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High Throughput Correlative Electrochemistry-Microscopy Analysis on a Zn–Al Alloy Zn-Al 合金的高通量电化学-显微镜关联分析
ACS Physical Chemistry Au Pub Date : 2024-05-10 DOI: 10.1021/acsphyschemau.4c00016
Gunani Jayamaha, Levi Tegg, Cameron L. Bentley, Minkyung Kang
{"title":"High Throughput Correlative Electrochemistry-Microscopy Analysis on a Zn–Al Alloy","authors":"Gunani Jayamaha, Levi Tegg, Cameron L. Bentley, Minkyung Kang","doi":"10.1021/acsphyschemau.4c00016","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00016","url":null,"abstract":"Conventional electrodes and electrocatalysts possess complex compositional and structural motifs that impact their overall electrochemical activity. These motifs range from defects and crystal orientation on the electrode surface to layers and composites with other electrode components, such as binders. Therefore, it is vital to identify how these individual motifs alter the electrochemical activity of the electrode. Scanning electrochemical cell microscopy (SECCM) is a powerful tool that has been developed for investigating the electrochemical properties of complex structures. An example of a complex electrode surface is Zn–Al alloys, which are utilized in various sectors ranging from cathodic protection of steel to battery electrodes. Herein, voltammetric SECCM and correlative microstructure analysis are deployed to probe the electrochemical activities of a range of microstructural features, with 651 independent voltammetric measurements made in six distinctive areas on the surface of a Zn–Al alloy. Energy-dispersive X-ray spectroscopy (EDS) mapping reveals that specific phases of the alloy structure, particularly the α-phase Zn–Al, favor the early stages of metal dissolution (i.e., oxidation) and electrochemical reduction processes such as the oxygen reduction reaction (ORR) and redeposition of dissolved metal ions. A correlative analysis performed by comparing high-resolution quantitative elemental composition (i.e., EDS) with the corresponding spatially resolved cyclic voltammograms (i.e., SECCM) shows that the nanospot α-phase of the Zn–Al alloy contains high Al content (30–50%), which may facilitate local Al dissolution as the local pH increases during the ORR in unbuffered aqueous media. Overall, SECCM-based high-throughput electrochemical screening, combined with microstructure analysis, conclusively demonstrates that structure-composition heterogeneity significantly influences the local electrochemical activity on complex electrode surfaces. These insights are invaluable for the rational design of advanced electromaterials.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"14 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140935570","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High Throughput Correlative Electrochemistry-Microscopy Analysis on a Zn–Al Alloy Zn-Al 合金的高通量电化学-显微镜关联分析
IF 3.7
ACS Physical Chemistry Au Pub Date : 2024-05-10 DOI: 10.1021/acsphyschemau.4c0001610.1021/acsphyschemau.4c00016
Gunani Jayamaha, Levi Tegg, Cameron L. Bentley and Minkyung Kang*, 
{"title":"High Throughput Correlative Electrochemistry-Microscopy Analysis on a Zn–Al Alloy","authors":"Gunani Jayamaha,&nbsp;Levi Tegg,&nbsp;Cameron L. Bentley and Minkyung Kang*,&nbsp;","doi":"10.1021/acsphyschemau.4c0001610.1021/acsphyschemau.4c00016","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00016https://doi.org/10.1021/acsphyschemau.4c00016","url":null,"abstract":"<p >Conventional electrodes and electrocatalysts possess complex compositional and structural motifs that impact their overall electrochemical activity. These motifs range from defects and crystal orientation on the electrode surface to layers and composites with other electrode components, such as binders. Therefore, it is vital to identify how these individual motifs alter the electrochemical activity of the electrode. Scanning electrochemical cell microscopy (SECCM) is a powerful tool that has been developed for investigating the electrochemical properties of complex structures. An example of a complex electrode surface is Zn–Al alloys, which are