Chemistry of Materials最新文献_第10页

Cation-Driven Vibrational Hierarchy in NaCdX (X = As, Sb) Thermoelectrics: From Static Insulation to Rattling-Like Dissipation

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-02-28 DOI: 10.1021/acs.chemmater.4c03102

Pengfei Zhang, Shuwei Tang, Da Wan, Xiaodong Li, Peng Ai, Wanrong Guo, Tengyue Yan, Yunzhuo Zhang, Qingshun Li, Shulin Bai

{"title":"Cation-Driven Vibrational Hierarchy in NaCdX (X = As, Sb) Thermoelectrics: From Static Insulation to Rattling-Like Dissipation","authors":"Pengfei Zhang, Shuwei Tang, Da Wan, Xiaodong Li, Peng Ai, Wanrong Guo, Tengyue Yan, Yunzhuo Zhang, Qingshun Li, Shulin Bai","doi":"10.1021/acs.chemmater.4c03102","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03102","url":null,"abstract":"In the current work, the crystal structure, phonon, electronic transport, and thermoelectric (TE) properties of NaCdX (X = As, Sb) compounds are systematically investigated through first-principles calculations, Boltzmann transport theory, and a two-channel model. The Na+ ion in NaCdX (X = As, Sb) compounds vibrates along different directions due to the different X (X = As, Sb) lone-pair electrons. Consequently, a pronounced anisotropy is discovered for the lattice thermal conductivity. The synergistic effect of the lone-pair electrons of X (X = As, Sb) atoms and the “static insulation to rattling-like dissipation” properties of the Na+ ion contribute to the low lattice thermal conductivities (0.52 and 0.55 W m–1K–1 @ 600 K) of NaCdX (X = As, Sb) compounds. Additionally, the TE performance of the NaCdX (X = As, Sb) compounds is evaluated by considering the multicarrier scatterings. The p-type NaCdAs compound exhibits an optimal figure of merit (ZT) of 1.2, while the n-type NaCdSb compound demonstrates a high ZT of 2.1 at 600 K. The present work not only offers a fundamental insight of the transition from the “static insulation” to “rattling-like dissipation” in suppressing lattice thermal conductivity, but also reveals the excellent TE properties of n-type NaCdSb compound.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"11 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518418","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

Synthesis, Stability, and Magnetic Properties of Antiperovskite Co3PdN

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-02-28 DOI: 10.1021/acs.chemmater.4c0314710.1021/acs.chemmater.4c03147

Sita Dugu*, Sharad Mahatara, Corlyn E. Regier, Ian A. Leahy, Andriy Zakutayev, James R. Neilson, Stephan Lany and Sage R. Bauers*,

{"title":"Synthesis, Stability, and Magnetic Properties of Antiperovskite Co3PdN","authors":"Sita Dugu*, Sharad Mahatara, Corlyn E. Regier, Ian A. Leahy, Andriy Zakutayev, James R. Neilson, Stephan Lany and Sage R. Bauers*, ","doi":"10.1021/acs.chemmater.4c0314710.1021/acs.chemmater.4c03147","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03147https://doi.org/10.1021/acs.chemmater.4c03147","url":null,"abstract":"Experimental synthesis and characterization of theoretically predicted compounds are important steps in the materials discovery pipeline. Here, we report on the synthesis of Co3PdN, which was recently predicted to be a stable magnetic antiperovskite. The Co3PdN thin films were grown by reactive sputtering and were confirmed to form in an antiperovskite crystal structure. The thermal stability of the compound is demonstrated up to 600 K by in situ X-ray diffraction, though the phase persists at slightly higher temperatures (700 K) in an air-free magnetometer. Both ab initio calculations and magnetization measurements find Co3PdN to be ferromagnetic with an experimentally determined Curie temperature of TC = 560 ± 5 K. The saturation magnetization of 1.2 μB/Co found in the experiment is slightly lower than the 1.7 μB/Co value expected by theory. A narrow magnetic hysteresis loop with a coercive field of 100 Oe at low temperature suggests that Co3PdN might be useful in electronic applications requiring fast switching of the magnetization vector. While prior prediction of Co3PdN showed a gapped electronic band structure for each spin channel, we show that this was due to incomplete sampling of Brillouin zone paths and that band crossings exist along R-X|M and X|M-R paths. The metallic nature of Co3PdN is further confirmed by temperature-dependent transport measurements, which also show a considerable anomalous Hall effect. Altogether, this work represents an appreciable step toward understanding the synthesis, structure, stability, and properties of a new magnetic material.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 5","pages":"1906–1913 1906–1913"},"PeriodicalIF":7.2,"publicationDate":"2025-02-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03147","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143591013","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhancing Performance of Cross-Linking Negative-Tone Chemically Amplified Photoresists by Controlling Interfacial Interactions via Molecular Hydrophilicity Adjustment

