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Self-Assembled Monolayers in p-i-n Perovskite Solar Cells: Molecular Design, Interfacial Engineering, and Machine Learning-Accelerated Material Discovery. p-i-n钙钛矿太阳能电池中的自组装单层:分子设计、界面工程和机器学习加速材料发现。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202520220
Asmat Ullah, Ying Luo, Stefaan De Wolf

Self-assembled monolayers (SAMs) have precipitated a paradigm shift in the design of hole transport layers (HTLs) for p-i-n perovskite solar cells, emerging as the cornerstone of modern, high-efficiency devices. This review comprehensively charts the evolution of SAM-based HTLs from fundamental molecular-level insights to their pivotal role in commercial-scale applications and record-breaking perovskite/silicon tandem cells. We delve into the intricate structure-property-performance relationships that govern SAMs' function, examining how meticulous engineering of anchoring groups, π-bridges, and functional headgroups dictates critical features such as energy level alignment, interfacial defect passivation, and perovskite crystallization control. The discussion extends beyond champion efficiencies to critically assess the scalability of deposition techniques, the limitations of operational stability under real-world conditions, and the pathways for integration into tandem architectures. Furthermore, we highlight the transformative potential of machine learning in accelerating the discovery and optimization of next-generation SAM materials. Finally, we provide a forward-looking perspective on molecular design strategies required to overcome existing challenges and fully unlock SAM potential for stable, high-performance photovoltaics.

自组装单层(sam)已经促成了p-i-n钙钛矿太阳能电池空穴传输层(HTLs)设计的范式转变,成为现代高效设备的基石。本文全面回顾了基于sam的HTLs的发展,从基本的分子水平的见解到它们在商业规模应用和破纪录的钙钛矿/硅串联电池中的关键作用。我们深入研究了控制sam功能的复杂结构-性能-性能关系,研究了锚定基团,π桥和功能头基团的细致工程如何决定了诸如能级排列,界面缺陷钝化和钙钛矿结晶控制等关键特性。讨论超越了冠军效率,批判性地评估了沉积技术的可扩展性,实际条件下操作稳定性的局限性,以及集成到串联架构中的途径。此外,我们强调了机器学习在加速发现和优化下一代SAM材料方面的变革潜力。最后,我们提供了前瞻性的分子设计策略,以克服现有的挑战,并充分释放稳定,高性能光伏电池的SAM潜力。
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引用次数: 0
Organic Radical Accelerates Charge Carrier Funneling in Quasi-2D Perovskite LEDs. 有机自由基加速准二维钙钛矿led中的载流子漏斗。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202517839
Hongkang Xu, Tianle Fan, Zihao Zhu, Alim Abdurahman, Boning Wu, Wenming Tian, Jonghee Yang, Wenzhe Li, Meiqin Xiao, Simin Gong, Ping Chen

Quasi-2D metal halide perovskites (MHP) have emerged as promising candidates for light-emitting diodes (PeLEDs) due to their intrinsic advantages in color purity, bandgap tunability, and stability. The prime working principle realizing high radiative emission in quasi-2D MHP is the ultrafast, consecutive charge transfer (CT) process toward the low-bandgap crystallites across multiple quantum wells, called charge carrier funneling. Ironically, such a key process is intrinsically limited in the quasi-2D MHP by the molecular spacers, which have electronically insulating natures. To challenge this limit, herein, we explore the impact of a judiciously designed, stable, and conductive organic radical, (5H-pyrido[3,2-b]indole-2,6-dichlorophenyl)bis(2,4,6-trichlorophenyl)methyl as a molecular additive in the MHP matrix. It is found that the spatially delocalized singly occupied molecular orbital offers an electronic bridge accelerating interfacial CT and the carrier funneling by surface adsorption, thus maximizing radiation recombination yield. As a result, the radical-incorporating PeLEDs (peaking at ≈ 684 nm) achieve a remarkable external quantum efficiency of 26.8% with an operational half-lifetime of ≈ 340 min, ranking among the best deep-red devices reported to date. This work demonstrates that rational radical molecular design offers a powerful route to resolve intrinsic CT limitations in quasi-2D MHP, unlocking both high efficiency and long-term stability in next-generation PeLEDs.

