Journal of Materiomics最新文献_第6页

Design rules for improving dielectric constants of hafnium-based oxides 提高铪基氧化物介电常数的设计规则

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-11-26 DOI: 10.1016/j.jmat.2025.101148

Qi-Wen He , Jia-Le Jian , Yongchang Li , Dongdong Li , Shanting Zhang , Shuai Kong , Ni Zhong , Chun-Gang Duan , Wen-Yi Tong

As promising dielectric alternatives to SiO₂, hafnium-based oxides show broad application prospects in integrated circuits, dielectric sensors, and optoelectronics. Nevertheless, stabilizing the T-phase with a high dielectric constant (high-κ) and further improving its κ value remain key challenges for practical applications. Using first-principles calculations, we reveal the dielectric enhancement mechanism in the T-phase HfO₂ by demonstrating that the high-κ primarily originates from the softening of phonon vibration frequencies, which can be effectively tuned by bond length and atomic mass. Furthermore, we find that doping atoms with lower electronegativity form stronger ionic interactions with O atoms, favoring the stabilization of the high-coordination T-phase. Based on these analyses, we propose a general design rule: doping atoms with remarkable size, heavy mass, and small electronegativity could effectively improve high-κ and stabilize the T-phase simultaneously. Guided by this rule, a more promising Ce-doping strategy in HfO₂ than Zr-doping is proposed, which is also supported by some experimental results. This work not only delves into the physical mechanism of the high-κ in hafnium-based oxides, but also provides practical methods to enhance their dielectric constants.

作为二氧化硅的极具潜力的介质替代品，铪基氧化物在集成电路、介电传感器、光电等领域具有广阔的应用前景。然而，用高介电常数（高κ）稳定t相并进一步提高其κ值仍然是实际应用的关键挑战。利用第一性原理计算，我们揭示了t相HfO2的介电增强机制，证明了高κ主要来自声子振动频率的软化，这可以通过键长和原子质量有效地调节。此外，我们发现具有较低电负性的掺杂原子与O原子形成更强的离子相互作用，有利于高配位t相的稳定。基于这些分析，我们提出了一个通用的设计规则：掺杂尺寸大、质量大、电负性小的原子可以有效地提高高κ，同时稳定t相。在此规律的指导下，提出了在HfO2中掺杂ce比掺杂zr更有前途的策略，并得到了一些实验结果的支持。这项工作不仅深入研究了高κ in铪基氧化物的物理机制，而且为提高其介电常数提供了实用的方法。

{"title":"Design rules for improving dielectric constants of hafnium-based oxides","authors":"Qi-Wen He , Jia-Le Jian , Yongchang Li , Dongdong Li , Shanting Zhang , Shuai Kong , Ni Zhong , Chun-Gang Duan , Wen-Yi Tong","doi":"10.1016/j.jmat.2025.101148","DOIUrl":"10.1016/j.jmat.2025.101148","url":null,"abstract":"<div><div>As promising dielectric alternatives to SiO2, hafnium-based oxides show broad application prospects in integrated circuits, dielectric sensors, and optoelectronics. Nevertheless, stabilizing the T-phase with a high dielectric constant (high-κ) and further improving its κ value remain key challenges for practical applications. Using first-principles calculations, we reveal the dielectric enhancement mechanism in the T-phase HfO2 by demonstrating that the high-κ primarily originates from the softening of phonon vibration frequencies, which can be effectively tuned by bond length and atomic mass. Furthermore, we find that doping atoms with lower electronegativity form stronger ionic interactions with O atoms, favoring the stabilization of the high-coordination T-phase. Based on these analyses, we propose a general design rule: doping atoms with remarkable size, heavy mass, and small electronegativity could effectively improve high-κ and stabilize the T-phase simultaneously. Guided by this rule, a more promising Ce-doping strategy in HfO2 than Zr-doping is proposed, which is also supported by some experimental results. This work not only delves into the physical mechanism of the high-κ in hafnium-based oxides, but also provides practical methods to enhance their dielectric constants.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101148"},"PeriodicalIF":9.6,"publicationDate":"2025-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145600094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Strain-engineered flexoelectricity and oxygen vacancy dynamics for modulating interfacial charge transport in BaTiO3 应变工程柔性电和氧空位动力学对BaTiO3中界面电荷输运的调节

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-11-06 DOI: 10.1016/j.jmat.2025.101145