utilized in various sectors ranging from cathodic protection of steel to battery electrodes. Herein, voltammetric SECCM and correlative microstructure analysis are deployed to probe the electrochemical activities of a range of microstructural features, with 651 independent voltammetric measurements made in six distinctive areas on the surface of a Zn–Al alloy. Energy-dispersive X-ray spectroscopy (EDS) mapping reveals that specific phases of the alloy structure, particularly the α-phase Zn–Al, favor the early stages of metal dissolution (i.e., oxidation) and electrochemical reduction processes such as the oxygen reduction reaction (ORR) and redeposition of dissolved metal ions. A correlative analysis performed by comparing high-resolution quantitative elemental composition (i.e., EDS) with the corresponding spatially resolved cyclic voltammograms (i.e., SECCM) shows that the nanospot α-phase of the Zn–Al alloy contains high Al content (30–50%), which may facilitate local Al dissolution as the local pH increases during the ORR in unbuffered aqueous media. Overall, SECCM-based high-throughput electrochemical screening, combined with microstructure analysis, conclusively demonstrates that structure-composition heterogeneity significantly influences the local electrochemical activity on complex electrode surfaces. These insights are invaluable for the rational design of advanced electromaterials.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"4 4","pages":"375–384 375–384"},"PeriodicalIF":3.7,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00016","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141959309","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Theoretical Studies of Anisotropic Melting of Ice Induced by Ultrafast Nonthermal Heating 超快非热加热诱导冰各向异性熔化的理论研究
ACS Physical Chemistry Au Pub Date : 2024-05-08 DOI: 10.1021/acsphyschemau.3c00072
Ibrahim Dawod, Kajwal Patra, Sebastian Cardoch, H. Olof Jönsson, Jonas A. Sellberg, Andrew V. Martin, Jack Binns, Oscar Grånäs, Adrian P. Mancuso, Carl Caleman, Nicusor Timneanu
{"title":"Theoretical Studies of Anisotropic Melting of Ice Induced by Ultrafast Nonthermal Heating","authors":"Ibrahim Dawod, Kajwal Patra, Sebastian Cardoch, H. Olof Jönsson, Jonas A. Sellberg, Andrew V. Martin, Jack Binns, Oscar Grånäs, Adrian P. Mancuso, Carl Caleman, Nicusor Timneanu","doi":"10.1021/acsphyschemau.3c00072","DOIUrl":"https://doi.org/10.1021/acsphyschemau.3c00072","url":null,"abstract":"Water and ice are routinely studied with X-rays to reveal their diverse structures and anomalous properties. We employ a hybrid collisional-radiative/molecular-dynamics method to explore how femtosecond X-ray pulses interact with hexagonal ice. We find that ice makes a phase transition into a crystalline plasma where its initial structure is maintained up to tens of femtoseconds. The ultrafast melting process occurs anisotropically, where different geometric configurations of the structure melt on different time scales. The transient state and anisotropic melting of crystals can be captured by X-ray diffraction, which impacts any study of crystalline structures probed by femtosecond X-ray lasers.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"79 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140935509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Theoretical Studies of Anisotropic Melting of Ice Induced by Ultrafast Nonthermal Heating 超快非热加热诱导冰各向异性熔化的理论研究
IF 3.7
ACS Physical Chemistry Au Pub Date : 2024-05-08 DOI: 10.1021/acsphyschemau.3c0007210.1021/acsphyschemau.3c00072
Ibrahim Dawod*, Kajwal Patra, Sebastian Cardoch, H. Olof Jönsson, Jonas A. Sellberg, Andrew V. Martin, Jack Binns, Oscar Grånäs, Adrian P. Mancuso, Carl Caleman and Nicusor Timneanu*, 