准二维金属卤化物钙钛矿(MHP)由于其在颜色纯度、带隙可调性和稳定性方面的固有优势而成为发光二极管(PeLEDs)的有前途的候选者。在准二维MHP中实现高辐射发射的主要工作原理是跨多个量子阱向低带隙晶体的超快、连续电荷转移(CT)过程,称为电荷载流子漏斗。具有讽刺意味的是,这种关键过程在准二维MHP中受到具有电子绝缘性质的分子间隔剂的内在限制。为了挑战这一限制,本文探讨了一种精心设计的、稳定的、导电的有机自由基(5h -吡啶[3,2-b]吲哚-2,6-二氯苯基)和(2,4,6-三氯苯基)甲基作为分子添加剂在MHP基质中的影响。发现空间离域的单占据分子轨道提供了一个电子桥,加速了界面CT和载流子的表面吸附漏斗,从而最大化了辐射复合收率。结果表明,结合自由基的peled(峰值约为684 nm)实现了26.8%的外量子效率,工作半衰期约为340 min,是迄今为止报道的最好的深红色器件之一。这项工作表明,合理的自由基分子设计为解决准二维MHP固有的CT限制提供了一条强有力的途径,从而实现了下一代peds的高效率和长期稳定性。
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引用次数: 0
Mild Coordination Enabled by Steric Hindrance Facilitates Fabrication of Large-Area Perovskite Solar Modules. 空间位阻的温和配位促进了大面积钙钛矿太阳能组件的制造。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202521181
Jialiang Liu, Mengjie Li, Jun Ji, Zhiguo Zhao, Meicheng Li

The scalable fabrication of high-efficiency perovskite solar modules is critically challenged by the difficulty in controlling crystallization homogeneity and mitigating buried interfacial defects across large-area substrates. The commonly used dimethyl sulfoxide (DMSO) can induce heterogeneous nucleation and is prone to remain trapped within the films. Herein, diethyl sulfoxide (DESO) is introduced, a volatile Lewis acid-base additive that leverages steric hindrance effects from its branched-chain structure to achieve mild coordination with PbI2. This structural feature reduces the binding energy between DESO and PbI2, which avoid the formation of complex metastable intermediate phases. Moreover, the low binding energy of DESO enables its complete removal during vacuum quenching via rapid evaporation, effectively suppressing void formation at the buried interfaces during the subsequent annealing. The resultant perovskite films yield perovskite solar modules (PSMs) with power conversion efficiencies (PCEs) of 22.9% (11.2 cm2, aperture area) and 20.8% (692 cm2, aperture area) via scalable processes. These devices exhibit operational stability, retaining >96% of their initial PCE after 2000 h under continuous 1-sun illumination and >95% PCE following 2000 h damp-heat testing (85°C/85% RH).

高效钙钛矿太阳能组件的可扩展制造面临着难以控制结晶均匀性和减轻大面积衬底上的埋藏界面缺陷的严峻挑战。常用的二甲基亚砜(DMSO)可以诱导非均相成核,并且容易被困在薄膜内。本文介绍了二乙基亚砜(DESO),这是一种挥发性路易斯酸碱添加剂,利用其支链结构的空间位阻效应与PbI2实现温和配位。这种结构特征降低了DESO与PbI2之间的结合能,避免了复杂亚稳中间相的形成。此外,DESO的低结合能使其在真空淬火过程中通过快速蒸发完全去除,有效地抑制了后续退火过程中埋藏界面处的空洞形成。所得到的钙钛矿薄膜通过可扩展工艺生产的钙钛矿太阳能组件(psm)的功率转换效率(pce)分别为22.9% (11.2 cm2,孔径面积)和20.8% (692 cm2,孔径面积)。这些器件表现出工作稳定性,在连续1个太阳照射2000小时后保持>96%的初始PCE,在2000小时湿热测试(85°C/85% RH)后保持>95%的PCE。
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引用次数: 0
Sensitive Shortwave Infrared Organic Photodetectors Enabled by Nonfullerene Acceptor Featuring an Ultralow Optical Bandgap of Less than 1.0 eV. 具有小于1.0 eV的超低带隙的非富勒烯受体实现的灵敏短波红外有机光电探测器。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202520509
Yingqi Zheng, Lixiang Wang, Yongjie Chen, Zhong-Ze Qu, Yanjun Fang, Yi Lin, Zheng Tang, Wuyue Liu, Yunlong Guo, Thuc-Quyen Nguyen, Xiaozhang Zhu

