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A Tribute to Alec M. Wodtke
IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1021/acs.jpca.5c0132210.1021/acs.jpca.5c01322
Hua Guo*, Gerard Meijer* and Xueming Yang*, 
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引用次数: 0
Looking Backward and Forward
IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1021/acs.jpcc.5c0132310.1021/acs.jpcc.5c01323
Alec Wodtke*, 
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引用次数: 0
A Tribute to Alec M. Wodtke
IF 3.3 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1021/acs.jpcc.5c0132110.1021/acs.jpcc.5c01321
Hua Guo*, Gerard Meijer* and Xueming Yang*, 
{"title":"A Tribute to Alec M. Wodtke","authors":"Hua Guo*, Gerard Meijer* and Xueming Yang*, ","doi":"10.1021/acs.jpcc.5c0132110.1021/acs.jpcc.5c01321","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c01321https://doi.org/10.1021/acs.jpcc.5c01321","url":null,"abstract":"","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"129 13","pages":"6059–6061 6059–6061"},"PeriodicalIF":3.3,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758756","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
Looking Backward and Forward
IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-04-03 DOI: 10.1021/acs.jpca.5c0132410.1021/acs.jpca.5c01324
Alec Wodtke*, 
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引用次数: 0
Excitation Induced Mechanical Softening and Plastic Deformation in SiO2 and Al2O3
IF 4.126 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1021/acs.jpcc.5c00352
T. Thuy Hoang, Junhyeok Bang
Precise shaping of glass oxides is vital for microelectronics, but it traditionally requires high-temperature processes that can damage components. Recent experiments revealed low-temperature but electron-beam-induced superplastic deformation in amorphous silica, hinting at a nonthermal mechanism, though the role of electronic excitation remains unclear. In this work, we investigated the nonthermal effects of electronic excitation on the mechanical and electronic properties of α-SiO2, α-Al2O3, κ-Al2O3, and amorphous SiO2. While the glass oxides exhibit strong covalent or ionic bonding in the electronic ground state, characterized by high elastic constants and phonon frequencies, both properties significantly decrease under electronic excitation. Based on the results, we found that the superplastic deformation under electron beam irradiation is primarily driven by a bond-switching mechanism. This study provides theoretical insights into the mechanisms underlying superplastic deformation and offers a foundation for developing precise nanoscale shaping techniques for oxide materials.
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引用次数: 0
Active Learning for the Discovery of Binary Intermetallic Compounds as Advanced Interconnects
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1021/acs.jpclett.5c00386
Guoxiang Cui, Zikang Guo, Xiangyu Ren, Yuhang Jiang, Xinyu Jin, Yunwen Wu, Shenghong Ju
The scaling of advanced integrated circuits has posed significant challenges for traditional Cu interconnects, including increased resistivity and reduced electromigration lifetime. Materials with high cohesive energy and low ρ0 × λ values are emerging as promising alternatives. In this work, active learning coupling density functional theory (DFT) computation is employed to accelerate the discovery of binary intermetallic compounds for interconnect materials. Following five active learning iterations, 100 compounds are screened out. Among them, the proportion of promising materials reaches an impressive 76%, in sharp contrast to a paltry 4.9% under traditional random screening. Moreover, this research adopts an interpretable machine learning method to provide further physical insights. The Shapley additive explanations (SHAP) analysis revealed that binary intermetallic compounds featuring small cell volumes and similar Mendeleev numbers tend to possess low ρ0 × λ values. Several promising intermetallic candidates were also identified, including VMo, IrRh3, PtRh3, NbRu, and CrIr3, as potential alternatives to traditional Cu interconnects in future technology nodes. The findings in the study highlight the immense potential of machine learning techniques to accelerate the discovery of novel high-performance interconnect materials.
