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Monomer Substitution Assisted CdTeSe Magic-Size Cluster Development from CdTe and CdSe Prenucleation Clusters in Dispersion at Room Temperature
IF 7.2 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-10 DOI: 10.1021/acs.chemmater.5c0003010.1021/acs.chemmater.5c00030
Yusha Yang, Rui Huang, Yuqi Liu, Chunchun Zhang, Andrei V. Sapelkin, Xiaoqin Chen* and Kui Yu*, 
{"title":"Monomer Substitution Assisted CdTeSe Magic-Size Cluster Development from CdTe and CdSe Prenucleation Clusters in Dispersion at Room Temperature","authors":"Yusha Yang,&nbsp;Rui Huang,&nbsp;Yuqi Liu,&nbsp;Chunchun Zhang,&nbsp;Andrei V. Sapelkin,&nbsp;Xiaoqin Chen* and Kui Yu*,&nbsp;","doi":"10.1021/acs.chemmater.5c0003010.1021/acs.chemmater.5c00030","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00030https://doi.org/10.1021/acs.chemmater.5c00030","url":null,"abstract":"<p >The synthesis promise of prenucleation-stage samples of binary semiconductor quantum dots at room temperature (RT) remains largely unknown. Here we present the development of ternary CdTeSe magic-size clusters (MSCs) MSC-422 (displaying optical absorption peaking at 422 nm) at RT from mixtures of two prenucleation-stage samples of CdTe and CdSe in alcohol-containing toluene. The two samples were prepared at 130 or 140 °C from a reaction of cadmium acetate [Cd(OAc)<sub>2</sub>] and tri-<i>n</i>-octylphosphine chalcogenide (ETOP, E = Te, Se) in oleylamine, respectively. When CdTe was dispersed in the alcohol–toluene mixture, CdTe MSC-448 was seen; after CdSe addition, CdTeSe MSC-422 developed. To explain the result, we propose that the prenucleation cluster in CdTe transformed to CdTeSe MSC-422 via an intermediate stage involving the precursor compound (PC-448) of MSC-448 and PC-422. The PC-448 to PC-422 transformation was assisted by monomer substitution (rather than anion exchange). Our findings bring deeper insights into the synthesis power of PNCs that proceeds with number conservation of Cd–E bonds and pave the way to utilizing monomer substitution for MSC synthesis.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2855–2866 2855–2866"},"PeriodicalIF":7.2,"publicationDate":"2025-04-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Reversible On-Surface Metalation and Demetalation of Porphyrins in a Solvent-Free Ultrahigh-Vacuum Environment 无溶剂超高真空环境中卟啉的可逆表面金属化和脱金属化
IF 7.2 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-09 DOI: 10.1021/acs.chemmater.4c0342010.1021/acs.chemmater.4c03420
Zewei Yi, Zhaoyu Zhang, Rujia Hou, Yuhong Gao, Yuan Guo, Yuanqi Ding, Lei Xie, Fei Song, Chi Zhang* and Wei Xu*, 
{"title":"Reversible On-Surface Metalation and Demetalation of Porphyrins in a Solvent-Free Ultrahigh-Vacuum Environment","authors":"Zewei Yi,&nbsp;Zhaoyu Zhang,&nbsp;Rujia Hou,&nbsp;Yuhong Gao,&nbsp;Yuan Guo,&nbsp;Yuanqi Ding,&nbsp;Lei Xie,&nbsp;Fei Song,&nbsp;Chi Zhang* and Wei Xu*,&nbsp;","doi":"10.1021/acs.chemmater.4c0342010.1021/acs.chemmater.4c03420","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03420https://doi.org/10.1021/acs.chemmater.4c03420","url":null,"abstract":"<p >Controlling molecular interconversions reversibly is of great interest in chemistry. Reversible molecular interconversions have been extensively realized on solid surfaces by the regulation of intermolecular noncovalent interactions and intramolecular covalent bonds. Among others, molecular reactions involving the reversible tuning of intramolecular covalent bonds have typically been induced by local manipulations on individual molecules using a scanning probe microscopy (SPM) tip. However, reversible control of on-surface molecular reactions in a global manner remains challenging. In this work, by a combination of scanning tunneling microscopy (STM) imaging, X-ray photoelectron spectroscopy (XPS) measurements, and density functional theory (DFT) calculations, we report the reversible metalation and demetalation of porphyrin molecules on Au(111) in a controllable and global manner in a solvent-free ultrahigh-vacuum (UHV) environment by providing different atmospheres. The universality of such reactions involving the alkali metal Na was demonstrated by two types of porphyrins with different molecular backbones, while the on-surface metalation with the transition metal Co forming Co-porphyrin was found to be unidirectional. DFT calculations revealed the driving force for their different demetalation behaviors and further illustrated the critical role of extrinsic H atoms in the demetalation pathways. Our results represent a general strategy to reversibly steer the on-surface molecular metalation and demetalation, which should provide fundamental understanding of reversible molecular interconversions.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2806–2814 2806–2814"},"PeriodicalIF":7.2,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Reversible On-Surface Metalation and Demetalation of Porphyrins in a Solvent-Free Ultrahigh-Vacuum Environment