Shortwave infrared (SWIR) photodetectors are in high demand in modern applications, including night surveillance, biological imaging, and optical communication. Emerging organic semiconductors, featuring a tailorable spectral response and solution processability, open new avenues for SWIR light detection. However, SWIR organic photodetectors (OPDs) suffer from a scarcity of ultralow-bandgap organic semiconductors and low responsivity above 1000 nm. Here, we report a new electron-rich building block, thieno[3',2':4,5]cyclopenta[1,2-b]thieno[2,3-d]pyrrole (SNCS), that exhibits strong electron-donating ability. By applying acceptor-donor-acceptor and acceptor-quinoidal-donor-quinoidal-acceptor strategy, we developed two new nonfullerene acceptors: SNCS-4F and SNCSTT-4F. The latter, with thieno[3,4-b]thiophene moiety, exhibits strong SWIR absorption up to 1400 nm in thin films. The best-performing PTB7-Th:SNCSTT-4F-based OPD exhibits a record external quantum efficiency of 50.2%, a responsivity of 0.49 A W-1 and remarkable specific detectivity of 4.47 × 1012 Jones at 1200 nm under zero bias. This is the highest performance among reported SWIR organic photodiodes and is comparable with commercial InGaAs photodetectors. Ultraviolet photoelectron spectra, Mott-Schottky analysis and trap density of states analysis were applied to evaluate the OPDs' performances. Finally, we demonstrate that the OPDs can detect SWIR light with high sensitivity in photoplethysmography measurements and infrared audio communication applications.

短波红外(SWIR)光电探测器在现代应用中有很高的需求,包括夜间监视,生物成像和光通信。新兴的有机半导体具有可定制的光谱响应和溶液可加工性,为SWIR光检测开辟了新的途径。然而,SWIR有机光电探测器(opd)受到超低带隙有机半导体的缺乏和1000 nm以上的低响应率的困扰。在这里,我们报道了一种新的富电子构建块-噻吩[3',2':4,5]环penta[1,2-b]噻吩[2,3-d]吡咯(SNCS),它具有很强的给电子能力。采用受体-供体-受体和受体-喹酮-供体-喹酮-受体策略,我们开发了两个新的非富勒烯受体:SNCS-4F和SNCSTT-4F。后者具有噻吩[3,4-b]部分,在薄膜中表现出强烈的SWIR吸收,最高可达1400 nm。性能最好的基于PTB7-Th: sncstt - 4f的OPD具有创纪录的50.2%的外量子效率,0.49 a W-1的响应率和4.47 × 1012 Jones的零偏置下1200 nm比检出率。这是目前报道的SWIR有机光电二极管中性能最高的,与商用InGaAs光电探测器相当。应用紫外光电子能谱、Mott-Schottky分析和阱态密度分析对opd的性能进行了评价。最后,我们证明了opd可以在光体积脉搏波测量和红外音频通信应用中以高灵敏度检测SWIR光。
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引用次数: 0
Dynamic Electron-Hole Shuttle at Atomic Interfaces for Solar-Driven H2O2 and Benzaldehyde Coproduction. 太阳能驱动H2O2和苯甲醛协同生产的原子界面动态电子-空穴穿梭。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202522711
Jugong Shi, Xunlu Wang, Molly Meng-Jung Li, Jiacheng Wang, J Paul Attfield, Ye Zhu, Minghui Yang