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引用次数: 0
Three-Component Synthesis of Oxazolidinones via Phosphine-Catalyzed Fixation of Carbon Dioxide and Mechanistic Investigation in Mass Spectrometry
IF 4.354 2区 化学 Q1 CHEMISTRY, ORGANIC Pub Date : 2025-04-02 DOI: 10.1021/acs.joc.4c03034
Wangyu Li, Shiwen Zhou, He Tang, Fengjian Chu, Hongru Feng, Yuanjiang Pan
A phosphine-catalyzed three-component cyclization reaction between anilines, carbon dioxide, and chloroalkanes was developed for the synthesis of oxazolidinones. This strategy not only proceeds under ambient CO2 pressure and metal-free condition but also shows a broad substrate scope, including aromatic amines, aliphatic amines, chiral amino acid esters, and bioactive molecules, providing an efficient and environmentally benign route to synthesize pharmaceutically relevant N-aryl-oxazolidinones. Mechanistic investigations utilizing mass spectrometry (MS) indicate the involvement of multiple phosphine intermediates in this process, thereby elucidating the underlying mechanism. Moreover, the relationships between these phosphine intermediates and Tolman cone angles or the solvent effect of phosphines were examined through mass spectrometry.
{"title":"Three-Component Synthesis of Oxazolidinones via Phosphine-Catalyzed Fixation of Carbon Dioxide and Mechanistic Investigation in Mass Spectrometry","authors":"Wangyu Li, Shiwen Zhou, He Tang, Fengjian Chu, Hongru Feng, Yuanjiang Pan","doi":"10.1021/acs.joc.4c03034","DOIUrl":"https://doi.org/10.1021/acs.joc.4c03034","url":null,"abstract":"A phosphine-catalyzed three-component cyclization reaction between anilines, carbon dioxide, and chloroalkanes was developed for the synthesis of oxazolidinones. This strategy not only proceeds under ambient CO<sub>2</sub> pressure and metal-free condition but also shows a broad substrate scope, including aromatic amines, aliphatic amines, chiral amino acid esters, and bioactive molecules, providing an efficient and environmentally benign route to synthesize pharmaceutically relevant <i>N</i>-aryl-oxazolidinones. Mechanistic investigations utilizing mass spectrometry (MS) indicate the involvement of multiple phosphine intermediates in this process, thereby elucidating the underlying mechanism. Moreover, the relationships between these phosphine intermediates and Tolman cone angles or the solvent effect of phosphines were examined through mass spectrometry.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"25 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Hydrogen technology for maritime applications: A review of challenges, opportunities, and lessons from the port authority of New York and New Jersey
IF 16.3 1区 工程技术 Q1 ENERGY & FUELS Pub Date : 2025-04-02 DOI: 10.1016/j.rser.2025.115641
Veronika Semchukova, Kevin Topolski, Zainul Abdin
The maritime industry faces increasing demand for energy security, operational efficiency, and environmental performance improvements. Hydrogen technology, considered a potential energy carrier, is being explored for port operations, including cargo-handling equipment, heavy-duty vehicles, and stationary power systems. This review evaluates the feasibility, challenges, and potential benefits of hydrogen integration within port infrastructure, using the Port Authority of New York and New Jersey as a representative case study. Drawing on case studies, technical reports, and policy analyses, this study examines the infrastructural, regulatory, and operational factors influencing large-scale deployment, emphasizing supply chain development, storage requirements, and refueling infrastructure. By situating hydrogen within broader maritime energy transition efforts, this review provides an evidence-based assessment of its role in port operations and energy diversification strategies. The findings outline key barriers to adoption and emphasize the need for coordinated efforts among stakeholders to determine hydrogen's role alongside other emerging energy technologies.
{"title":"Hydrogen technology for maritime applications: A review of challenges, opportunities, and lessons from the port authority of New York and New Jersey","authors":"Veronika Semchukova,&nbsp;Kevin Topolski,&nbsp;Zainul Abdin","doi":"10.1016/j.rser.2025.115641","DOIUrl":"10.1016/j.rser.2025.115641","url":null,"abstract":"<div><div>The maritime industry faces increasing demand for energy security, operational efficiency, and environmental performance improvements. Hydrogen technology, considered a potential energy carrier, is being explored for port operations, including cargo-handling equipment, heavy-duty vehicles, and stationary power systems. This review evaluates the feasibility, challenges, and potential benefits of hydrogen integration within port infrastructure, using the Port Authority of New York and New Jersey as a representative case study. Drawing on case studies, technical reports, and policy analyses, this study examines the infrastructural, regulatory, and operational factors influencing large-scale deployment, emphasizing supply chain development, storage requirements, and refueling infrastructure. By situating hydrogen within broader maritime energy transition efforts, this review provides an evidence-based assessment of its role in port operations and energy diversification strategies. The findings outline key barriers to adoption and emphasize the need for coordinated efforts among stakeholders to determine hydrogen's role alongside other emerging energy technologies.</div></div>","PeriodicalId":418,"journal":{"name":"Renewable and Sustainable Energy Reviews","volume":"216 ","pages":"Article 115641"},"PeriodicalIF":16.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143759700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Numerical Calculations of Electric Response Properties Using the Bubbles and Cube Framework.