IF 8.6 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-09 DOI: 10.1021/acs.chemmater.4c03420
Zewei Yi, Zhaoyu Zhang, Rujia Hou, Yuhong Gao, Yuan Guo, Yuanqi Ding, Lei Xie, Fei Song, Chi Zhang, Wei Xu
{"title":"Reversible On-Surface Metalation and Demetalation of Porphyrins in a Solvent-Free Ultrahigh-Vacuum Environment","authors":"Zewei Yi, Zhaoyu Zhang, Rujia Hou, Yuhong Gao, Yuan Guo, Yuanqi Ding, Lei Xie, Fei Song, Chi Zhang, Wei Xu","doi":"10.1021/acs.chemmater.4c03420","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03420","url":null,"abstract":"Controlling molecular interconversions reversibly is of great interest in chemistry. Reversible molecular interconversions have been extensively realized on solid surfaces by the regulation of intermolecular noncovalent interactions and intramolecular covalent bonds. Among others, molecular reactions involving the reversible tuning of intramolecular covalent bonds have typically been induced by local manipulations on individual molecules using a scanning probe microscopy (SPM) tip. However, reversible control of on-surface molecular reactions in a global manner remains challenging. In this work, by a combination of scanning tunneling microscopy (STM) imaging, X-ray photoelectron spectroscopy (XPS) measurements, and density functional theory (DFT) calculations, we report the reversible metalation and demetalation of porphyrin molecules on Au(111) in a controllable and global manner in a solvent-free ultrahigh-vacuum (UHV) environment by providing different atmospheres. The universality of such reactions involving the alkali metal Na was demonstrated by two types of porphyrins with different molecular backbones, while the on-surface metalation with the transition metal Co forming Co-porphyrin was found to be unidirectional. DFT calculations revealed the driving force for their different demetalation behaviors and further illustrated the critical role of extrinsic H atoms in the demetalation pathways. Our results represent a general strategy to reversibly steer the on-surface molecular metalation and demetalation, which should provide fundamental understanding of reversible molecular interconversions.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"21 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806420","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Steric Hindrance and Film Quality in HfO2 Atomic Layer Deposition: Comparative Kinetic Monte Carlo Simulation of TEMA-Hf and HfCp(NMe2)3 Precursors
IF 8.6 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.5c00024
Haojie Li, Yanwei Wen, Yiao Ge, Qiyuan Ruan, Hongliang Lü, Wanliang Tan, Fangzhou Yu, Zhang Liu, Kun Cao, Bin Shan, Jeffrey Xu, Rong Chen
{"title":"Steric Hindrance and Film Quality in HfO2 Atomic Layer Deposition: Comparative Kinetic Monte Carlo Simulation of TEMA-Hf and HfCp(NMe2)3 Precursors","authors":"Haojie Li, Yanwei Wen, Yiao Ge, Qiyuan Ruan, Hongliang Lü, Wanliang Tan, Fangzhou Yu, Zhang Liu, Kun Cao, Bin Shan, Jeffrey Xu, Rong Chen","doi":"10.1021/acs.chemmater.5c00024","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00024","url":null,"abstract":"Hafnia (HfO<sub>2</sub>)-based ferroelectrics have attracted considerable attention for next-generation memory devices due to their robust ferroelectricity at ultrathin scales. Achieving desired ferroelectric properties relies on the precise control of film quality, which is strongly influenced by deposition conditions, precursor chemistry, and the presence of impurities. Here, we combine density functional theory and kinetic Monte Carlo simulations to investigate the atomic layer deposition of HfO<sub>2</sub> films from TEMA–Hf and HfCp(NMe<sub>2</sub>)<sub>3</sub> precursors using O<sub>3</sub> as the oxidant. Our results show that both precursors decompose preferentially at 2-coordinate O sites on the HfO<sub>2</sub> surface, while 3-coordinate O sites present much higher energy barriers. Kinetic Monte Carlo simulations reveal that growth rates per cycle (GPC) of TEMA-Hf and HfCp(NMe<sub>2</sub>)<sub>3</sub> with O<sub>3</sub> are 0.094–0.109 nm/cycle and 0.081–0.096 nm/cycle from 150 to 350 °C, aligning closely with experiments. The slower GPC observed for HfCp(NMe<sub>2</sub>)<sub>3</sub> is attributed to the greater steric hindrance of the cyclopentadienyl ligand (Cp) compared to the dimethylamide(NMe<sub>2</sub>) groups. Film morphology analysis suggests TEMA-Hf leads to smoother HfO<sub>2</sub> films. Nitrogen incorporation remains at about 1% for TEMA–Hf and HfCp(NMe<sub>2</sub>)<sub>3</sub>, consistent with experimental observations, while the concentration of O vacancies slightly decreases with the increase of deposition temperature. These findings provide insights into how precursor selection and atomic-level reaction pathways influence film growth and composition, thereby affecting the ferroelectric performance in HfO<sub>2</sub>-based devices.