Harnessing solar energy to produce value-added chemicals simultaneously requires the critical step of spatially separating redox processes. However, conventional photocatalysts remain fundamentally constrained by sluggish charge dynamics and irreversible recombination. Here, we propose an atomic-level interfacial shuttle mechanism in sub-nanometer gold cluster-anchored nickel manganite (H-NiMn2O4-β/Au0.5 NCs), which couples dynamic electron-hole separation with Ni3+/Ni2+ redox cycling. Ultrafast transient absorption spectroscopy indicates electron transfer occurring within 3.06 ps, mediated by an Au-O-Ni coordination interface. In this system, Ni3+ functions as a transient electron trap, undergoing rapid reduction to Ni2+ and subsequently transferring electrons to adjacent Au clusters, accelerating charge kinetics by 22.16-fold. This atomic-scale electron relay selectively steers 2e- oxygen reduction by balancing *OOH intermediate stabilization and desorption, yielding H2O2 at 1.00 mmol g-1 h-1. Simultaneously, hole accumulation on lattice oxygen drives α-H abstraction, enabling photooxidation of benzyl alcohol to benzaldehyde (14.59 mmol g-1 h-1). This work presents a dynamic dual-site catalysis model, offering atomic-level insight into interfacial charge management for solar-driven redox transformations.

利用太阳能同时生产增值化学品需要空间分离氧化还原过程的关键步骤。然而,传统的光催化剂仍然受到缓慢的电荷动力学和不可逆重组的限制。在这里,我们提出了亚纳米金簇锚定镍锰矿(H-NiMn2O4-β/Au0.5 NCs)中原子水平的界面穿梭机制,该机制将动态电子空穴分离与Ni3+/Ni2+氧化还原循环耦合在一起。超快瞬态吸收光谱表明,电子转移发生在3.06 ps内,由Au-O-Ni配位界面介导。在该体系中,Ni3+作为一个瞬态电子陷阱,快速还原为Ni2+,随后将电子转移到相邻的Au团簇,将电荷动力学加速22.16倍。这种原子级电子继电器通过平衡OOH中间体稳定和解吸,选择性地控制2e-氧还原,产生1.00 mmol g-1 h-1的H2O2。同时,晶格氧上的空穴积累驱动α-H萃取,使苯甲醇光氧化生成苯甲醛(14.59 mmol g-1 h-1)。这项工作提出了一个动态的双位点催化模型,为太阳能驱动的氧化还原转化的界面电荷管理提供了原子水平的见解。
{"title":"Dynamic Electron-Hole Shuttle at Atomic Interfaces for Solar-Driven H<sub>2</sub>O<sub>2</sub> and Benzaldehyde Coproduction.","authors":"Jugong Shi, Xunlu Wang, Molly Meng-Jung Li, Jiacheng Wang, J Paul Attfield, Ye Zhu, Minghui Yang","doi":"10.1002/adma.202522711","DOIUrl":"https://doi.org/10.1002/adma.202522711","url":null,"abstract":"<p><p>Harnessing solar energy to produce value-added chemicals simultaneously requires the critical step of spatially separating redox processes. However, conventional photocatalysts remain fundamentally constrained by sluggish charge dynamics and irreversible recombination. Here, we propose an atomic-level interfacial shuttle mechanism in sub-nanometer gold cluster-anchored nickel manganite (H-NiMn<sub>2</sub>O<sub>4-β</sub>/Au<sub>0.5</sub> NCs), which couples dynamic electron-hole separation with Ni<sup>3+</sup>/Ni<sup>2+</sup> redox cycling. Ultrafast transient absorption spectroscopy indicates electron transfer occurring within 3.06 ps, mediated by an Au-O-Ni coordination interface. In this system, Ni<sup>3+</sup> functions as a transient electron trap, undergoing rapid reduction to Ni<sup>2+</sup> and subsequently transferring electrons to adjacent Au clusters, accelerating charge kinetics by 22.16-fold. This atomic-scale electron relay selectively steers 2e<sup>-</sup> oxygen reduction by balancing *OOH intermediate stabilization and desorption, yielding H<sub>2</sub>O<sub>2</sub> at 1.00 mmol g<sup>-1</sup> h<sup>-1</sup>. Simultaneously, hole accumulation on lattice oxygen drives α-H abstraction, enabling photooxidation of benzyl alcohol to benzaldehyde (14.59 mmol g<sup>-1</sup> h<sup>-1</sup>). This work presents a dynamic dual-site catalysis model, offering atomic-level insight into interfacial charge management for solar-driven redox transformations.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e22711"},"PeriodicalIF":26.8,"publicationDate":"2026-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146130576","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tailored Redox-Active Catholytes Enabling High-Rate and High-Loading All-Solid-State Lithium-Sulfur Batteries. 定制氧化还原活性阴极,实现高倍率和高负载全固态锂硫电池。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202513204
Jingui Yang, Ruizhuo Zhang, Ramon Zimmermanns, Mareen Schaller, Sylvio Indris, Jaehoon Choi, Simon Fleischmann, Torsten Brezesinski, Florian Strauss