{"title":"Theoretical Studies of Anisotropic Melting of Ice Induced by Ultrafast Nonthermal Heating","authors":"Ibrahim Dawod*,&nbsp;Kajwal Patra,&nbsp;Sebastian Cardoch,&nbsp;H. Olof Jönsson,&nbsp;Jonas A. Sellberg,&nbsp;Andrew V. Martin,&nbsp;Jack Binns,&nbsp;Oscar Grånäs,&nbsp;Adrian P. Mancuso,&nbsp;Carl Caleman and Nicusor Timneanu*,&nbsp;","doi":"10.1021/acsphyschemau.3c0007210.1021/acsphyschemau.3c00072","DOIUrl":"https://doi.org/10.1021/acsphyschemau.3c00072https://doi.org/10.1021/acsphyschemau.3c00072","url":null,"abstract":"<p >Water and ice are routinely studied with X-rays to reveal their diverse structures and anomalous properties. We employ a hybrid collisional-radiative/molecular-dynamics method to explore how femtosecond X-ray pulses interact with hexagonal ice. We find that ice makes a phase transition into a crystalline plasma where its initial structure is maintained up to tens of femtoseconds. The ultrafast melting process occurs anisotropically, where different geometric configurations of the structure melt on different time scales. The transient state and anisotropic melting of crystals can be captured by X-ray diffraction, which impacts any study of crystalline structures probed by femtosecond X-ray lasers.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"4 4","pages":"385–392 385–392"},"PeriodicalIF":3.7,"publicationDate":"2024-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.3c00072","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141957203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rational Design of Far-Red Archaerhodopsin-3-Based Fluorescent Genetically Encoded Voltage Indicators: from Elucidation of the Fluorescence Mechanism in Archers to Novel Red-Shifted Variants 基于远红弓形虫核素-3 的荧光基因编码电压指示器的合理设计:从阐明弓形虫的荧光机制到新型红移变体
ACS Physical Chemistry Au Pub Date : 2024-04-29 DOI: 10.1021/acsphyschemau.3c00073
Dmitrii M. Nikolaev, Vladimir N. Mironov, Ekaterina M. Metelkina, Andrey A. Shtyrov, Andrey S. Mereshchenko, Nikita A. Demidov, Sergey Yu. Vyazmin, Tatiana B. Tennikova, Svetlana E. Moskalenko, Stanislav A. Bondarev, Galina A. Zhouravleva, Andrey V. Vasin, Maxim S. Panov, Mikhail N. Ryazantsev
{"title":"Rational Design of Far-Red Archaerhodopsin-3-Based Fluorescent Genetically Encoded Voltage Indicators: from Elucidation of the Fluorescence Mechanism in Archers to Novel Red-Shifted Variants","authors":"Dmitrii M. Nikolaev, Vladimir N. Mironov, Ekaterina M. Metelkina, Andrey A. Shtyrov, Andrey S. Mereshchenko, Nikita A. Demidov, Sergey Yu. Vyazmin, Tatiana B. Tennikova, Svetlana E. Moskalenko, Stanislav A. Bondarev, Galina A. Zhouravleva, Andrey V. Vasin, Maxim S. Panov, Mikhail N. Ryazantsev","doi":"10.1021/acsphyschemau.3c00073","DOIUrl":"https://doi.org/10.1021/acsphyschemau.3c00073","url":null,"abstract":"Genetically encoded voltage indicators (GEVIs) have found wide applications as molecular tools for visualization of changes in cell membrane potential. Among others, several classes of archaerhodopsin-3-based GEVIs have been developed and have proved themselves promising in various molecular imaging studies. To expand the application range for this type of GEVIs, new variants with absorption band maxima shifted toward the first biological window and enhanced fluorescence signal are required. Here, we integrate computational and experimental strategies to reveal structural factors that distinguish far-red bright archaerhodopsin-3-based GEVIs, Archers, obtained by directed evolution in a previous study (McIsaac et al., <i>PNAS,</i> 2014) and the wild-type archaerhodopsin-3 with an extremely dim fluorescence signal, aiming to use the obtained information in subsequent rational design. We found that the fluorescence can be enhanced by stabilization of a certain conformation of the protein, which, in turn, can be achieved by tuning the p<i>K</i><sub>a</sub> value of two titratable residues. These findings were supported further by introducing mutations into wild-type archeorhodopsin-3 and detecting the enhancement of the fluorescence signal. Finally, we came up with a rational design and proposed previously unknown Archers variants with red-shifted absorption bands (λ<sub>max</sub> up to 640 nm) and potential-dependent bright fluorescence (quantum yield up to 0.97%).","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"76 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140832055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rational Design of Far-Red Archaerhodopsin-3-Based Fluorescent Genetically Encoded Voltage Indicators: from Elucidation of the Fluorescence Mechanism in Archers to Novel Red-Shifted Variants 基于远红弓形虫核素-3 的荧光基因编码电压指示器的合理设计:从阐明弓形虫的荧光机制到新型红移变体