IF 2.7 2区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1021/acs.jpca.5c00849
Eelis Solala, Wen-Hua Xu, Pauli Parkkinen, Dage Sundholm

We have developed a fully numerical method for calculating the response of the Hartree-Fock orbitals to an external electric field. The Hartree-Fock orbitals are optimized using Green's function methods by iterative numerical integration of the convolution with the Helmholtz kernel. The orbital response is obtained analogously by iterative numerical integration of the convolution with the Helmholtz kernel of the Sternheimer equation. The orbitals are expanded in atom-centered functions (bubbles), consisting of numerical radial functions multiplied by spherical harmonics. The remainder, i.e., the difference between the bubble expansion and the exact orbitals, is expanded in numerical tensorial local basis functions on a three-dimensional grid (cube). The methods have been tested by calculating polarizabilities for He, H2, and NH3, which are compared to the literature values.

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引用次数: 0
Electron–Vibration Couplings Open New Channels for Energy Redistribution of Self-Assembled Monolayers on Plasmonic Nanoparticles
IF 6.475 2区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-04-02 DOI: 10.1021/acs.jpclett.4c02930
Quanbing Pei, Xiaoxuan Zheng, Junjun Tan, Yi Luo, Shuji Ye
Unveiling how the interaction between self-assembled monolayers and plasmonic nanoparticles (PNPs) impacts molecular vibrational energy redistribution (VER) is crucial for optimizing plasmon-mediated chemical reactions (PMCRs). However, direct experimental evidence for molecule–PNP interactions opening new energy channels, such as up-pumping energy transfer and self-trapping of vibrational excitation, for VER has yet to be validated. Here, we demonstrate that electron–vibration coupling (EVC) induced by molecule–PNP interactions can open these new pathways for VER by utilizing femtosecond time-resolved sum-frequency generation vibrational spectroscopy. Using self-assembled 4-nitrothiophenol (4-NTP) monolayers on PNPs as a model, we observed that EVC opens a “forbidden” up-pumping energy transfer channel from 4-NTP nitro symmetric stretching (νNO2) to phenyl ring C═C stretching (νC═C) modes. The self-trapped state of excited νC═C modes is found, which originates from EVC-driven intermolecular coupling. These findings contribute to a better understanding of PMCR mechanisms and help guide the design of plasmonic catalysts with excellent performance.
{"title":"Electron–Vibration Couplings Open New Channels for Energy Redistribution of Self-Assembled Monolayers on Plasmonic Nanoparticles","authors":"Quanbing Pei, Xiaoxuan Zheng, Junjun Tan, Yi Luo, Shuji Ye","doi":"10.1021/acs.jpclett.4c02930","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02930","url":null,"abstract":"Unveiling how the interaction between self-assembled monolayers and plasmonic nanoparticles (PNPs) impacts molecular vibrational energy redistribution (VER) is crucial for optimizing plasmon-mediated chemical reactions (PMCRs). However, direct experimental evidence for molecule–PNP interactions opening new energy channels, such as up-pumping energy transfer and self-trapping of vibrational excitation, for VER has yet to be validated. Here, we demonstrate that electron–vibration coupling (EVC) induced by molecule–PNP interactions can open these new pathways for VER by utilizing femtosecond time-resolved sum-frequency generation vibrational spectroscopy. Using self-assembled 4-nitrothiophenol (4-NTP) monolayers on PNPs as a model, we observed that EVC opens a “forbidden” up-pumping energy transfer channel from 4-NTP nitro symmetric stretching (ν<sub>NO2</sub>) to phenyl ring C═C stretching (ν<sub>C═C</sub>) modes. The self-trapped state of excited ν<sub>C═C</sub> modes is found, which originates from EVC-driven intermolecular coupling. These findings contribute to a better understanding of PMCR mechanisms and help guide the design of plasmonic catalysts with excellent performance.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"73 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
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