All-solid-state lithium-sulfur batteries (ASSLSBs) hold great promise for next-generation electrochemical energy storage due to sulfur's high theoretical specific capacity and low cost. However, sluggish sulfur conversion kinetics and severe volume variations during cycling, as well as poor ionic percolation in composite cathodes, limit their practical viability. To overcome these challenges, we herein introduce solid electrolytes of nominal composition Li10.5- xSi1.5P1.5S12- xIx (with x = 0, 0.2, 0.4), possessing high ionic conductivities of ≥ 7 mS cm-1 at room temperature. We show that increasing iodine content alters the phase composition and triggers reversible redox activity in these materials. If implemented as catholytes, this enables very fast sulfur conversion kinetics, ultimately leading to ASSLSBs with exceptional performance. The cells achieve 86% sulfur utilization at a rate of C/2 and at 45°C and offer high-rate capability by delivering 1175 mAh gsulfur -1 at 5C and 590 mAh gsulfur -1 at 15C. Furthermore, the synergistic effects of ionic percolation and redox-activity enable record areal capacities up to 14 mAh cm-2 with a sulfur loading of 10 mg cm-2. Taken together, our findings provide new strategies for designing redox-active catholytes for application in advanced ASSLSBs and further strengthen the redox-mediating role of iodine therein.

由于硫具有较高的理论比容量和较低的成本,全固态锂硫电池(ASSLSBs)在下一代电化学储能领域具有很大的前景。然而,缓慢的硫转化动力学和循环过程中严重的体积变化,以及复合阴极中不良的离子渗透,限制了它们的实际可行性。为了克服这些挑战,本文引入了标称成分为Li10.5- xSi1.5P1.5S12- xIx (x = 0,0.2, 0.4)的固体电解质,在室温下具有≥7 mS cm-1的高离子电导率。我们发现增加碘含量会改变这些材料的相组成并触发可逆氧化还原活性。如果作为阴极电解质实施,这可以实现非常快的硫转化动力学,最终产生具有优异性能的asslsb。在C/2和45°C的条件下,电池的硫利用率达到86%,在5C和15C下分别提供1175 mAh和590 mAh的硫-1。此外,离子渗透和氧化还原活性的协同作用使其面积容量达到14 mAh cm-2,硫负荷为10 mg cm-2。综上所述,我们的研究结果为设计用于晚期asslbs的氧化还原活性阴极物提供了新的策略,并进一步加强了碘在其中的氧化还原介导作用。
{"title":"Tailored Redox-Active Catholytes Enabling High-Rate and High-Loading All-Solid-State Lithium-Sulfur Batteries.","authors":"Jingui Yang, Ruizhuo Zhang, Ramon Zimmermanns, Mareen Schaller, Sylvio Indris, Jaehoon Choi, Simon Fleischmann, Torsten Brezesinski, Florian Strauss","doi":"10.1002/adma.202513204","DOIUrl":"https://doi.org/10.1002/adma.202513204","url":null,"abstract":"<p><p>All-solid-state lithium-sulfur batteries (ASSLSBs) hold great promise for next-generation electrochemical energy storage due to sulfur's high theoretical specific capacity and low cost. However, sluggish sulfur conversion kinetics and severe volume variations during cycling, as well as poor ionic percolation in composite cathodes, limit their practical viability. To overcome these challenges, we herein introduce solid electrolytes of nominal composition Li<sub>10.5-</sub> <sub>x</sub>Si<sub>1.5</sub>P<sub>1.5</sub>S<sub>12-</sub> <sub>x</sub>I<sub>x</sub> (with x = 0, 0.2, 0.4), possessing high ionic conductivities of ≥ 7 mS cm<sup>-1</sup> at room temperature. We show that increasing iodine content alters the phase composition and triggers reversible redox activity in these materials. If implemented as catholytes, this enables very fast sulfur conversion kinetics, ultimately leading to ASSLSBs with exceptional performance. The cells achieve 86% sulfur utilization at a rate of C/2 and at 45°C and offer high-rate capability by delivering 1175 mAh g<sub>sulfur</sub> <sup>-1</sup> at 5C and 590 mAh g<sub>sulfur</sub> <sup>-1</sup> at 15C. Furthermore, the synergistic effects of ionic percolation and redox-activity enable record areal capacities up to 14 mAh cm<sup>-2</sup> with a sulfur loading of 10 mg cm<sup>-2</sup>. Taken together, our findings provide new strategies for designing redox-active catholytes for application in advanced ASSLSBs and further strengthen the redox-mediating role of iodine therein.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e13204"},"PeriodicalIF":26.8,"publicationDate":"2026-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146130482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
All-Optical Reconfigurable Physical Unclonable Function for Sustainable Security. 可持续安全的全光可重构物理不可克隆功能。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202521712
Jang-Kyun Kwak, Changgyun Moon, Hyun-Bin Yu, Sunkook Kim, Dong-Hwan Kim

