ACS Earth and Space Chemistry最新文献

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Vapor Infiltration Synthesis of Indium Sulfide Magic Size Cluster 蒸汽渗透法合成硫化铟魔簇
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-11-01 DOI: 10.1021/acsnano.4c1094310.1021/acsnano.4c10943
Kihoon Kim, Shana Havenridge, Nestor J. Zaluzec, Donghyeon Kang, Nuwanthaka P. Jayaweera, Jeffrey W. Elam, Karen L. Mulfort, Cong Liu and Alex B. F. Martinson*, 
{"title":"Vapor Infiltration Synthesis of Indium Sulfide Magic Size Cluster","authors":"Kihoon Kim,&nbsp;Shana Havenridge,&nbsp;Nestor J. Zaluzec,&nbsp;Donghyeon Kang,&nbsp;Nuwanthaka P. Jayaweera,&nbsp;Jeffrey W. Elam,&nbsp;Karen L. Mulfort,&nbsp;Cong Liu and Alex B. F. Martinson*,&nbsp;","doi":"10.1021/acsnano.4c1094310.1021/acsnano.4c10943","DOIUrl":"https://doi.org/10.1021/acsnano.4c10943https://doi.org/10.1021/acsnano.4c10943","url":null,"abstract":"<p >The energetically favorable formation of atomically precise clusters, known as magic size clusters, in the solution phase enables a precision nanoscale synthesis with exquisite uniformity. We report the synthesis of magic size clusters via vapor infiltration of atomic layer deposition precursors directly in a polymer thin film. Sequential infiltration of trimethylindium vapor and hydrogen sulfide gas into poly(methyl methacrylate) leads to the formation of clusters with uniform properties consistent with a magic size cluster─In<sub>6</sub>S<sub>6</sub>(CH<sub>3</sub>)<sub>6</sub>. While an increase in cluster size might be expected with additional sequential infiltration cycles of the reactive In and S precursors, uniform properties consistent with magic size clusters form in multiple polymers under a range of processing conditions. Ultraviolet–visible absorption spectra of In<sub>6</sub>S<sub>6</sub>(CH<sub>3</sub>)<sub>6</sub> are largely independent of the number of sequential infiltration cycles and exhibit air stability, both of which are attributed to an energetically favorable synthetic pathway that is evaluated with density functional theory.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31372–31380 31372–31380"},"PeriodicalIF":15.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608444","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
An Amplification-Free Digital Assay Based on Primer Exchange Reaction-Mediated Botryoidal-Like Fluorescent Polystyrene Dots to Detect Multiple Pathogenic Bacteria 基于引物交换反应介导的类菌体荧光聚苯乙烯点的免扩增数字测定法可检测多种病原菌
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-11-01 DOI: 10.1021/acsnano.4c0906910.1021/acsnano.4c09069
Zhipan Wang, Aimin Ma and Yiping Chen*, 
{"title":"An Amplification-Free Digital Assay Based on Primer Exchange Reaction-Mediated Botryoidal-Like Fluorescent Polystyrene Dots to Detect Multiple Pathogenic Bacteria","authors":"Zhipan Wang,&nbsp;Aimin Ma and Yiping Chen*,&nbsp;","doi":"10.1021/acsnano.4c0906910.1021/acsnano.4c09069","DOIUrl":"https://doi.org/10.1021/acsnano.4c09069https://doi.org/10.1021/acsnano.4c09069","url":null,"abstract":"<p >Multiple and ultrasensitive detection of pathogenic bacteria is critical but remains a challenge. Here, we introduce a digital assay for multiplexed and target DNA amplification-free detection of pathogenic bacteria using botryoidal-like fluorescent polystyrene dots (PS-dots), which were first prepared through the hybridization reaction between primer exchange reaction chains and polystyrene nanospheres that encapsulated polymer dots for signal preamplification. The pathogenic bacteria’s DNA was cleavaged by the argonaute (Ago) protein-mediated multiple and precise cleavage reactions, where the obtained target sequences bridged the magnetic beads (MBs) and botryoidal-like PS-dots via a hybridization reaction, and the fluorescent MB-botryoidal PS-dot complexes were utilized as digital probes based on colors and