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-02-27 DOI: 10.1021/acs.chemmater.4c03166

Siliang Zhang, Xuewen Cui, Xue Cong, Yurui Wu, Xudong Guo, Rui Hu, Shuangqing Wang, Jinping Chen, Yi Li, Guoqiang Yang

{"title":"Enhancing Performance of Cross-Linking Negative-Tone Chemically Amplified Photoresists by Controlling Interfacial Interactions via Molecular Hydrophilicity Adjustment","authors":"Siliang Zhang, Xuewen Cui, Xue Cong, Yurui Wu, Xudong Guo, Rui Hu, Shuangqing Wang, Jinping Chen, Yi Li, Guoqiang Yang","doi":"10.1021/acs.chemmater.4c03166","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03166","url":null,"abstract":"Polyphenolic compounds, when cross-linking with polymethoxylated compounds under acidic conditions, exhibit altered solubility, enabling their application as matrix materials in chemically amplified photoresists. Herein, BPA-6-OH, a polyphenolic compound used in negative-tone lithography, is modified with hydrophobic tert-butyldimethylsilyl (TBDMS) groups to form 4-OH-TBDMS. The TBDMS modification enhances the hydrophobicity and thus adhesion of the resist to silicon wafers, increasing resistance to capillary forces during development. The adhesion work between the 4-OH-TBDMS resist and hydrophobically treated silicon wafers is 58.7 mN/m, surpassing that of the BPA-6-OH resist. Fewer residual hydroxyl groups in the exposed area of 4-OH-TBDMS resist, as confirmed by infrared (IR) spectroscopy, reduce its hydrophilicity, resulting in a greater solubility contrast between exposed and unexposed areas in the developer. Consequently, the 4-OH-TBDMS resist achieves higher resolution than BPA-6-OH, producing dense lines with a line width of 20.8 nm and a line edge roughness (LER) of 3.6 nm at 80 μC/cm2, and semidense lines with a line width of 19.3 nm and an LER of 3.6 nm at 75 μC/cm2 using electron beam lithography. This study introduces strategies for designing cross-linking chemically amplified photoresists and advances the development of materials for advanced lithography.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"51 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506945","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

Constructing Three-Dimensional Covalent Organic Framework with aea Topology and Flattened Spherical Cages

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-02-27 DOI: 10.1021/acs.chemmater.4c03256

Zonglong Li, Jia Chen, Guojie Xu, Zhuozhuo Tang, Xiaotao Liang, Guo Tian, Feng Lu, Yaxiong Yu, Yanliang Wen, Jiangong Yang, Mingpei Wang, Yen Wei, Yang Yang, Fei Wei, Chenxi Zhang

{"title":"Constructing Three-Dimensional Covalent Organic Framework with aea Topology and Flattened Spherical Cages","authors":"Zonglong Li, Jia Chen, Guojie Xu, Zhuozhuo Tang, Xiaotao Liang, Guo Tian, Feng Lu, Yaxiong Yu, Yanliang Wen, Jiangong Yang, Mingpei Wang, Yen Wei, Yang Yang, Fei Wei, Chenxi Zhang","doi":"10.1021/acs.chemmater.4c03256","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03256","url":null,"abstract":"Constructing three-dimensional (3D) covalent organic frameworks (COFs) with novel topologies is one of the most effective strategies to enhance the diversity and complexity of crystalline organic porous materials. Herein, we have designed and synthesized a 3D COF (3D-OLC-aea-COF, OLC = Ordos Laboratory China) with an unprecedented aea topology, condensed from the 12-connected building units (triptycene-12-aldehyde) and the planar 3-connected building units. Structural simulations and high-resolution transmission electron microscopy successfully determined the crystal structure. Interestingly, the unique connection between two precursors creates novel cages with large cavities and small windows within the framework, which will likely bring valuable implications for guest molecular storage and nanoreactors. Notably, huge intrinsic free volume (IFV) of triptycene and the periodic arrangement of cages endowed 3D-OLC-aea-COF with excellent CO2 capture capability. This work not only enhances the topological diversity and structural complexity of 3D COFs based on high-connectivity building units (≥8) but also provides inspiration for designing targeted materials through structure–activity relationships.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"28 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518422","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

Constructing Three-Dimensional Covalent Organic Framework with aea Topology and Flattened Spherical Cages