IF 3.7
ACS Physical Chemistry Au Pub Date : 2024-04-29 DOI: 10.1021/acsphyschemau.3c0007310.1021/acsphyschemau.3c00073
Dmitrii M. Nikolaev, Vladimir N. Mironov, Ekaterina M. Metelkina, Andrey A. Shtyrov, Andrey S. Mereshchenko, Nikita A. Demidov, Sergey Yu. Vyazmin, Tatiana B. Tennikova, Svetlana E. Moskalenko, Stanislav A. Bondarev, Galina A. Zhouravleva, Andrey V. Vasin, Maxim S. Panov and Mikhail N. Ryazantsev*, 
{"title":"Rational Design of Far-Red Archaerhodopsin-3-Based Fluorescent Genetically Encoded Voltage Indicators: from Elucidation of the Fluorescence Mechanism in Archers to Novel Red-Shifted Variants","authors":"Dmitrii M. Nikolaev,&nbsp;Vladimir N. Mironov,&nbsp;Ekaterina M. Metelkina,&nbsp;Andrey A. Shtyrov,&nbsp;Andrey S. Mereshchenko,&nbsp;Nikita A. Demidov,&nbsp;Sergey Yu. Vyazmin,&nbsp;Tatiana B. Tennikova,&nbsp;Svetlana E. Moskalenko,&nbsp;Stanislav A. Bondarev,&nbsp;Galina A. Zhouravleva,&nbsp;Andrey V. Vasin,&nbsp;Maxim S. Panov and Mikhail N. Ryazantsev*,&nbsp;","doi":"10.1021/acsphyschemau.3c0007310.1021/acsphyschemau.3c00073","DOIUrl":"https://doi.org/10.1021/acsphyschemau.3c00073https://doi.org/10.1021/acsphyschemau.3c00073","url":null,"abstract":"<p >Genetically encoded voltage indicators (GEVIs) have found wide applications as molecular tools for visualization of changes in cell membrane potential. Among others, several classes of archaerhodopsin-3-based GEVIs have been developed and have proved themselves promising in various molecular imaging studies. To expand the application range for this type of GEVIs, new variants with absorption band maxima shifted toward the first biological window and enhanced fluorescence signal are required. Here, we integrate computational and experimental strategies to reveal structural factors that distinguish far-red bright archaerhodopsin-3-based GEVIs, Archers, obtained by directed evolution in a previous study (McIsaac et al., <i>PNAS,</i> 2014) and the wild-type archaerhodopsin-3 with an extremely dim fluorescence signal, aiming to use the obtained information in subsequent rational design. We found that the fluorescence can be enhanced by stabilization of a certain conformation of the protein, which, in turn, can be achieved by tuning the p<i>K</i><sub>a</sub> value of two titratable residues. These findings were supported further by introducing mutations into wild-type archeorhodopsin-3 and detecting the enhancement of the fluorescence signal. Finally, we came up with a rational design and proposed previously unknown Archers variants with red-shifted absorption bands (λ<sub>max</sub> up to 640 nm) and potential-dependent bright fluorescence (quantum yield up to 0.97%).</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"4 4","pages":"347–362 347–362"},"PeriodicalIF":3.7,"publicationDate":"2024-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.3c00073","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141955179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Important Elements of Spin-Exciton and Magnon-Exciton Coupling 自旋-激子和磁子-激子耦合的重要元素
IF 3.7
ACS Physical Chemistry Au Pub Date : 2024-04-26 DOI: 10.1021/acsphyschemau.4c0001010.1021/acsphyschemau.4c00010
Nicholas J. Brennan, Cora A. Noble, Jiacheng Tang, Michael E. Ziebel* and Youn Jue Bae*, 
{"title":"Important Elements of Spin-Exciton and Magnon-Exciton Coupling","authors":"Nicholas J. Brennan,&nbsp;Cora A. Noble,&nbsp;Jiacheng Tang,&nbsp;Michael E. Ziebel* and Youn Jue Bae*,&nbsp;","doi":"10.1021/acsphyschemau.4c0001010.1021/acsphyschemau.4c00010","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00010https://doi.org/10.1021/acsphyschemau.4c00010","url":null,"abstract":"<p >The recent discovery of spin-exciton and magnon-exciton coupling in a layered antiferromagnetic semiconductor, CrSBr, is both fundamentally intriguing and technologically significant. This discovery unveils a unique capability to optically access and manipulate spin information using excitons, opening doors to applications in quantum interconnects, quantum photonics, and opto-spintronics. Despite their remarkable potential, materials exhibiting spin-exciton and magnon-exciton coupling remain limited. To broaden the library of such materials, we explore key parameters for achieving and tuning spin-exciton and magnon-exciton couplings. We begin by examining the mechanisms of couplings in CrSBr and drawing comparisons with other recently identified two-dimensional magnetic semiconductors. Furthermore, we propose various promising scenarios for spin-exciton coupling, laying the groundwork for future research endeavors.