sizes for digital encoding. An artificial-intelligence-fluorescent microsphere counting algorithm was applied to identify and count the fluorescent MBs for digital readout. This digital assay combined the ultrabright botryoidal-like PS-dots with <i>Clostridium butyricum</i> Ago’s precise enzyme cleavage properties, achieving simultaneous detection of three pathogenic bacteria with a linearity range from 10<sup>2</sup> to 10<sup>6</sup> CFU/mL without target DNA amplification within 1.5 h. This digital assay has also been applied to detect aquatic and clinical samples with accepted accuracy (98%), which offers an avenue for a next-generation multiplexed digital platform for pathogenic bacteria analysis.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31174–31187 31174–31187"},"PeriodicalIF":15.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Mucus-Penetrable Biomimetic Nanoantibiotics for Pathogen-Induced Pneumonia Treatment 用于治疗病原体引起的肺炎的可穿透黏液的仿生纳米抗生素
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-11-01 DOI: 10.1021/acsnano.4c1083710.1021/acsnano.4c10837
Yue Wang, Qihang Ding*, Gongcheng Ma, Zhiwei Zhang, Jiaqi Wang, Chang Lu, Chunbai Xiang, Kun Qian, Jun Zheng, Yaming Shan, Pengfei Zhang*, Zhen Cheng*, Ping Gong* and Qi Zhao*, 
{"title":"Mucus-Penetrable Biomimetic Nanoantibiotics for Pathogen-Induced Pneumonia Treatment","authors":"Yue Wang,&nbsp;Qihang Ding*,&nbsp;Gongcheng Ma,&nbsp;Zhiwei Zhang,&nbsp;Jiaqi Wang,&nbsp;Chang Lu,&nbsp;Chunbai Xiang,&nbsp;Kun Qian,&nbsp;Jun Zheng,&nbsp;Yaming Shan,&nbsp;Pengfei Zhang*,&nbsp;Zhen Cheng*,&nbsp;Ping Gong* and Qi Zhao*,&nbsp;","doi":"10.1021/acsnano.4c1083710.1021/acsnano.4c10837","DOIUrl":"https://doi.org/10.1021/acsnano.4c10837https://doi.org/10.1021/acsnano.4c10837","url":null,"abstract":"<p >Bacterial pneumonia has garnered significant attention in the realm of infectious diseases owing to a surge in the incidence of severe infections coupled with the growing scarcity of efficacious therapeutic modalities. Antibiotic treatment is still an irreplaceable method for bacterial pneumonia because of its strong bactericidal activity and good clinical efficacy. However, the mucus layer forming after a bacterial infection in the lungs has been considered as the “Achilles’ heels” facing the clinical application of such treatment. Herein, traceable biomimetic nanoantibiotics (BioNanoCFPs) were developed by loading indacenodithieno[3,2-<i>b</i>]thiophene (ITIC) and cefoperazone (CFP) in nanoplatforms coated with natural killer (NK) cell membranes. The BioNanoCFP exhibited excellent demonstrated mucus-penetrating abilities, facilitating their arrival at the infection site. The presence of Toll-like receptors in the NK cell membrane rendered the BioNanoCFP with the capability to recognize pathogen-associated molecular patterns within bacteria, allowing precise targeting of bacterial colonization sites and achieving substantial therapeutic efficacy. Overall, our findings demonstrate the viability and desirability of using NK cell membrane-mediated drug delivery as a promising strategy for precision treatment.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31349–31359 31349–31359"},"PeriodicalIF":15.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Insights into the Hierarchical Assembly of a Chemically Diverse Peptide Hydrogel Derived from Human Semenogelin I 从人类精蛋白Ⅰ中提取的化学性质多样的多肽水凝胶的分层组装透视
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-11-01 DOI: 10.1021/acsnano.4c0867210.1021/acsnano.4c08672
Brett H. Pogostin*, Kerilyn Godbe, Marija Dubackic, Isabelle Angstman, William Fox, Natalie Giovino, Matija Lagator, Abigail Payson, Marisa LaBarca, Birgitta Frohm, Katja Bernfur, Sara Linse, Casey H. Londergan, Ulf Olsson, Luigi Gentile and Karin S. Åkerfeldt*, 