As security threats continue to evolve, static physical unclonable function (PUF) systems are facing inherent limitations in their security sustainability. This growing demand for sustainable security is driving a paradigm shift toward dynamic and reconfigurable PUF systems. However, previous approaches relying on thermal treatments to reconstruct physical entities can be limited in practicality due to concerns over thermal stability and scalability. Here, we present an all-optical reconfigurable PUF that fills this unmet need through non-invasive and scalable optical techniques. To demonstrate this, we introduce a nanopatterning method that employs plasmonic coupling-induced sintering of optically trapped gold nanoparticles (AuNPs) to fabricate optical PUFs. The resulting PUFs, which leverage complex spatiospectral information, deliver practically sufficient security, outstanding encoding density, and robust resistance against machine learning-based modeling attacks. Furthermore, we validate the applicability of the proposed PUF system for anti-counterfeiting and traceability applications by implementing a lightweight authentication protocol that exhibits reliable performance. Lastly, we demonstrate that irreversible and on-demand reconfiguration through optothermal nudging of patterned AuNPs enables repeated generation of unpredictable and independent responses while maintaining consistent security. These demonstrations signify the potential of our all-optical approach as a promising pathway toward achieving sustainable hardware-based security.

随着安全威胁的不断演变,静态物理不可克隆功能(PUF)系统在其安全可持续性方面面临着固有的限制。这种对可持续安全日益增长的需求正在推动向动态和可重构PUF系统的范式转变。然而,由于对热稳定性和可扩展性的担忧,以前依靠热处理来重建物理实体的方法在实用性上受到限制。在这里,我们提出了一种全光可重构PUF,通过非侵入性和可扩展的光学技术填补了这一未满足的需求。为了证明这一点,我们引入了一种纳米图像化方法,该方法利用等离子体耦合烧结光学捕获金纳米粒子(AuNPs)来制造光学PUFs。由此产生的puf利用复杂的空间光谱信息,提供了几乎足够的安全性,出色的编码密度,以及对基于机器学习的建模攻击的强大抵抗力。此外,我们通过实现具有可靠性能的轻量级身份验证协议,验证了所提出的PUF系统在防伪和可追溯性应用中的适用性。最后,我们证明了通过光热推动模式aunp的不可逆和按需重构可以在保持一致安全性的同时重复产生不可预测的独立响应。这些演示表明了我们的全光方法作为实现基于硬件的可持续安全的有希望的途径的潜力。
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引用次数: 0
The Rise of Aqueous Selenium-Based Batteries: Challenges, Strategies, and the Path Forward. 水硒基电池的兴起:挑战、策略和前进的道路。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202522085
Zhichao Wang, Chaoyi Qiu, Zhiwei Chen, Zening Wu, Haoxiang Yu, Lei Yan, Liyuan Zhang, Ting-Feng Yi, Jie Shu

