response. However, the mechanisms by which metal ions facilitate dendritic cell maturation through the activation of interferon remain poorly understood. This research identifies a nanomaterial Calcium phosphate-containing liposome (NanoCa), characterized by an atypical crystal structure and pH-responsive profile. NanoCa promotes bone marrow-derived dendritic cell maturation and exhibits antiviral effects and anti-tumor properties in different tumor models. Also, NanoCa acts as an immunostimulant by fostering antibody production. Furthermore, when combined with programmed cell death 1 receptor (PD-1)  blocking antibodies, NanoCa synergistically enhances anti-tumor efficacy in CT26 models. Mechanistically, NanoCa rapidly releases Ca2+ via the lysosome pathway post-endocytosis, subsequently triggering interferon through the Ca2+-calcineurin (CaN) - nuclear factor of activated T cells 2 (NFATc2) - protein kinase C beta (PKCβ) - interferon regulatory factor 3 (IRF3) signal pathway. Single-cell RNA sequencing (scRNA-seq) shows NanoCa increases the population of tumoral infiltrating dendritic cell (DC), C1qc+ TAM, and CD8T_eff cells and decreases the CD8T_ex and immunosuppressive SPP1+ TAM population in tumor-draining lymph nodes. Overall, NanoCa shows translational potential for anti-tumor immune therapeutics.

1D Van Der Waals Superlattices for Polarization‐Sensitive Photodetectors

Thu, 03/07/2025 - 09:23

1D PbI2 superlattice are synthesized utilizing an antisolvent diffusion method, in which demonstrates in-plane anisotropic phonon vibrations and optical transport characteristics. Leveraging on the anisotropic optical transport nature and effective coupling with vdWMs, filter-free polarization-sensitive photodetector comprising vdWMs and PbI2 superlattice waveguide are realized in a broad spectra range with linear dichroism ratio values of 1.43–1.73.


Abstract

The ability to detect polarimetric information of light over a broad spectra range is central to practical optoelectronic applications and has been successfully demonstrated with photodetectors of low-symmetry 2D van der Waals materials (vdWMs). However, polarization sensitivity within such a photodetectors remains elusive due to the limited diversity. To address this challenge, an approach is proposed by transforms 2D Lead iodine (PbI2) into 1D superlattice microwires (SLMs) through a solution-phase antisolvent diffusion method. This structural shifting enables the creation of low-symmetry crystal characteristics, a well-defined geometric microcavity structure, and an increased bandgap, which collectively confer anisotropic waveguide properties across visible and near-infrared wavelengths. By integrating PbI2 SLMs with isotropic 2D vdWMs, that waveguide-integrated photodetectors are demonstrated capable of polarization detection, achieving linear dichroism ratio (LDR) values of 1.66 at 405 nm for PbI2 photodetectors and 1.73 at 785 nm for WSe2 photodetectors. This paradigm-shifting strategy enables polarimetric information detection using isotropic vdWMs and advances the development of next-generation polarization-resolved optoelectronic devices.

Adaptive Stress Response in 2D Graphene@Se Composite toward Ultra‐Stable All‐Solid‐State Lithium‐Selenium Batteries

Thu, 03/07/2025 - 09:23

The accumulation of stress leads to electrochemical-mechanical degradation, resulting in rapid capacity loss of solid-state batteries. A stress-adaptive graphene@selenium cathode is developed in this work to enhance ion transport and relieve mechanical stress in all-solid-state lithium-selenium batteries, enabling superior electrochemical performance.


Abstract

All-solid-state lithium-selenium batteries (ASSLSeBs) offer high energy density and improved safety for next-generation energy storage. Still, selenium cathodes suffer from large volume changes during cycling, leading to mechanical stress and rapid capacity fade. To address this, a stress-adaptive 2D graphene@Se composite cathode is developed, where small Se nanoparticles are anchored onto acid-treated expanded graphite (AcEG) to enhance charge transport and alleviate stress. Mechanical characterization confirms that the composite effectively mitigates Li-ion-induced strain. As a result, ASSLSeBs with this cathode achieve exceptional cycling stability with ultrahigh capacity retention after 4000 cycles at 2 C and stable performance for over 400 cycles even under high active-material loading. Furthermore, an all-solid-state Li-Se pouch cell with a record energy density of 376.8 Wh kg⁻¹ is demonstrated, the highest reported for ASSLSeBs. This work presents a strategy for designing stress-adaptive cathodes, enabling ultra-stable ASSLSeBs for practical applications.