{"title":"Insights into the Hierarchical Assembly of a Chemically Diverse Peptide Hydrogel Derived from Human Semenogelin I","authors":"Brett H. Pogostin*,&nbsp;Kerilyn Godbe,&nbsp;Marija Dubackic,&nbsp;Isabelle Angstman,&nbsp;William Fox,&nbsp;Natalie Giovino,&nbsp;Matija Lagator,&nbsp;Abigail Payson,&nbsp;Marisa LaBarca,&nbsp;Birgitta Frohm,&nbsp;Katja Bernfur,&nbsp;Sara Linse,&nbsp;Casey H. Londergan,&nbsp;Ulf Olsson,&nbsp;Luigi Gentile and Karin S. Åkerfeldt*,&nbsp;","doi":"10.1021/acsnano.4c0867210.1021/acsnano.4c08672","DOIUrl":"https://doi.org/10.1021/acsnano.4c08672https://doi.org/10.1021/acsnano.4c08672","url":null,"abstract":"<p >A peptide corresponding to a 13-residue segment of the human protein semenogelin I has been shown to generate a hydrogel consisting of amyloid-like fibrils. The relative chemical diversity (compared to synthetic <i>de novo</i> sequences) with 11 distinct amino acids makes this peptide (P0) an ideal candidate for investigating the role of individual residues in gelation. Herein, the <i>N-</i>terminal residues have been sequentially removed to furnish a series of truncated peptides, P1–P10, ranging from 12 to 3 residues in length. FTIR spectroscopy investigations reveal that P0–P6 forms a β-sheet secondary structure while shorter sequences do not self-assemble. Site-specific isotope labeling of the amide backbone of P0–P2 with the IR-sensitive vibrational probe <sup>13</sup>C═O yields FTIR spectra indicative of the initial formation of a kinetic product that slowly transforms into a structurally different thermodynamic product. The effects of the isotopic labels on the IR spectra facilitate the assignment of parallel and antiparallel structures, which are sometimes coexistent. Additional IR studies of three Phe<sup>CN</sup>-labeled P0 sequences are consistent with an H-bonded β-sheet amide core, spanning the 7 central residues. The macromolecular assembly of peptides that form β-sheets was assessed by cryo<i>-</i>TEM, SAXS/WAXS, and rheology. Cryo<i>-</i>TEM images of peptides P1–P6 display μm-long nanofibrils. Peptides P0–P3 generate homogeneous hydrogels composed of colloidally stable nanofibrils, and P4–P6 undergo phase separation due to the accumulation of attractive interfibrillar interactions. Three amino acid residues, Ser39, Phe40, and Gln43, were identified to be of particular interest in the truncated peptide series as the removal of any one of them, as the sequence shortens, leads to a major change in material properties.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31109–31122 31109–31122"},"PeriodicalIF":15.8,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c08672","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142607980","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Multifunctional Smart Fabrics with Integration of Self-Cleaning, Energy Harvesting, and Thermal Management Properties 集成自清洁、能量收集和热管理特性的多功能智能织物
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsnano.4c0832410.1021/acsnano.4c08324
Rumin Liu, Kequan Xia, Tao Yu, Feng Gao, Qinghua Zhang, Liping Zhu, Zhizhen Ye, Shikuan Yang*, Yaoguang Ma* and Jianguo Lu*, 
{"title":"Multifunctional Smart Fabrics with Integration of Self-Cleaning, Energy Harvesting, and Thermal Management Properties","authors":"Rumin Liu,&nbsp;Kequan Xia,&nbsp;Tao Yu,&nbsp;Feng Gao,&nbsp;Qinghua Zhang,&nbsp;Liping Zhu,&nbsp;Zhizhen Ye,&nbsp;Shikuan Yang*,&nbsp;Yaoguang Ma* and Jianguo Lu*,&nbsp;","doi":"10.1021/acsnano.4c0832410.1021/acsnano.4c08324","DOIUrl":"https://doi.org/10.1021/acsnano.4c08324https://doi.org/10.1021/acsnano.4c08324","url":null,"abstract":"<p >Due to their good wearability, smart fabrics have gradually developed into one of the important components of multifunctional flexible electronics. Nevertheless, function integration is typically accomplished through the intricate stacking of diverse modules, which inevitably compromises comfort and elevates processing