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"4 4","pages":"322–327 322–327"},"PeriodicalIF":3.7,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00010","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141955354","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Physical, Thermal, and Optical Properties of Mn2+ and Nd3+ Containing Barium Phosphate Glasses 含 Mn2+ 和 Nd3+ 磷酸钡玻璃的物理、热和光学特性
ACS Physical Chemistry Au Pub Date : 2024-04-26 DOI: 10.1021/acsphyschemau.4c00020
José A. Jiménez
{"title":"Physical, Thermal, and Optical Properties of Mn2+ and Nd3+ Containing Barium Phosphate Glasses","authors":"José A. Jiménez","doi":"10.1021/acsphyschemau.4c00020","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00020","url":null,"abstract":"This work reports on various properties and analysis of optical interactions in phosphate glasses containing red-emitting Mn<sup>2+</sup> and near-infrared (NIR)-emitting Nd<sup>3+</sup> ions, which are of interest for energy applications and solar spectral converters. The glasses were made by melting with 50P<sub>2</sub>O<sub>5</sub>–(48 – <i>x</i>)BaO–2MnO–<i>x</i>Nd<sub>2</sub>O<sub>3</sub> (<i>x</i> = 0, 0.5, 1.0, and 2.0 mol %) nominal compositions and characterized by X-ray diffraction, density and related physical properties, differential scanning calorimetry, dilatometry, UV–vis–NIR optical absorption, and photoluminescence spectroscopy with decay kinetics analysis. The glasses were X-ray amorphous, wherein the physical and thermal properties of the Mn<sup>2+</sup>/Nd<sup>3+</sup>-codoped glasses were largely impacted by Nd<sub>2</sub>O<sub>3</sub> contents. The optical absorption spectra supported the occurrence of Mn<sup>2+</sup> ions and the lack of Mn<sup>3+</sup> in the codoped glasses, while the absorption due to Nd<sup>3+</sup> ions increased steadily with Nd<sub>2</sub>O<sub>3</sub> contents. Analyzing the glass absorption edges via Tauc and Urbach plots was further pursued for a comparison. The photoluminescence evaluation showed a consistent suppression of the emission from Mn<sup>2+</sup> ions with increasing Nd<sup>3+</sup> concentration, while the decay kinetics revealed shorter lifetimes in connection with increased Mn<sup>2+</sup> → Nd<sup>3+</sup> transfer efficiencies. Excitation of Mn<sup>2+</sup> at 410 nm, however, led to the Nd<sup>3+</sup> NIR emission being most intense for 1.0 mol % Nd<sub>2</sub>O<sub>3</sub>, despite the <sup>4</sup>F<sub>3/2</sub> emission decay analysis showing lifetime shortening throughout. Considering the compromise between red and NIR emissions, the Mn-containing glass doped with 0.5 mol % Nd<sub>2</sub>O<sub>3</sub> is put in perspective with the concept of solar spectral conversion.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"122 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140801901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rotational Symmetry Effects on Multibody Lateral Interactions between Co-Adsorbates at Heterogeneous Interfaces 旋转对称性对异质界面共吸附剂之间多体侧向相互作用的影响
ACS Physical Chemistry Au Pub Date : 2024-04-26 DOI: 10.1021/acsphyschemau.4c00019
Shuqiao Wang, Alyssa J.R. Hensley
