ACS Materials Letters最新文献

Biomimetic Gradient Structured Dielectric Elastomer Actuators for Long-Term Large Out-of-Plane Actuation 用于长期大面外驱动的仿生梯度结构介电弹性体致动器

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-24 DOI: 10.1021/acsmaterialslett.5c0010810.1021/acsmaterialslett.5c00108

Huifeng Dong, Zike Chen, Jiangshan Zhuo, Ruifen Tang, Junbo Peng, Lvting Wang, Shengchao Jiang, Rui Xiao* and Ye Shi*,

{"title":"Biomimetic Gradient Structured Dielectric Elastomer Actuators for Long-Term Large Out-of-Plane Actuation","authors":"Huifeng Dong, Zike Chen, Jiangshan Zhuo, Ruifen Tang, Junbo Peng, Lvting Wang, Shengchao Jiang, Rui Xiao* and Ye Shi*, ","doi":"10.1021/acsmaterialslett.5c0010810.1021/acsmaterialslett.5c00108","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00108https://doi.org/10.1021/acsmaterialslett.5c00108","url":null,"abstract":"Dielectric elastomer actuators (DEAs) have been widely studied as artificial muscles, owing to their large actuation strain and high energy density. To generate out-of-plane actuation, which can be conveniently coupled in motions such as grasping, walking, and swinging, asymmetrically structured DEAs (AS-DEAs) have been developed by attaching active dielectric elastomer (DE) films to passive substrates. However, traditional AS-DEAs usually suffer from a short actuation life caused by stress concentration at the soft–stiff interface. Here, inspired by the human bone–cartilage tissue interface, we developed gradient structured DEAs (GS-DEAs) by preparing thin DE films in which the modulus was increased stepwise and inserting them as buffer layers between active DE films and substrates. This gradient structure effectively reduces the interface shear stresses to below the interfacial bonding strength, thus greatly improving the durability of the actuator. GS-DEAs maintain large out-of-plane actuation and force output after 100,000 cycles and successfully drive a robotic fish for long-term underwater swimming.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"2002–2009 2002–2009"},"PeriodicalIF":9.6,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Reliability Challenges in Equivalent-Oxide-Thickness Scaling with High-κ Er2O3 Dielectrics on Two-Dimensional MoS2 Field-Effect Transistors 高κ Er2O3介电体在二维MoS2场效应晶体管上等效氧化层厚度缩放的可靠性挑战

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-23 DOI: 10.1021/acsmaterialslett.5c0029110.1021/acsmaterialslett.5c00291

Shuhong Li, Ryotaro Otake, Tomonori Nishimura, Takashi Taniguchi, Kenji Watanabe, Yoshiki Sakuma and Kosuke Nagashio*,

{"title":"Reliability Challenges in Equivalent-Oxide-Thickness Scaling with High-κ Er2O3 Dielectrics on Two-Dimensional MoS2 Field-Effect Transistors","authors":"Shuhong Li, Ryotaro Otake, Tomonori Nishimura, Takashi Taniguchi, Kenji Watanabe, Yoshiki Sakuma and Kosuke Nagashio*, ","doi":"10.1021/acsmaterialslett.5c0029110.1021/acsmaterialslett.5c00291","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00291https://doi.org/10.1021/acsmaterialslett.5c00291","url":null,"abstract":"The integration of high-κ films with two-dimensional (2D) semiconductors offers a pathway to advance metal-oxide-semiconductor technology scaling. While reliability studies on gate stacks with 2D semiconductors have focused on device performance instabilities, the stability of bulk dielectric properties, particularly for ultrathin high-κ films on 2D semiconductors, remains underexplored. This work demonstrates the scalability of high-κ Er2O3 on mechanically transferred MoS2, achieving an equivalent oxide thickness below 1 nm. However, the critical issue is identified: time-dependent degradation of the dielectric constant, which persists despite various passivation methods. Notably, this instability is absent when the high-κ film is deposited on a clean surface of MoS2 grown on a sapphire substrate, revealing that the degradation originates from suboptimal surface conditions of the 2D semiconductor rather than the dielectric itself. These findings highlight the necessity of addressing 2D material surface effects to fully realize the potential of ultrathin high-κ dielectrics in future device applications.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1993–2001 1993–2001"},"PeriodicalIF":9.6,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