complexities. The integration of these discrete functional modules into a unified design for smart fabrics represents a superior solution. Here, we put forward a rational approach to functional integration for the typical challenges of thermal management, energy supply, and surface contamination in smart fabrics. This sandwich-structured multilayer fabric (MLF) is obtained by continuous electrospinning of two layer P(VDF-HFP) fabric and one layer P(VDF-HFP) fabric functionalized with core–shell SiO<sub>2</sub>/ZnO/ZIF-8 (SZZ) nanoparticles. Specifically, MLFs achieve effective and stable energy harvesting in triboelectric nanogenerators (TENGs) with hydrophobicity and antibacterial properties. Meanwhile, MLFs also have high mid-infrared emissivity and sunlight reflectivity, successfully realizing radiative cooling under different climates, and have been applied in wearing clothing, roof shading, and car covers. This work may contribute to the design and manufacturing of next-generation thermal comfort smart fabrics and wearable electronics, particularly in terms of the rational design of multifunctional devices.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31085–31097 31085–31097"},"PeriodicalIF":15.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609544","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Biocompatible Acellular Dermal Matrix-Based Neuromorphic Device with Ultralow Voltage, Ion Channel Emulation, and Synaptic Forgetting Visualization Computation 具有超低电压、离子通道仿真和突触遗忘可视化计算功能的生物相容性细胞真皮基质神经形态设备
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsnano.4c1038310.1021/acsnano.4c10383
Lei Li, Yihua Xu, Qunkai Peng, Pei Huang, Xinqing Duan, Mingqiang Wang, Yu Jiang, Jie Wang, Srinivasan Periasamy, Dar-Jen Hsieh and Kuan-Chang Chang*, 
{"title":"Biocompatible Acellular Dermal Matrix-Based Neuromorphic Device with Ultralow Voltage, Ion Channel Emulation, and Synaptic Forgetting Visualization Computation","authors":"Lei Li,&nbsp;Yihua Xu,&nbsp;Qunkai Peng,&nbsp;Pei Huang,&nbsp;Xinqing Duan,&nbsp;Mingqiang Wang,&nbsp;Yu Jiang,&nbsp;Jie Wang,&nbsp;Srinivasan Periasamy,&nbsp;Dar-Jen Hsieh and Kuan-Chang Chang*,&nbsp;","doi":"10.1021/acsnano.4c1038310.1021/acsnano.4c10383","DOIUrl":"https://doi.org/10.1021/acsnano.4c10383https://doi.org/10.1021/acsnano.4c10383","url":null,"abstract":"<p >Neuromorphic bioelectronics aim to integrate electronics with biological systems yet encounter challenges in biocompatibility, operating voltages, power consumption, and stability. This study presents biocompatible neuromorphic devices fabricated from acellular dermal matrix (ADM) derived from porcine dermis using low-temperature supercritical CO<sub>2</sub> extraction. The ADM preserves the natural scaffold structure of collagen and minimizes immunogenicity by eliminating cells, fats, and noncollagenous impurities, ensuring excellent biocompatibility. The ADM-based devices emulate biological ion channels with biphasic membrane current modulation, exhibiting temperature dependency and pH sensitivity. It operates at an ultralow voltage of 1 mV and demonstrates reliable synaptic modulation exceeding 4 × 10<sup>4</sup> endurance cycles. The activation voltage can be theoretically as low as 59 μV, comparable to brainwave signals with a power of merely 7 aJ/event. Furthermore, a brain-like forgetting visualization algorithm is developed, leveraging the synaptic forgetting plasticity of ADM-based devices to achieve complex computing tasks in a highly energy-efficient manner. Neuromorphic devices based on ADM not only hold potential in implantable biointerfaces due to their exceptional biocompatibility, ultralow voltage, and power but also provide a feasible way for energy-efficient computing paradigms through a synergistic hardware-software approach.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31309–31322 31309–31322"},"PeriodicalIF":15.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Molecular Dynamics of Catalyst-Free Edge Elongation of Boron Nitride Nanotubes Coaxially Grown on Single-Walled Carbon Nanotubes 单壁碳纳米管上同轴生长的氮化硼纳米管无催化剂边缘伸长的分子动力学研究