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"64 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Integrating Large Language Models into the Chemistry and Materials Science Laboratory Curricula
IF 8.6 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.5c00111
Annalise E. Maughan, Eric S. Toberer, Alexandra Zevalkink
{"title":"Integrating Large Language Models into the Chemistry and Materials Science Laboratory Curricula","authors":"Annalise E. Maughan, Eric S. Toberer, Alexandra Zevalkink","doi":"10.1021/acs.chemmater.5c00111","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00111","url":null,"abstract":"How might LLMs impact student learning in laboratory settings, especially regarding critical thinking, core concepts, and scientific identity? What are the ramifications of LLMs for course delivery strategies, including course design, scaffolding, and assessment? Can LLMs facilitate the incorporation of alternative delivery strategies into the undergraduate curriculum, such as course-based undergraduate research experiences (CUREs), to potentially broaden access to authentic research? Figure 1. Demonstration of data visualization and analysis generated entirely by natural language prompting using ChatGPT-4o. The first example highlights data analysis from a general chemistry absorption spectroscopy laboratory, in which students are asked to (a) generate a calibration curve and (b) determine the concentration of an unknown analyte using Beer’s law. The second example illustrates a chemical kinetics experiment familiar to upper division physical chemistry laboratories. Students (c) collect and visualize time-dependent absorbance data, relate the measured absorbance to analyte concentration with Beer’s law, and then (d) linearize the data to determine the reaction order, rate constant, and integrated rate law. The authors gratefully acknowledge support from the National Science Foundation under Grant No. DMR-2333654. The authors thank the invited workshop speakers: Allyson Fry-Petit, Bo Wu, Taylor Sparks, Boris Kiefer, Susan Gentry, Sam Cox, Mayk Caldas Ramos, and Shruti Badhwar. The authors also gratefully acknowledge all workshop participants for their attendance. This article references 31 other publications. This article has not yet been cited by other publications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"24 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Engineering Noncovalent Molecular Interactions during Polymerization for Tunable Polyampholyte Properties
IF 7.2 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.5c0032810.1021/acs.chemmater.5c00328
Pengyu Chen, Manh Tien Nguyen, Zheyuan Zhang, Alexandra Khlyustova, Xiaojing Ma, Qing Shao* and Rong Yang*, 
{"title":"Engineering Noncovalent Molecular Interactions during Polymerization for Tunable Polyampholyte Properties","authors":"Pengyu Chen,&nbsp;Manh Tien Nguyen,&nbsp;Zheyuan Zhang,&nbsp;Alexandra Khlyustova,&nbsp;Xiaojing Ma,&nbsp;Qing Shao* and Rong Yang*,&nbsp;","doi":"10.1021/acs.chemmater.5c0032810.1021/acs.chemmater.5c00328","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00328https://doi.org/10.1021/acs.chemmater.5c00328","url":null,"abstract":"<p >Conventional free radical polymerization is a prevalent synthesis technique, yet it faces limitations in achieving precisely-controlled copolymers with emergent properties due to the statistical nature and lack of control over noncovalent interactions. This study addresses these challenges by developing a methodology that enables the precise tuning of noncovalent interactions during polymerization through the use of vapor-phase comonomers within a reduced-pressure environment. Utilizing initiated CVD (iCVD), polyampholyte copolymers, which are conventionally difficult to control in terms of composition and solubility, were synthesized with tailored noncovalent interactions. By designing vapor-phase molecular complexes guided by quantum chemical calculations, we demonstrated the