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-02-27 DOI: 10.1021/acs.chemmater.4c0325610.1021/acs.chemmater.4c03256

Zonglong Li, Jia Chen, Guojie Xu, Zhuozhuo Tang, Xiaotao Liang, Guo Tian, Feng Lu, Yaxiong Yu, Yanliang Wen, Jiangong Yang, Mingpei Wang, Yen Wei, Yang Yang*, Fei Wei* and Chenxi Zhang*,

{"title":"Constructing Three-Dimensional Covalent Organic Framework with aea Topology and Flattened Spherical Cages","authors":"Zonglong Li, Jia Chen, Guojie Xu, Zhuozhuo Tang, Xiaotao Liang, Guo Tian, Feng Lu, Yaxiong Yu, Yanliang Wen, Jiangong Yang, Mingpei Wang, Yen Wei, Yang Yang*, Fei Wei* and Chenxi Zhang*, ","doi":"10.1021/acs.chemmater.4c0325610.1021/acs.chemmater.4c03256","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03256https://doi.org/10.1021/acs.chemmater.4c03256","url":null,"abstract":"Constructing three-dimensional (3D) covalent organic frameworks (COFs) with novel topologies is one of the most effective strategies to enhance the diversity and complexity of crystalline organic porous materials. Herein, we have designed and synthesized a 3D COF (3D-OLC-aea-COF, OLC = Ordos Laboratory China) with an unprecedented aea topology, condensed from the 12-connected building units (triptycene-12-aldehyde) and the planar 3-connected building units. Structural simulations and high-resolution transmission electron microscopy successfully determined the crystal structure. Interestingly, the unique connection between two precursors creates novel cages with large cavities and small windows within the framework, which will likely bring valuable implications for guest molecular storage and nanoreactors. Notably, huge intrinsic free volume (IFV) of triptycene and the periodic arrangement of cages endowed 3D-OLC-aea-COF with excellent CO2 capture capability. This work not only enhances the topological diversity and structural complexity of 3D COFs based on high-connectivity building units (≥8) but also provides inspiration for designing targeted materials through structure–activity relationships.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 5","pages":"1942–1948 1942–1948"},"PeriodicalIF":7.2,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590404","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

Enhancing Performance of Cross-Linking Negative-Tone Chemically Amplified Photoresists by Controlling Interfacial Interactions via Molecular Hydrophilicity Adjustment

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-02-27 DOI: 10.1021/acs.chemmater.4c0316610.1021/acs.chemmater.4c03166

Siliang Zhang, Xuewen Cui, Xue Cong, Yurui Wu, Xudong Guo*, Rui Hu, Shuangqing Wang*, Jinping Chen, Yi Li and Guoqiang Yang*,

{"title":"Enhancing Performance of Cross-Linking Negative-Tone Chemically Amplified Photoresists by Controlling Interfacial Interactions via Molecular Hydrophilicity Adjustment","authors":"Siliang Zhang, Xuewen Cui, Xue Cong, Yurui Wu, Xudong Guo*, Rui Hu, Shuangqing Wang*, Jinping Chen, Yi Li and Guoqiang Yang*, ","doi":"10.1021/acs.chemmater.4c0316610.1021/acs.chemmater.4c03166","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03166https://doi.org/10.1021/acs.chemmater.4c03166","url":null,"abstract":"Polyphenolic compounds, when cross-linking with polymethoxylated compounds under acidic conditions, exhibit altered solubility, enabling their application as matrix materials in chemically amplified photoresists. Herein, BPA-6-OH, a polyphenolic compound used in negative-tone lithography, is modified with hydrophobic tert-butyldimethylsilyl (TBDMS) groups to form 4-OH-TBDMS. The TBDMS modification enhances the hydrophobicity and thus adhesion of the resist to silicon wafers, increasing resistance to capillary forces during development. The adhesion work between the 4-OH-TBDMS resist and hydrophobically treated silicon wafers is 58.7 mN/m, surpassing that of the BPA-6-OH resist. Fewer residual hydroxyl groups in the exposed area of 4-OH-TBDMS resist, as confirmed by infrared (IR) spectroscopy, reduce its hydrophilicity, resulting in a greater solubility contrast between exposed and unexposed areas in the developer. Consequently, the 4-OH-TBDMS resist achieves higher resolution than BPA-6-OH, producing dense lines with a line width of 20.8 nm and a line edge roughness (LER) of 3.6 nm at 80 μC/cm2, and semidense lines with a line width of 19.3 nm and an LER of 3.6 nm at 75 μC/cm2 using electron beam lithography. This study introduces strategies for designing cross-linking chemically amplified photoresists and advances the development of materials for advanced lithography.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 5","pages":"1914–1922 1914–1922"},"PeriodicalIF":7.2,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590521","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