A Chiral Amino Acid-Modified pH-Responsive Nanoplatform Coactivates Cuproptosis and cGAS-STING Signaling Pathways for Cancer Therapy 手性氨基酸修饰的ph响应纳米平台协同激活cuprotosis和cGAS-STING信号通路用于癌症治疗

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmaterialslett.5c0009710.1021/acsmaterialslett.5c00097

Lin Li, Guanheng Wang, Biao Xue, Xueao Li, Jiapeng Wang, Wenjun Wang, Chang Liu*, Chunlei Li* and Xiuwen Zheng*,

{"title":"A Chiral Amino Acid-Modified pH-Responsive Nanoplatform Coactivates Cuproptosis and cGAS-STING Signaling Pathways for Cancer Therapy","authors":"Lin Li, Guanheng Wang, Biao Xue, Xueao Li, Jiapeng Wang, Wenjun Wang, Chang Liu*, Chunlei Li* and Xiuwen Zheng*, ","doi":"10.1021/acsmaterialslett.5c0009710.1021/acsmaterialslett.5c00097","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00097https://doi.org/10.1021/acsmaterialslett.5c00097","url":null,"abstract":"We engineered l/d-Cu/Z@MH, a multimodal therapeutic nanoplatform functionalized with hyaluronic acid (HA) and chiral amino acids, to enhance tumor-targeting specificity and cellular internalization. The nanoparticles exhibit pH-responsive degradation, rapidly releasing Cu2+ and MnO2 layers upon cellular uptake. These agents drive a tumor microenvironment (TME)-amplified Fenton-like reaction with endogenous H2O2, generating cytotoxic reactive oxygen species (ROS), depleting glutathione, and augmenting chemodynamic therapy (CDT). Copper ions induce cuproptosis, while manganese ions activate the cGAS-STING signaling pathway. Synergistically, ROS overproduction and cGAS-STING activation provoke endoplasmic reticulum stress and immunogenic cell death (ICD), effectively reprogramming the tumor’s immunosuppressive microenvironment. The results of this study demonstrated potent tumor suppression by l/d-Cu/Z@MH nanoparticles, with l-Cu/Z@MH showing superior efficacy.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1973–1983 1973–1983"},"PeriodicalIF":9.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Kinetically and Thermodynamically Controlled Cross-Linking in Sustainable Digital Light Processing Printing: Enabling Thermoset Reprocessing via Thermal Leveling Effect 可持续数字光处理印刷中的动力学和热力学控制交联：通过热平整效应实现热固性再加工

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmaterialslett.4c0246510.1021/acsmaterialslett.4c02465

Yi Ting Chong, Suxi Wang, Sirawit Pruksawan, Zhuang Mao Png*, Qiang Zhu, Zibiao Li and FuKe Wang*,

{"title":"Kinetically and Thermodynamically Controlled Cross-Linking in Sustainable Digital Light Processing Printing: Enabling Thermoset Reprocessing via Thermal Leveling Effect","authors":"Yi Ting Chong, Suxi Wang, Sirawit Pruksawan, Zhuang Mao Png*, Qiang Zhu, Zibiao Li and FuKe Wang*, ","doi":"10.1021/acsmaterialslett.4c0246510.1021/acsmaterialslett.4c02465","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02465https://doi.org/10.1021/acsmaterialslett.4c02465","url":null,"abstract":"High-performance resins are essential for digital light processing (DLP) 3D printing, yet most are thermosetting and lack reprocessability. Recently developed covalent adaptive networks address this limitation, but their reliance on specialized monomers hinders scalability and practical application. Herein, we report a 3D-printable resin formulated with isobornyl acrylate, a 1,2-diol-based boronic ester cross-linker (<4%), and tetradecanol as a trans-borylesterification mediator. At room temperature, tetradecanol remains unreactive, preserving a rigid thermoset matrix while forming microelastic domains that dissipate impact energy, achieving an 8600% increase in toughness with 15% tetradecanol. During hot pressing, the thermal leveling effect kinetically drives dynamic bond exchange, converting the thermoset into a thermoplastic material. Upon cooling, the reaction becomes thermodynamically controlled again, reestablishing the thermoset polymer network and recovering its mechanical properties. This resin uniquely transitions to a thermoplastic state only during reprocessing, reverting to a durable thermoset upon cooling, enabling sustainable, high-performance DLP printing with end-of-life reusability.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1963–1972 1963–1972"},"PeriodicalIF":9.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ionic-Bond Regulated Cross-Linking Polyurethane with Multilevel Energy Dissipation, Enhanced Chain Rearrangement and Solvent Reprocessability 具有多层能量耗散、增强链重排和溶剂再加工性的离子键调控交联聚氨酯