Aqueous metal-selenium batteries (AMSeBs) have emerged as promising candidates for safe, cost-effective, and high-energy-density energy storage, yet their development is hindered by challenges spanning electrode stability, reaction reversibility, and electrolyte compatibility. This review systematically explores the thermodynamic and electrochemical landscape of AMSeBs, integrating theoretical analysis with experimental advances to establish a rational design framework. First, by evaluating key parameters, including electrode potentials, volume change rates, solubility of metal selenides, and energy metrics, we identify promising systems such as Zn-Se and Cu-Se, along with unexplored candidates like Fe-Se and Ga-Se. Second, selenium-based cathodes are categorized into three types, elemental Se & SexSy composites, organic selenides, and transition metal selenides, with emphasis on multi-electron transfer mechanisms, particularly the six-electron Se4+/Se2- redox pathway, which offers a route to overcome capacity limitations. Third, strategies for stabilizing metal anodes, expanding the electrochemical stability window of aqueous electrolytes, and mitigating shuttle effects are critically discussed. Finally, we outline future directions, including interface engineering, artificial intelligence-assisted material screening, and flexible device integration, providing a roadmap toward high-performance AMSeBs for next-generation energy storage applications.

水金属硒电池(amseb)已成为安全、经济、高能量密度储能的有前途的候选材料,但其发展受到电极稳定性、反应可逆性和电解质相容性等挑战的阻碍。本文系统地探讨了amseb的热力学和电化学景观,将理论分析与实验进展相结合,以建立合理的设计框架。首先,通过评估关键参数,包括电极电位、体积变化率、金属硒化物的溶解度和能量指标,我们确定了有前途的体系,如Zn-Se和Cu-Se,以及未开发的候选体系,如Fe-Se和Ga-Se。其次,将硒基阴极分为元素Se & SexSy复合材料、有机硒化物和过渡金属硒化物三种类型,重点介绍了多电子转移机制,特别是六电子Se4+/Se2-氧化还原途径,为克服容量限制提供了途径。第三,重点讨论了稳定金属阳极、扩大水电解质电化学稳定窗口和减轻穿梭效应的策略。最后,我们概述了未来的发展方向,包括界面工程、人工智能辅助材料筛选和灵活的器件集成,为下一代储能应用的高性能amseb提供了路线图。
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引用次数: 0
Pressure-Independent Acoustic-Vortex Communication With Enhanced-Capacity and Cryptographic Information by Free-Flooded Metasurfaces. 自由泛洪超表面上具有增强容量和加密信息的不依赖压力的声涡通信。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202521718
Zhiwen Ren, Xudong He, Hao-Wen Dong, Mingji Chen, Daining Fang

Structured vortex beams have driven significant advances in multiplexing communication technologies and have been demonstrated experimentally in optics, electromagnetics, and airborne acoustics. However, the strong vibroacoustic coupling and high hydrostatic pressure hamper the experimental enhancement of acoustic information capacity in underwater communication via passively modulating coaxial beams. Here, we report the experimental realization of simultaneous information capacity enhancement and hybrid physical-computational camouflage in underwater free-space pressure-independent acoustic-vortex communication. Two inverse-designed free-flooded metasurfaces, with hydrostatically resilient stability and customized wave scattering characteristics, synthesize and demodulate experimentally coaxial vortex beams of different topological charges, enabling physically encrypted, port-to-port information transfer. A computational-mask encryption scheme further digitally conceals a plaintext image within two ciphertext bitstreams. Transmission of these ciphertexts through the synthesized hetero-order vortex beams experimentally confirms physical-computational anti-eavesdropping capabilities of the system. Our research charts an unprecedented path toward high-capacity, highly secure underwater acoustic communication technologies in the deep ocean.