{"title":"Rotational Symmetry Effects on Multibody Lateral Interactions between Co-Adsorbates at Heterogeneous Interfaces","authors":"Shuqiao Wang, Alyssa J.R. Hensley","doi":"10.1021/acsphyschemau.4c00019","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00019","url":null,"abstract":"Heterogeneous interfaces are critical in a wide range of applications, and their material properties can be tuned via changes in the coverage and configuration of chemical adsorbates. However, the tunability of such adlayers is limited by a lack of knowledge surrounding the impact of adsorbate internal structure and rotational symmetry on lateral interactions between coadsorbates. Using density functional theory (DFT) and cluster expansions, we systematically determine the impacts of rotational symmetry on lateral interactions between coadsorbates as a function of DFT functional, adsorbate type, metal type, and cluster configuration. Results indicate that the rotational symmetry effects can be nearly exclusively partitioned into the shortest 2-body clusters. By electronic analysis, the nature and strength of such effects on the lateral interactions are attributed to a balance of repulsive and attractive electrostatic interactions that are dependent on the adsorbate and metal types. Taken together, our characterization of the impacts of adsorbate internal structure and rotational symmetry on lateral interactions enables improved accuracy within multiscale modeling of multibody adsorbates at heterogeneous interfaces.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"41 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140801785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Physical, Thermal, and Optical Properties of Mn2+ and Nd3+ Containing Barium Phosphate Glasses 含 Mn2+ 和 Nd3+ 磷酸钡玻璃的物理、热和光学特性
IF 3.7
ACS Physical Chemistry Au Pub Date : 2024-04-26 DOI: 10.1021/acsphyschemau.4c0002010.1021/acsphyschemau.4c00020
José A. Jiménez*, 
{"title":"Physical, Thermal, and Optical Properties of Mn2+ and Nd3+ Containing Barium Phosphate Glasses","authors":"José A. Jiménez*,&nbsp;","doi":"10.1021/acsphyschemau.4c0002010.1021/acsphyschemau.4c00020","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00020https://doi.org/10.1021/acsphyschemau.4c00020","url":null,"abstract":"<p >This work reports on various properties and analysis of optical interactions in phosphate glasses containing red-emitting Mn<sup>2+</sup> and near-infrared (NIR)-emitting Nd<sup>3+</sup> ions, which are of interest for energy applications and solar spectral converters. The glasses were made by melting with 50P<sub>2</sub>O<sub>5</sub>–(48 – <i>x</i>)BaO–2MnO–<i>x</i>Nd<sub>2</sub>O<sub>3</sub> (<i>x</i> = 0, 0.5, 1.0, and 2.0 mol %) nominal compositions and characterized by X-ray diffraction, density and related physical properties, differential scanning calorimetry, dilatometry, UV–vis–NIR optical absorption, and photoluminescence spectroscopy with decay kinetics analysis. The glasses were X-ray amorphous, wherein the physical and thermal properties of the Mn<sup>2+</sup>/Nd<sup>3+</sup>-codoped glasses were largely impacted by Nd<sub>2</sub>O<sub>3</sub> contents. The optical absorption spectra supported the occurrence of Mn<sup>2+</sup> ions and the lack of Mn<sup>3+</sup> in the codoped glasses, while the absorption due to Nd<sup>3+</sup> ions increased steadily with Nd<sub>2</sub>O<sub>3</sub> contents. Analyzing the glass absorption edges via Tauc and Urbach plots was further pursued for a comparison. The photoluminescence evaluation showed a consistent suppression of the emission from Mn<sup>2+</sup> ions with increasing Nd<sup>3+</sup> concentration, while the decay kinetics revealed shorter lifetimes in connection with increased Mn<sup>2+</sup> → Nd<sup>3+</sup> transfer efficiencies. Excitation of Mn<sup>2+</sup> at 410 nm, however, led to the Nd<sup>3+</sup> NIR emission being most intense for 1.0 mol % Nd<sub>2</sub>O<sub>3</sub>, despite the <sup>4</sup>F<sub>3/2</sub> emission decay analysis showing lifetime shortening throughout. Considering the compromise between red and NIR emissions, the Mn-containing glass doped with 0.5 mol % Nd<sub>2</sub>O<sub>3</sub> is put in perspective with the concept of solar spectral conversion.</p>","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"4 4","pages":"363–374 363–374"},"PeriodicalIF":3.7,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00020","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141955356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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