synthesis of polyampholytes with a broad range of noncovalent interaction strengths. These interactions altered the hydrophilicity and hydrophobicity of polyampholytes beyond those of the homopolymers. Critically, these tuned interactions significantly influenced biofilm formation by common bacteria, providing a pathway to polyampholyte materials with enhanced or reduced biofilm growth, ranging from 5% to 205% of those grown on homopolymers for applications in engineered living materials or antifouling coatings. This research elucidates a scalable, cost-effective approach to designing functional materials with tailored emergent properties, creating new possibilities for applications across varied sectors, from filtration to biomaterials.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2943–2952 2943–2952"},"PeriodicalIF":7.2,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Integrating Large Language Models into the Chemistry and Materials Science Laboratory Curricula
IF 7.2 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.5c0011110.1021/acs.chemmater.5c00111
Annalise E. Maughan*, Eric S. Toberer* and Alexandra Zevalkink*, 
{"title":"Integrating Large Language Models into the Chemistry and Materials Science Laboratory Curricula","authors":"Annalise E. Maughan*,&nbsp;Eric S. Toberer* and Alexandra Zevalkink*,&nbsp;","doi":"10.1021/acs.chemmater.5c0011110.1021/acs.chemmater.5c00111","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00111https://doi.org/10.1021/acs.chemmater.5c00111","url":null,"abstract":"","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 7","pages":"2389–2394 2389–2394"},"PeriodicalIF":7.2,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Engineering Noncovalent Molecular Interactions during Polymerization for Tunable Polyampholyte Properties
IF 8.6 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.5c00328
Pengyu Chen, Manh Tien Nguyen, Zheyuan Zhang, Alexandra Khlyustova, Xiaojing Ma, Qing Shao, Rong Yang
{"title":"Engineering Noncovalent Molecular Interactions during Polymerization for Tunable Polyampholyte Properties","authors":"Pengyu Chen, Manh Tien Nguyen, Zheyuan Zhang, Alexandra Khlyustova, Xiaojing Ma, Qing Shao, Rong Yang","doi":"10.1021/acs.chemmater.5c00328","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00328","url":null,"abstract":"Conventional free radical polymerization is a prevalent synthesis technique, yet it faces limitations in achieving precisely-controlled copolymers with emergent properties due to the statistical nature and lack of control over noncovalent interactions. This study addresses these challenges by developing a methodology that enables the precise tuning of noncovalent interactions during polymerization through the use of vapor-phase comonomers within a reduced-pressure environment. Utilizing initiated CVD (iCVD), polyampholyte copolymers, which are conventionally difficult to control in terms of composition and solubility, were synthesized with tailored noncovalent interactions. By designing vapor-phase molecular complexes guided by quantum chemical calculations, we demonstrated the synthesis of polyampholytes with a broad range of noncovalent interaction strengths. These interactions altered the hydrophilicity and hydrophobicity of polyampholytes beyond those of the homopolymers. Critically, these tuned interactions significantly influenced biofilm formation by common bacteria, providing a pathway to polyampholyte materials with enhanced or reduced biofilm growth, ranging from 5% to 205% of those grown on homopolymers for applications in engineered living materials or antifouling coatings. This research elucidates a scalable, cost-effective approach to designing functional materials with tailored emergent properties, creating new possibilities for applications across varied sectors, from filtration to biomaterials.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"92 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798534","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Wafer-Scale Evaporated Metallic BiOx as Contact Electrodes of MoS2 Transistors with Enhanced Thermal Stability 晶圆级蒸发金属生物氧化物作为具有更高热稳定性的 MoS2 晶体管的接触电极
IF 7.2 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.4c0354010.1021/acs.chemmater.4c03540
Zhaochao Liu, Jiabiao Chen, Wei Ai, Shuyi Chen, Yuyu He, Zunxian Lv, Mingjian Yang, Wenbin Li, Feng Luo* and Jinxiong Wu*, 