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsnano.4c1379210.1021/acsnano.4c13792
Kaoru Hisama*, Ksenia V. Bets, Nitant Gupta, Ryo Yoshikawa, Yongjia Zheng, Shuhui Wang, Ming Liu, Rong Xiang, Keigo Otsuka, Shohei Chiashi, Boris I. Yakobson and Shigeo Maruyama*, 
{"title":"Molecular Dynamics of Catalyst-Free Edge Elongation of Boron Nitride Nanotubes Coaxially Grown on Single-Walled Carbon Nanotubes","authors":"Kaoru Hisama*,&nbsp;Ksenia V. Bets,&nbsp;Nitant Gupta,&nbsp;Ryo Yoshikawa,&nbsp;Yongjia Zheng,&nbsp;Shuhui Wang,&nbsp;Ming Liu,&nbsp;Rong Xiang,&nbsp;Keigo Otsuka,&nbsp;Shohei Chiashi,&nbsp;Boris I. Yakobson and Shigeo Maruyama*,&nbsp;","doi":"10.1021/acsnano.4c1379210.1021/acsnano.4c13792","DOIUrl":"https://doi.org/10.1021/acsnano.4c13792https://doi.org/10.1021/acsnano.4c13792","url":null,"abstract":"<p >Recent advances in low-dimensional materials have enabled the synthesis of single-walled carbon nanotubes encapsulated in hexagonal boron nitride (BN) nanotubes (SWCNT@BNNT), creating one-dimensional van der Waals (vdW) heterostructures. However, controlling the quality and crystallinity of BNNT on the surface of SWCNTs using chemical vapor deposition (CVD) remains a challenge. To better understand the growth mechanism of the BNNT in SWCNT@BNNT, we conducted molecular dynamics (MD) simulations using empirical potentials. The simulation results suggest that spontaneous BN nucleation is unlikely to occur on the outer surface of the SWCNT when we assume only vdW interaction between the BN and SWCNT layers. However, we observe the elongation of the BNNT when a short BNNT is provided as a seed nucleus on the SWCNT. This grown BNNT structure, with its sharply cut edges, aligns with experimental observations made using transmission electron microscopy (TEM). Moreover, the edge-reconstruction process favors zigzag B edges, which exhibit low edge energy according to the ReaxFF potential. Our simulation successfully provides insights into the catalyst-free growth process of this one-dimensional vdW heterostructure.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31586–31595 31586–31595"},"PeriodicalIF":15.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c13792","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609282","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Ultrasonic Control of Polymer-Capped Plasmonic Molecules 超声波控制聚合物封装的质子分子
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsnano.4c1091210.1021/acsnano.4c10912
Yingying Cai*, Swagato Sarkar, Yuwen Peng, Tobias A. F. König and Philipp Vana, 
{"title":"Ultrasonic Control of Polymer-Capped Plasmonic Molecules","authors":"Yingying Cai*,&nbsp;Swagato Sarkar,&nbsp;Yuwen Peng,&nbsp;Tobias A. F. König and Philipp Vana,&nbsp;","doi":"10.1021/acsnano.4c1091210.1021/acsnano.4c10912","DOIUrl":"https://doi.org/10.1021/acsnano.4c10912https://doi.org/10.1021/acsnano.4c10912","url":null,"abstract":"<p >Plasmonic molecules (PMs) composed of polymer-capped nanoparticles represent an emerging material class with precise optical functionalities. However, achieving controlled structural changes in metallic nanoparticle aggregation at the nanoscale, similar to the modification of atomic structures, remains challenging. This study demonstrates the 2D/3D isomerization of such plasmonic molecules induced by a controlled ultrasound process. We used two types of gold nanoparticles, each functionalized with hydrogen bonding (HB) donor or acceptor polymers, to self-assemble into different AB<sub><i>N</i></sub>-type complexes via interparticle polymer bundles acting as molecular bonds. Post-ultrasonication treatment significantly shortens these bonds from approximately 14 to 2 nm by enhancing HB cross-linking within the bundles. This drastic change in the bond length increases the stiffness of the resulting clusters, facilitating the transition from 2D to 3D configurations in 100% yield during drop-casting onto substrates. Our results advance the precise control of PMs’ nanoarchitectures and provide insights for their broad applications in sensing, optoelectronics, and metamaterials.