Self‐Evolving Discovery of Carrier Biomaterials with Ultra‐Low Nonspecific Protein Adsorption for Single Cell Analysis

Thu, 03/07/2025 - 07:34

A self-evolving discovery integrating automation and AI is developed to address the high-dimensional-parameter-space challenge in carrier biomaterials. The discovered biomaterials showed ultra-low nonspecific protein adsorption, achieving a 10 000-fold reduction in experiment workload; and they are further fabricated into microfluidic-used carriers for protein-analysis applications, showing a 9-fold enhancement in detection sensitivity. This study has potential for applications in single-cell analysis.


Abstract

Carrier biomaterials used in single-cell analysis face a bottleneck in protein detection sensitivity, primarily attributed to elevated false positives caused by nonspecific protein adsorption. Toward carrier biomaterials with ultra-low nonspecific protein adsorption, a self-evolving discovery is developed to address the challenge of high-dimensional parameter spaces. Automation across nine self-developed or modified workstations is integrated to achieve a “can-do” capability, and develop a synergy-enhanced Bayesian optimization algorithm as the artificial intelligence brain to enable a “can-think” capability for small-data problems inherent to time-consuming biological experiments, thereby establishing a self-evolving discovery for carrier biomaterials. Through this approach, carrier biomaterials with an ultra-low nonspecific protein adsorption index of 0.2537 are successfully discovered, representing an over 80% decrease, while achieving a 10 000-fold reduction in experiment workload. Furthermore, the discovered biomaterials are fabricated into microfluidic-used carriers for protein-analysis applications, showing a 9-fold enhancement in detection sensitivity compared to conventional carriers. This is the very demonstration of a self-evolving discovery for carrier biomaterials, paving the way for advancements in single-cell protein analysis and further its integration with genomics and transcriptomics.

Stochastic Orientational Encoding via Hydrogen Bonding Driven Assembly of Woven‐Like Molecular Physically Unclonable Functions

Thu, 03/07/2025 - 07:23

This study presents a novel stochastic orientational encoding approach utilizing a nanoscopic film of a novel rod-shaped π-architecture, achieved through facile ambient-atmosphere solution processing. Energetically favorable molecular assembly, driven by directional multiple hydrogen-bonding motifs and uniaxial microcrystal growth, results in a woven-textured pattern with random 1D features. The rich variations in microcrystal domain properties and crystal orientations coupled with artificial coloration enable high encoding capacity in a single-material, solution-processed system.


Abstract

The prevention of counterfeiting and the assurance of object authenticity require stochastic encoding schemes based on physically unclonable functions (PUFs). There is an urgent need for exceptionally large encoding capacities and multi-level responses within a molecularly defined, single-material system. Herein, a novel stochastic orientational encoding approach is demonstrated using a facile ambient-atmosphere solution processing of a molecular thin film based on the rod-shaped oligo(p-phenyleneethynylene) (OPE) π-architecture. The nanoscopic film, derived from the small molecule 2EHO-CF3PyPE with donor, acceptor, and π-spacer building units, is designed for energetically favorable uniaxial molecular assembly and crystal growth via directional multiple hydrogen-bonding motifs at the molecular termini and short C─H···π contacts at the center. A facile solvent vapor annealing induces concurrent dewetting and microscopic 1D random crystallization, yielding a woven-textured random features. Using convolutional neural networks, the rich variations in microcrystal domain properties and stochastic encoding of 1D crystal orientations generate artificial coloration, achieving an encoding capacity reaching (6.5 × 10⁴)(2752 × 2208). The results demonstrate an effective strategy for achieving ultrahigh encoding capacities in a thin film composed of a single-material. This approach enables low-cost, solution-processed fabrication for mass production and broad adoption, while opening new opportunities to explore molecular-PUFs through structural design and engineering noncovalent interactions.

Observation of Z2 Non‐Hermitian Skin Effect in Projective Mirror‐Symmetric Acoustic Metamaterials

Thu, 03/07/2025 - 07:21

A symmetry-protected Z₂ non-Hermitian skin effect (NHSE) is experimentally demonstrated in acoustic metamaterials. By implementing projective mirror symmetry—which enables pseudospins in spinless systems—both uniform and bidirectional Z₂ NHSEs characterized by different accumulation directions are observed. Active feedback circuits provide the requisite non-Hermitian gain/loss, establishing a platform for topological wave manipulation.