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-21 DOI: 10.1021/acsmaterialslett.5c0031710.1021/acsmaterialslett.5c00317

Qingyun Zhao, Linzhu Xu, Birong Zeng*, Yiting Xu, Weiang Luo, Conghui Yuan and Lizong Dai*,

{"title":"Ionic-Bond Regulated Cross-Linking Polyurethane with Multilevel Energy Dissipation, Enhanced Chain Rearrangement and Solvent Reprocessability","authors":"Qingyun Zhao, Linzhu Xu, Birong Zeng*, Yiting Xu, Weiang Luo, Conghui Yuan and Lizong Dai*, ","doi":"10.1021/acsmaterialslett.5c0031710.1021/acsmaterialslett.5c00317","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00317https://doi.org/10.1021/acsmaterialslett.5c00317","url":null,"abstract":"Highly cross-linked thermosetting polyurethanes based on covalent adaptable networks (CANs) have limitations in network rearrangement due to reduced polymer chain mobility. Herein, the strategy of multilevel dynamic nanodomains (MDND) based on ionic-bond regulation was proposed for constructing a series of ionic polyurethane (Ionic-PU) with high mechanical properties, self-healing and solvent reprocessing ability. Specifically, three ionic chain extenders were synthesized using mercaptopropionate (SH(CH2)2COO–) as the anion part and N-substituted 1,4-bis(imidazol-1-yl)-butane (IC4I) containing different carbon chain length in a pendant group as the cation part, which were then polymerized into the main chain. Ionic-PUs exhibited customizable mechanical properties and multilevel energy dissipation due to the steric hindrance, the magnitude of electrostatic force, and the type of noncovalent interaction on the construction of MDND. Ionic-PUs had enhanced chain rearrangement and even solvent reprocessing due to the fact that ionic bonds break and reorganize efficiently at elevated temperatures or in highly polar solvents.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1984–1992 1984–1992"},"PeriodicalIF":9.6,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903285","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

BODIPY-Based Photosensitizer with Outstanding Photocytotoxicity for Deep-Tissue Photodynamic Therapy 基于bodipi的光敏剂具有突出的光细胞毒性，用于深层组织光动力治疗

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-19 DOI: 10.1021/acsmaterialslett.5c0008610.1021/acsmaterialslett.5c00086

Bin-Kai Liu, Kun-Xu Teng, Li-Ya Niu and Qing-Zheng Yang*,

{"title":"BODIPY-Based Photosensitizer with Outstanding Photocytotoxicity for Deep-Tissue Photodynamic Therapy","authors":"Bin-Kai Liu, Kun-Xu Teng, Li-Ya Niu and Qing-Zheng Yang*, ","doi":"10.1021/acsmaterialslett.5c0008610.1021/acsmaterialslett.5c00086","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00086https://doi.org/10.1021/acsmaterialslett.5c00086","url":null,"abstract":"Tissue penetration and hypoxia present significant challenges for photodynamic therapy (PDT), restricting its clinical utility. We here report a Type-I photosensitizer (OBDP) with outstanding photocytotoxicity to overcome these limitations for deep-tissue PDT. OBDP targets lipid droplets in cancer cells. Upon irradiation, OBDP oxidizes nearby polyunsaturated fatty acids (PUFAs) into hydroperoxides through a photoinduced electron transfer mechanism, ultimately evoking ferroptosis. Under ultralow-power light-irradiation (660 nm, 5 mW cm–2, 3 J cm–2), OBDP effectively kills cancer cells, displaying an impressively low half-maximal inhibitory concentration (IC50) of 55.5–76.3 nM for three cancer cell lines (HeLa, A549, and HepG2 cells) under hypoxic conditions (2% O2). Due to the outstanding photocytotoxicity, OBDP can efficiently ablate tumors in deep-tissue PDT model experiments, achieving a tumor growth inhibition rate of up to 88.1%. This work represents a significant advancement in PDT and offers valuable insights for the development of photosensitizers tailored for deep-tissue solid tumors.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1947–1955 1947–1955"},"PeriodicalIF":9.6,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anion Activity and Metastable Phase Formation in Li1–xFePO4 Investigated Using Soft-to-Hard X-ray Absorption and Emission Spectroscopy 用软硬x射线吸收和发射光谱研究Li1-xFePO4阴离子活性和亚稳相形成