Configuration Engineering of Plasmonic-Metal/Semiconductor Nanohybrids for Solar Fuel Production†

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-02-26 DOI: 10.1021/acs.chemmater.4c0317010.1021/acs.chemmater.4c03170

Tianyi Yang, Binbin Lu, Yong Zuo and Jianfeng Huang*,

{"title":"Configuration Engineering of Plasmonic-Metal/Semiconductor Nanohybrids for Solar Fuel Production†","authors":"Tianyi Yang, Binbin Lu, Yong Zuo and Jianfeng Huang*, ","doi":"10.1021/acs.chemmater.4c0317010.1021/acs.chemmater.4c03170","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03170https://doi.org/10.1021/acs.chemmater.4c03170","url":null,"abstract":"Solar fuel production, which primarily focuses on harnessing solar energy to convert CO2 into fuels or produce H2 through water splitting, holds transformative potential for addressing global energy demands and environmental challenges. However, several obstacles still need to be overcome, particularly concerning the efficiency and scalability of solar fuel systems. Plasmonic-metal/semiconductor nanohybrids (PSNs) represent a cutting-edge class of photocatalysts designed to overcome current efficiency bottlenecks by merging the unique localized surface plasmon resonance (LSPR) properties of plasmonic metals with the catalytic efficiency of semiconductors, thereby enhancing the overall efficiency of light-driven solar-to-fuel conversion. Precise regulation of PSN structures is essential for guiding the extraction and flow of energy and charge carriers within the nanohybrids, which ultimately determines their photocatalytic performance. In this perspective, we aim to highlight the direct impact that the configuration of these nanohybrids has on the efficiency of solar fuel production through various triggered plasmonic energy transfer mechanisms. To this end, we begin with a brief introduction to the basic plasmonic effects and fundamental energy transfer mechanisms between plasmonic metals and semiconductors. We then provide representative examples of how PSNs with five categories of engineered configurations (namely, core–shell, yolk–shell, Janus/heterodimer/dumbbell, core–satellite, and other hierarchical structures) enhance solar fuel production through three primary mechanisms: plasmon-induced resonance energy transfer, light absorption/trapping, and hot electron injection. We conclude this Perspective by outlining the remaining challenges and research directions in this field.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 5","pages":"1685–1715 1685–1715"},"PeriodicalIF":7.2,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590593","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

Guidelines for the Selection of Scintillators for Indirect Photon-Counting X-ray Detectors

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-02-26 DOI: 10.1021/acs.chemmater.4c0343710.1021/acs.chemmater.4c03437

J. Jasper van Blaaderen*, Casper van Aarle, David Leibold, Pieter Dorenbos and Dennis R. Schaart*,

{"title":"Guidelines for the Selection of Scintillators for Indirect Photon-Counting X-ray Detectors","authors":"J. Jasper van Blaaderen*, Casper van Aarle, David Leibold, Pieter Dorenbos and Dennis R. Schaart*, ","doi":"10.1021/acs.chemmater.4c0343710.1021/acs.chemmater.4c03437","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03437https://doi.org/10.1021/acs.chemmater.4c03437","url":null,"abstract":"X-ray photon-counting detectors (PCDs) are a rapidly developing technology. Current PCDs used in medical imaging are based on CdTe, CZT, or Si semiconductor detectors, which directly convert X-ray photons into electrical pulses. An alternative approach is to combine ultrafast scintillators with silicon photomultipliers (SiPMs). Here, an overview is presented of different classes of scintillators, with the aim of assessing their potential application in scintillator-SiPM based indirect X-ray PCDs. To this end, three figures of merit (FOMs) are defined: the pulse intensity, the pulse duration, and the pulse quality. These FOMs quantify how characteristics such as light yield, pulse shape, and energy resolution affect the suitability of scintillators for application in indirect PCDs. These FOMs are based on emissive characteristics; a fourth FOM (ρZeff3.5) is used to also take stopping power into account. Other important properties for the selection process include low self-absorption, low after-glow, possibility to produce sub-mm pitch pixel arrays, and cost-effectiveness. It is shown that material classes with promising emission properties are Ce3+- or Pr3+-doped materials, near band gap exciton emitters, plastics, and core–valence materials. Possible shortcomings of each of these groups, e.g., suboptimal emission wavelength, nonproportionality, and density, are discussed. Additionally, the engineering approach of quenching the scintillator emission, resulting in a targeted shortening of the decay time, and the possibility of codoping are explored. When selecting and/or engineering a material, it is important to consider not only the characteristics of the scintillator but also relevant SiPM properties, such as recharge time and photodetection efficiency.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 5","pages":"1716–1740 1716–1740"},"PeriodicalIF":7.2,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03437","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Guidelines for the Selection of Scintillators for Indirect Photon-Counting X-ray Detectors 间接光子计数 X 射线探测器闪烁体选择指南