{"title":"Wafer-Scale Evaporated Metallic BiOx as Contact Electrodes of MoS2 Transistors with Enhanced Thermal Stability","authors":"Zhaochao Liu,&nbsp;Jiabiao Chen,&nbsp;Wei Ai,&nbsp;Shuyi Chen,&nbsp;Yuyu He,&nbsp;Zunxian Lv,&nbsp;Mingjian Yang,&nbsp;Wenbin Li,&nbsp;Feng Luo* and Jinxiong Wu*,&nbsp;","doi":"10.1021/acs.chemmater.4c0354010.1021/acs.chemmater.4c03540","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03540https://doi.org/10.1021/acs.chemmater.4c03540","url":null,"abstract":"<p >Bismuth is one of the most widely used contact electrodes in MoS<sub>2</sub> transistors for its capability to minimize the Fermi-level pinning and form ultralow contact resistance. However, the low melting point of bismuth contact will undoubtedly make it incompatible to a high-temperature manufactory process and application scenarios. Here, we introduce that thermal evaporation of α-Bi<sub>2</sub>O<sub>3</sub>, a well-known insulating oxide, can form a highly metallic O-deficient BiO<sub><i>x</i></sub> phase, showing a high Hall mobility (∼60 cm<sup>2</sup> V<sup>–</sup><sup>1</sup> s<sup>–</sup><sup>1</sup>) and ultrahigh carrier density (1.5 × 10<sup>15</sup> cm<sup>–</sup><sup>2</sup>). Detailed microstructural analysis reveals that the wafer-scale evaporated BiO<sub><i>x</i></sub> film possesses a unique structure of polycrystalline Bi dispersed within an amorphous BiO<sub><i>x</i></sub> matrix, preserving ultraflat surface even after heating above the melting temperature of bismuth. Furthermore, the evaporated BiO<sub><i>x</i></sub> film is functionalized as contact electrodes of MoS<sub>2</sub> transistors, exhibiting a high on-state current and an ultrasmall contact resistance of 650 Ω μm. More importantly, thanks to the superior thermal stability, the BiO<sub><i>x</i></sub>-contacted MoS<sub>2</sub> transistor undergoes very slight electrical decays after annealing at 300 °C for 6 h, while the Bi-contacted one becomes totally broken down. Our findings demonstrate thermally evaporated BiO<sub><i>x</i></sub> thin films as an alternative promising contact for MoS<sub>2</sub> transistors.</p>","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 8","pages":"2836–2843 2836–2843"},"PeriodicalIF":7.2,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853960","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Wafer-Scale Evaporated Metallic BiOx as Contact Electrodes of MoS2 Transistors with Enhanced Thermal Stability
IF 8.6 2区 材料科学
Chemistry of Materials Pub Date : 2025-04-08 DOI: 10.1021/acs.chemmater.4c03540
Zhaochao Liu, Jiabiao Chen, Wei Ai, Shuyi Chen, Yuyu He, Zunxian Lv, Mingjian Yang, Wenbin Li, Feng Luo, Jinxiong Wu
{"title":"Wafer-Scale Evaporated Metallic BiOx as Contact Electrodes of MoS2 Transistors with Enhanced Thermal Stability","authors":"Zhaochao Liu, Jiabiao Chen, Wei Ai, Shuyi Chen, Yuyu He, Zunxian Lv, Mingjian Yang, Wenbin Li, Feng Luo, Jinxiong Wu","doi":"10.1021/acs.chemmater.4c03540","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03540","url":null,"abstract":"Bismuth is one of the most widely used contact electrodes in MoS<sub>2</sub> transistors for its capability to minimize the Fermi-level pinning and form ultralow contact resistance. However, the low melting point of bismuth contact will undoubtedly make it incompatible to a high-temperature manufactory process and application scenarios. Here, we introduce that thermal evaporation of α-Bi<sub>2</sub>O<sub>3</sub>, a well-known insulating oxide, can form a highly metallic O-deficient BiO<sub><i>x</i></sub> phase, showing a high Hall mobility (∼60 cm<sup>2</sup> V<sup>–</sup><sup>1</sup> s<sup>–</sup><sup>1</sup>) and ultrahigh carrier density (1.5 × 10<sup>15</sup> cm<sup>–</sup><sup>2</sup>). Detailed microstructural analysis reveals that the wafer-scale evaporated BiO<sub><i>x</i></sub> film possesses a unique structure of polycrystalline Bi dispersed within an amorphous BiO<sub><i>x</i></sub> matrix, preserving ultraflat surface even after heating above the melting temperature of bismuth. Furthermore, the evaporated BiO<sub><i>x</i></sub> film is functionalized as contact electrodes of MoS<sub>2</sub> transistors, exhibiting a high on-state current and an ultrasmall contact resistance of 650 Ω μm. More importantly, thanks to the superior thermal stability, the BiO<sub><i>x</i></sub>-contacted MoS<sub>2</sub> transistor undergoes very slight electrical decays after annealing at 300 °C for 6 h, while the Bi-contacted one becomes totally broken down. Our findings demonstrate thermally evaporated BiO<sub><i>x</i></sub> thin films as an alternative promising contact for MoS<sub>2</sub> transistors.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"74 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143798533","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
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