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-19 DOI: 10.1021/acsmaterialslett.4c0238910.1021/acsmaterialslett.4c02389

Abiram Krishnan, Doyoub Kim, Cherno Jaye and Faisal M Alamgir*,

{"title":"Anion Activity and Metastable Phase Formation in Li1–xFePO4 Investigated Using Soft-to-Hard X-ray Absorption and Emission Spectroscopy","authors":"Abiram Krishnan, Doyoub Kim, Cherno Jaye and Faisal M Alamgir*, ","doi":"10.1021/acsmaterialslett.4c0238910.1021/acsmaterialslett.4c02389","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02389https://doi.org/10.1021/acsmaterialslett.4c02389","url":null,"abstract":"We systematically investigate the intricate roles of cations as well as anions during phase transformation, specifically, the formation of a metastable phase in phospho-olivine, LiFePO4 (LFP). The cation- and anion-specific electronic structures are studied using a combination of high-resolution soft-to-hard X-ray absorption and emission spectroscopy. Our findings reveal that the formation of the metastable phase at higher states-of-charge (SoC) is associated with a decreased oxidation state of iron, assisted by oxygen release. Additionally, we find that phosphorus is active in the charge process, exhibiting reduction, resulting from an electron density redistribution between oxygen and its neighboring iron and phosphorus atoms. Furthermore, the phase transformation process in LFP impacts its magnetic properties, with iron retaining its high-spin configuration along with an increased average spin during its transformation into FePO4 (FP).","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1956–1962 1956–1962"},"PeriodicalIF":9.6,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialslett.4c02389","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Non-fluorinated Triazine-Functionalized Pentiptycene-Based Nanoporous Organic Polymer for Highly Efficient SF6/N2 Separation 高效分离SF6/N2的非氟化三嗪功能化戊苯基纳米多孔有机聚合物

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-18 DOI: 10.1021/acsmaterialslett.5c0054910.1021/acsmaterialslett.5c00549

Xinyu Yang, Qilin Wang, Jiangli Zhu, Jun Yan* and Shengwei Guo,

{"title":"Non-fluorinated Triazine-Functionalized Pentiptycene-Based Nanoporous Organic Polymer for Highly Efficient SF6/N2 Separation","authors":"Xinyu Yang, Qilin Wang, Jiangli Zhu, Jun Yan* and Shengwei Guo, ","doi":"10.1021/acsmaterialslett.5c0054910.1021/acsmaterialslett.5c00549","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00549https://doi.org/10.1021/acsmaterialslett.5c00549","url":null,"abstract":"Efficient separation of sulfur hexafluoride (SF6) from SF6/N2 mixtures is essential for both environmental protection and industrial applications. We report a non-fluorinated triazine-functionalized pentiptycene-based nanoporous organic polymer (TNOP-1) synthesized through a one-pot method of pentiptycene quinone with cyanuric chloride. TNOP-1 exhibits a high specific surface area of 822 m2·g–1 and remarkable SF6/N2 selectivities of 95.0 at 273 K and 84.7 at 298 K. Dynamic breakthrough experiments further confirm efficient SF6 capture under ambient conditions. Furthermore, molecular dynamics simulations reveal dominant SF6 adsorption sites where polar triazine and ketone functionalities enhance host–guest interactions via framework C–H bonds. These findings offer important molecular-level design principles for SF6 capture in nanoporous organic polymers (NOPs) and are expected to advance next-generation materials for energy-efficient gas separation.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1940–1946 1940–1946"},"PeriodicalIF":9.6,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903155","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unveiling the Inversion-Symmetry-Driven Excitation Switching in Aggregation-Induced Emission 揭示聚集诱导发射中逆对称驱动的激励开关

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-17 DOI: 10.1021/acsmaterialslett.4c0255010.1021/acsmaterialslett.4c02550