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-02-26 DOI: 10.1021/acs.chemmater.4c03437

J. Jasper van Blaaderen, Casper van Aarle, David Leibold, Pieter Dorenbos, Dennis R. Schaart

{"title":"Guidelines for the Selection of Scintillators for Indirect Photon-Counting X-ray Detectors","authors":"J. Jasper van Blaaderen, Casper van Aarle, David Leibold, Pieter Dorenbos, Dennis R. Schaart","doi":"10.1021/acs.chemmater.4c03437","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03437","url":null,"abstract":"X-ray photon-counting detectors (PCDs) are a rapidly developing technology. Current PCDs used in medical imaging are based on CdTe, CZT, or Si semiconductor detectors, which directly convert X-ray photons into electrical pulses. An alternative approach is to combine ultrafast scintillators with silicon photomultipliers (SiPMs). Here, an overview is presented of different classes of scintillators, with the aim of assessing their potential application in scintillator-SiPM based indirect X-ray PCDs. To this end, three figures of merit (FOMs) are defined: the pulse intensity, the pulse duration, and the pulse quality. These FOMs quantify how characteristics such as light yield, pulse shape, and energy resolution affect the suitability of scintillators for application in indirect PCDs. These FOMs are based on emissive characteristics; a fourth FOM (ρZeff3.5) is used to also take stopping power into account. Other important properties for the selection process include low self-absorption, low after-glow, possibility to produce sub-mm pitch pixel arrays, and cost-effectiveness. It is shown that material classes with promising emission properties are Ce3+- or Pr3+-doped materials, near band gap exciton emitters, plastics, and core–valence materials. Possible shortcomings of each of these groups, e.g., suboptimal emission wavelength, nonproportionality, and density, are discussed. Additionally, the engineering approach of quenching the scintillator emission, resulting in a targeted shortening of the decay time, and the possibility of codoping are explored. When selecting and/or engineering a material, it is important to consider not only the characteristics of the scintillator but also relevant SiPM properties, such as recharge time and photodetection efficiency.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"210 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495738","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

Configuration Engineering of Plasmonic-Metal/Semiconductor Nanohybrids for Solar Fuel Production†

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-02-26 DOI: 10.1021/acs.chemmater.4c03170

Tianyi Yang, Binbin Lu, Yong Zuo, Jianfeng Huang

{"title":"Configuration Engineering of Plasmonic-Metal/Semiconductor Nanohybrids for Solar Fuel Production†","authors":"Tianyi Yang, Binbin Lu, Yong Zuo, Jianfeng Huang","doi":"10.1021/acs.chemmater.4c03170","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03170","url":null,"abstract":"Solar fuel production, which primarily focuses on harnessing solar energy to convert CO2 into fuels or produce H2 through water splitting, holds transformative potential for addressing global energy demands and environmental challenges. However, several obstacles still need to be overcome, particularly concerning the efficiency and scalability of solar fuel systems. Plasmonic-metal/semiconductor nanohybrids (PSNs) represent a cutting-edge class of photocatalysts designed to overcome current efficiency bottlenecks by merging the unique localized surface plasmon resonance (LSPR) properties of plasmonic metals with the catalytic efficiency of semiconductors, thereby enhancing the overall efficiency of light-driven solar-to-fuel conversion. Precise regulation of PSN structures is essential for guiding the extraction and flow of energy and charge carriers within the nanohybrids, which ultimately determines their photocatalytic performance. In this perspective, we aim to highlight the direct impact that the configuration of these nanohybrids has on the efficiency of solar fuel production through various triggered plasmonic energy transfer mechanisms. To this end, we begin with a brief introduction to the basic plasmonic effects and fundamental energy transfer mechanisms between plasmonic metals and semiconductors. We then provide representative examples of how PSNs with five categories of engineered configurations (namely, core–shell, yolk–shell, Janus/heterodimer/dumbbell, core–satellite, and other hierarchical structures) enhance solar fuel production through three primary mechanisms: plasmon-induced resonance energy transfer, light absorption/trapping, and hot electron injection. We conclude this Perspective by outlining the remaining challenges and research directions in this field.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"6 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495902","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