结构涡旋光束在多路复用通信技术方面取得了重大进展,并在光学、电磁学和航空声学方面得到了实验证明。然而,强的声振耦合和高静水压力阻碍了同轴波束被动调制水下通信中声信息容量的实验增强。在这里,我们报告了在水下自由空间不依赖压力的声涡通信中同时实现信息容量增强和混合物理-计算伪装的实验实现。两个反向设计的自由淹没超表面,具有流体静力弹性稳定性和定制的波散射特性,在实验中合成和解调不同拓扑电荷的同轴涡旋光束,实现物理加密,端口到端口的信息传输。计算掩码加密方案进一步在两个密文位流中数字隐藏明文图像。这些密文通过合成异序涡旋光束的传输实验证实了系统的物理计算抗窃听能力。我们的研究为深海中高容量、高安全的水声通信技术开辟了一条前所未有的道路。
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引用次数: 0
Breaking Single-Reaction Limits: In Situ Visualization of TiS2-Driven Conversion-Intercalation Synergy in Lithium-Sulfur Batteries. 打破单一反应限制:锂硫电池中tis2驱动的转换-插层协同作用的原位可视化。
IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-07 DOI: 10.1002/adma.202522007
Jian-Xin Tian, Yuan Li, Xu-Sheng Zhang, Zhen-Zhen Shen, Rui-Zhi Liu, Shuang-Yan Lang, Yu-Guo Guo, Rui Wen

Conventional cathodes of lithium battery relying on single storage mechanisms-whether intercalation or conversion-face intrinsic limitations in energy density and sluggish electrode kinetics. Hybrid systems combining both mechanisms offer promising pathways to transcend these constraints; yet, their dynamic interfacial synergies remain poorly deciphered at the nanoscale. This study employs multimodal in situ characterization (Electrochemical atomic force microscopy/Raman/Electrochemical impedance spectroscopy) to elucidate the dynamic synergy in TiS2-S hybrid cathodes, revealing the concurrent interfacial evolution during cycling: nanoscale steps formation via Li-ion intercalation in the TiS2-LiTiS2 host and the phase transformation of S-Li2S/Li2S2. Crucially, the TiS2/LiTiS2 serves as a bifunctional interface that not only contributes capacity but also mediates sulfide adsorption and catalyzes preferential edge-directed sulfide deposition. The partially delithiated LixTiS2 enhances electronic conductivity, creating rapid electron transport that facilitates subsequent interfacial sulfide conversion reaction. The hybrid storage mechanism retains features characteristic of both S and TiS2 storage mechanisms, yet manifests synergistic interfacial reconstruction rather than simple superposition, achieving enhanced reversibility, exceptional cycling stability, and superior rate capability.

传统的锂电池阴极依赖于单一的存储机制,无论是插层还是转换,在能量密度和缓慢的电极动力学方面都面临着内在的限制。结合这两种机制的混合系统提供了超越这些限制的有希望的途径;然而,它们的动态界面协同作用在纳米尺度上仍然很难被破译。本研究采用多模态原位表征(电化学原子力显微镜/拉曼/电化学阻抗谱)来阐明TiS2-S杂化阴极的动态协同作用,揭示了循环过程中同步的界面演化:TiS2-LiTiS2基体中锂离子嵌入形成纳米级阶梯以及S-Li2S/Li2S2的相变。关键的是,TiS2/LiTiS2作为一个双功能界面,不仅可以提供容量,还可以介导硫化物吸附和催化优先的边缘定向硫化物沉积。部分稀释的LixTiS2增强了电子导电性,创造了快速的电子传递,促进了随后的界面硫化物转化反应。混合存储机制保留了S和TiS2存储机制的特征,但表现出协同界面重建而不是简单的叠加,实现了增强的可逆性、卓越的循环稳定性和优越的速率能力。
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