Charya J. Senanayake, Thalpage Don Dinithi Kavindi, D. H. Sanduni Deenalattha, Dinushika Kotudura Arachchige, Kaushanie Gunarathne, P. M. Anuradha Bandaranayake, U. Dulanjali Rodrigo, Nuwan de Silva and Neranga Abeyasinghe*,

{"title":"Unveiling the Inversion-Symmetry-Driven Excitation Switching in Aggregation-Induced Emission","authors":"Charya J. Senanayake, Thalpage Don Dinithi Kavindi, D. H. Sanduni Deenalattha, Dinushika Kotudura Arachchige, Kaushanie Gunarathne, P. M. Anuradha Bandaranayake, U. Dulanjali Rodrigo, Nuwan de Silva and Neranga Abeyasinghe*, ","doi":"10.1021/acsmaterialslett.4c0255010.1021/acsmaterialslett.4c02550","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.4c02550https://doi.org/10.1021/acsmaterialslett.4c02550","url":null,"abstract":"Understanding the aggregation-induced emission (AIE) mechanism, where the fluorescence is enhanced upon aggregation, is a critical step in predictably designing AIE molecules for use in novel applications. Here, we report a π–π stacked AIE chromophore, A3MN, that demonstrates the switching of the excitation maximum when moving from monomers to aggregates, which has never been reported before. Also, we elucidate such switching by revealing a novel electronic origin for AIE via inversion-symmetry-driven fluorescence in A3MN. We observe this unique fluorescence phenomenon being affected by mechanical crushing and the rate of dissolution of crystals in the solvent. This inversion-symmetry-driven emission phenomenon plays a pivotal role in modulating the AIE of A3MN aggregates in solution, films, and crystals. The insights unveiled here allow the design and engineering of AIE systems that can be adopted in a multitude of applications including mechanical impact/damage memory storage (and reading) using luminescence, quantum computing, sensing, and super-resolution imaging.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1930–1939 1930–1939"},"PeriodicalIF":9.6,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Three-Dimensional to Layered Halide Perovskites: A Parameter-Free Hybrid Functional Method for Predicting Electronic Band Gaps 三维到层状卤化物钙钛矿：一种预测电子带隙的无参数杂化泛函方法

IF 9.6 1区化学

ACS Materials Letters Pub Date : 2025-04-17 DOI: 10.1021/acsmaterialslett.5c0015810.1021/acsmaterialslett.5c00158

Ibrahim Buba Garba, Lorenzo Trombini, Claudine Katan, Jacky Even, Marios Zacharias, Mikael Kepenekian and George Volonakis*,

{"title":"Three-Dimensional to Layered Halide Perovskites: A Parameter-Free Hybrid Functional Method for Predicting Electronic Band Gaps","authors":"Ibrahim Buba Garba, Lorenzo Trombini, Claudine Katan, Jacky Even, Marios Zacharias, Mikael Kepenekian and George Volonakis*, ","doi":"10.1021/acsmaterialslett.5c0015810.1021/acsmaterialslett.5c00158","DOIUrl":"https://doi.org/10.1021/acsmaterialslett.5c00158https://doi.org/10.1021/acsmaterialslett.5c00158","url":null,"abstract":"Accurate prediction of electronic band gaps in halide perovskites is crucial for optoelectronic applications. Standard hybrid functionals like HSE and PBE0 often fail to predict band gaps for 3D and layered perovskites. This study evaluates the doubly screened dielectric-dependent hybrid (DSH) functional for Pb- and Sn-based 3D and layered perovskites. The DSH functional, with material-dependent screening parameters derived from the dielectric constant, accurately predicts band gaps for 3D perovskites when considering local disorder. For layered perovskites, using average dielectric constants tends to overestimate band gaps. We propose using the dielectric constant of respective 3D perovskites for DSH screening, improving predictions for layered structures of various organic spacers. PBE0 band gaps closely match DSH values, especially for iodides, while the HSE functional underestimates band gaps due to missing long-range dielectric screening. This efficient ab initio framework can facilitate the design of advanced optoelectronic devices based on 3D and layered perovskites and their heterostructures.","PeriodicalId":19,"journal":{"name":"ACS Materials Letters","volume":"7 5","pages":"1922–1929 1922–1929"},"PeriodicalIF":9.6,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143903191","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0