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31360–31371 31360–31371"},"PeriodicalIF":15.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnano.4c10912","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Persistent Exciton Dressed by Weak Polaronic Effect in Rigid and Harmonic Lattice Dion–Jacobson 2D Perovskites 刚性和谐波晶格迪昂-雅各布森二维过氧化物中受弱极性效应抑制的持久激子
IF 15.8 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsnano.4c1213210.1021/acsnano.4c12132
Haixin Lei, Yu Xu, Yao Zhang, Qingjie Feng, Hongzhi Zhou, Wei Tang, Jiaoyang Wang, Linjun Li, Guangjun Nan, Weigao Xu and Haiming Zhu*, 
{"title":"Persistent Exciton Dressed by Weak Polaronic Effect in Rigid and Harmonic Lattice Dion–Jacobson 2D Perovskites","authors":"Haixin Lei,&nbsp;Yu Xu,&nbsp;Yao Zhang,&nbsp;Qingjie Feng,&nbsp;Hongzhi Zhou,&nbsp;Wei Tang,&nbsp;Jiaoyang Wang,&nbsp;Linjun Li,&nbsp;Guangjun Nan,&nbsp;Weigao Xu and Haiming Zhu*,&nbsp;","doi":"10.1021/acsnano.4c1213210.1021/acsnano.4c12132","DOIUrl":"https://doi.org/10.1021/acsnano.4c12132https://doi.org/10.1021/acsnano.4c12132","url":null,"abstract":"<p >The emerging two-dimensional (2D) Dion–Jacobson (DJ) perovskites with bidentate ligands have attracted significant attention due to enhanced structural stability compared with conventional Ruddlesden–Popper (RP) perovskites with monodentate ligands linked by van der Waals interactions. However, how the pure chemical bond lattice interacts with excited state excitons and its impact on the exciton nature and dynamics in 2D DJ-perovskites, particularly in comparison to RP-perovskites, remains unexplored. Herein, by a combined spectroscopy study on excitonic and structural dynamics, we reveal a persistent exciton dressed by a weak polaronic effect in DJ-perovskite due to their rigid and harmonic lattice, in striking contrast to significantly screened exciton polaron observed in RP-perovskites. Despite the similar exciton binding energy (∼0.3 eV) in both <i>n</i> = 1 DJ- and RP-perovskites with near-identical crystal structure, photoexcitation results in a slightly screened exciton with minimal structural relaxation and a retained binding energy of ∼0.29 eV in DJ-perovskites but strongly screened exciton polaron with a binding energy of ∼0.13 eV in RP-perovskites. Structural dynamics further highlight the rigid and harmonic lattice motion in DJ-perovskites, as opposed to the thermally activated anharmonic lattice in RP-perovskites, arising from their distinct bonding modes. Our study offers insights into modulating excited state properties in 2D perovskites, simulating the rational design of hybrid semiconductors with tailored properties and functionalities.</p>","PeriodicalId":15,"journal":{"name":"ACS Earth and Space Chemistry","volume":"18 45","pages":"31485–31494 31485–31494"},"PeriodicalIF":15.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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
Oxychlorine and Carbonate Generation by Simulated Electrostatic Discharge of Martian Dust Activities and Detection by Raman Spectroscopy 火星尘埃活动的模拟静电放电产生的氧氯和碳酸盐以及拉曼光谱的检测
IF 2.9 3区 化学
ACS Earth and Space Chemistry Pub Date : 2024-10-31 DOI: 10.1021/acsearthspacechem.4c0010410.1021/acsearthspacechem.4c00104
Junqi Ren, Wenshuo Mao*, Zhongchen Wu, Xiaohui Fu, Qiyuan Hou, Mingyu Chen and Ziwei Fu, 
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