Abstract

Non-Hermitian skin effect (NHSE), where eigenstates localize at the boundary of non-Hermitian lattices, has gained significant attention in various fields. This phenomenon, driven by the point-gap topology of complex energy bands, occurs even without special symmetries. Nevertheless, additional symmetry may significantly enrich the NHSE. Notably, time-reversal symmetry protects a Z2 NHSE, featuring oppositely accumulated skin modes. Here, a 1D bilayer Z2 NHSE model based on projective mirror symmetry is proposed, making Z2 NHSE possible in spinless systems. Experimentally, both uniform and bidirectional Z2 NHSEs are observed in acoustic metamaterials, where the necessary non-Hermitian elements—gain and loss—are achieved through active feedback circuits. These findings open new avenues for exploring symmetry-enriched non-Hermitian topological phenomena and pave the way for potential applications in wave manipulation, sensing, and beyond.

Nanocrystal‐Nucleus Template Strategy for Efficient Wide‐Bandgap Perovskite Solar Cells with Enhanced Homogeneity and Energy‐Level Alignment

Thu, 03/07/2025 - 07:20

A nanocrystal-nucleus template strategy addresses nanoscale phase separation and energy-level mismatch in wide-bandgap perovskite solar cells. By tailoring nanocrystals to match the target perovskite's composition and structure, this approach enables uniform halide distribution, enhanced crystallization, and improved electron extraction. The strategy achieves 23.4%-efficient PSCs (1.68 eV) with a record V OC of 1.30 V and certified 31.7%-efficient perovskite/silicon tandem solar cells.


Abstract

Wide-bandgap (WBG) perovskite solar cells (PSCs) are critical for advancing tandem solar cell efficiencies, yet suffer from severe photovoltage deficits and halide segregation, substantially degrading their performance and stability. Here, a nanocrystal-nucleus template (NCNT) strategy is developed to directly addresses heterogeneous nucleation—the root cause of phase separation—by precisely matching the I/Br ratio of nanocrystal to that of the target perovskite film. This approach guides homogeneous assembly of Pb-I/Br octahedra, achieving exceptional halide uniformity and precise crystallization control for WBG films. The NCNT simultaneously induces p-type doping and reduces the perovskite/C60 interfacial energy barrier, significantly enhancing charge extraction. Remarkably, 1.68-eV WBG PSCs fabricated via this approach achieve a record open-circuit voltage (VOC) of 1.30 V, alongside a champion efficiency of 23.4%. The broad applicability of this strategy is demonstrated across a wide bandgap range of 1.63–1.76 eV, all exhibiting (001)-preferred orientation and exceptional photostability. When integrated into a 0.945 cm2 monolithic perovskite/silicon tandem solar cell, the NCNT-based device delivers a high efficiency of 32.0% (certified 31.7%). This work highlights the pivotal role of nanocrystals in regulating perovskite crystallization, resolves long-standing VOC limitations in WBG perovskites, and establishes a scalable platform for next-generation optoelectronic devices and tandem photovoltaics.

Superblack Carbon Hierarchitectures for Multispectral Absorption

Wed, 02/07/2025 - 09:35

Superblack carbon hierarchitectures are developed through synergistic cross-dimensional engineering that integrates physical structuring with chemical modification, enabling high-performance multispectral absorption across visible, infrared, and microwave regimes simultaneously. Carbon microparticles with a fractal dimension approaching 1.0, or those possessing a networked structure, inherently offer advantages in achieving broad and strong multispectral responses.


Abstract

Multispectral absorbing materials that can efficiently dissipate waves across the visible, infrared, and microwave regimes have long been pursued for advanced applications in fields such as space exploration, stealth, and camouflage. However, the wide range of incident wavelengths, spanning five orders of magnitude, presents a significant challenge for the practical implementation of multispectral absorbers. Herein, superblack carbon hierarchitectures (SCHs) are designed using a bottom-up approach involving the self-assembly and self-sacrifice of hydrogen-bonded organic frameworks (HOFs), realizing synergistic morphological customization and dielectric gene editing (via carbon nitride like-moieties conjugated with C═C short chains). Through the cross-dimensional coupling action between light-trapping hierarchitecture and robust dielectric loss, superb visible light absorption (>99.6%), high infrared absorption (98.5%/97.5%/99.6% for long-/mid-/short-wavelength infrared regimes), and ultrabroad microwave absorption (effective bandwidth of 8.52 GHz, nearly covering both the X and Ku bands) can be simultaneously achieved in monolayer SCHs-based absorbers. Furthermore, the topologically transformed structures of SCHs enable a systematic dissection of the longstanding ambiguity surrounding the geometrical effect, revealing the synergistic influence of fractal dimension and interconnection status of microparticles, particularly in the microwave regime. This work introduces a new paradigm for multispectral absorption and advances the understanding of absorption mechanisms for developing next-generation absorbers.

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