Guoyang Shen, Zhibin Wen, Zhiguo Wang, Longlong Shu

Strain engineering has emerged as a powerful strategy for tailoring the ferroelectric properties and interfacial charge transport behaviors in complex oxide heterostructures. However, the underlying coupling mechanisms between strain-induced polarization reversal and defect-mediated barrier modulation remain in-depth understanding. In this study, controllable strain gradients are introduced through the use of intermediate layers to simultaneously manipulate the polarization orientation of BaTiO₃ thin films and modulate interfacial barrier properties. We systematically investigate the interplay among strain states, polarization behavior, and oxygen vacancy dynamics. Opposing strain states induce distinct polarization orientations in BaTiO₃, as confirmed by phase reversal and local hysteresis loops. Vacuum annealing is employed to tune the overall oxygen vacancy concentration, while flexoelectric field induced by strain gradient governs the migration and spatial distribution of vacancies. Compressive and tensile strains respectively drive oxygen vacancy accumulation near the surface or at the bottom interface, thereby modulating the Schottky barrier height and associated rectifying behavior. These results reveal a synergistic mechanism whereby flexoelectric polarization and strain-driven redistribution of oxygen vacancy cooperatively regulate charge transport in ferroelectric heterostructures.

应变工程已成为调整复杂氧化物异质结构中铁电性质和界面电荷输运行为的有力策略。然而，应变诱导的极化逆转和缺陷介导的势垒调制之间的耦合机制仍有待深入研究。在本研究中，通过使用中间层引入可控应变梯度，同时操纵BaTiO3薄膜的极化取向和调节界面势垒性质。我们系统地研究了应变状态、极化行为和氧空位动力学之间的相互作用。相反的应变状态在BaTiO3中诱导出明显的极化取向，这一点由相反转和局部磁滞回线证实。真空退火可调节整体氧空位浓度，应变梯度诱导的柔性电场控制空位的迁移和空间分布。压缩应变和拉伸应变分别驱动表面或底部界面附近的氧空位积累，从而调节肖特基势垒高度和相关的整流行为。这些结果揭示了一种协同机制，即挠曲电极化和应变驱动的氧空位重分配协同调节铁电异质结构中的电荷输运。

{"title":"Strain-engineered flexoelectricity and oxygen vacancy dynamics for modulating interfacial charge transport in BaTiO3","authors":"Guoyang Shen, Zhibin Wen, Zhiguo Wang, Longlong Shu","doi":"10.1016/j.jmat.2025.101145","DOIUrl":"10.1016/j.jmat.2025.101145","url":null,"abstract":"<div><div>Strain engineering has emerged as a powerful strategy for tailoring the ferroelectric properties and interfacial charge transport behaviors in complex oxide heterostructures. However, the underlying coupling mechanisms between strain-induced polarization reversal and defect-mediated barrier modulation remain in-depth understanding. In this study, controllable strain gradients are introduced through the use of intermediate layers to simultaneously manipulate the polarization orientation of BaTiO3 thin films and modulate interfacial barrier properties. We systematically investigate the interplay among strain states, polarization behavior, and oxygen vacancy dynamics. Opposing strain states induce distinct polarization orientations in BaTiO3, as confirmed by phase reversal and local hysteresis loops. Vacuum annealing is employed to tune the overall oxygen vacancy concentration, while flexoelectric field induced by strain gradient governs the migration and spatial distribution of vacancies. Compressive and tensile strains respectively drive oxygen vacancy accumulation near the surface or at the bottom interface, thereby modulating the Schottky barrier height and associated rectifying behavior. These results reveal a synergistic mechanism whereby flexoelectric polarization and strain-driven redistribution of oxygen vacancy cooperatively regulate charge transport in ferroelectric heterostructures.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101145"},"PeriodicalIF":9.6,"publicationDate":"2025-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145455557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Highly oxygen/nitrogen doped enclosed carbon nanotubes as anode materials for advanced Li+/Na+/K+ hybrid ion batteries 高氧/氮掺杂封闭碳纳米管作为先进Li+/Na+/K+混合离子电池的负极材料

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-11-06 DOI: 10.1016/j.jmat.2025.101143

Shaoyang Dai , Xibing Wu , Dianhui Wang, Qianhui Fu, Peng Liu, Feng Wang, Daosheng Liu, Wenping Liu, Jianqiu Deng

The utilization of hybrid ion batteries (HIBs) effectively reduces the consumption of scarce Li resources and harnesses the synergistic effect of mixed ions to achieve performance comparable to that of lithium-ion batteries. However, there is currently a lack of anode materials that possess both high safety and excellent performance for HIBs. Herein, we present a novel structure of enclosed hard carbon nanotubes (HCNTs) doped with high levels of nitrogen and oxygen as anodes for HIBs. When utilized in LiNaK HIBs, they exhibit superior reversible capacity (440.1 mA⋅h·g⁻¹ at 100 mA/g) and enhanced rate performance (327.7 mA⋅h·g⁻¹ at 1 A/g) compared to single alkali metal ion batteries. These improvements can be attributed to the design of a one-dimensional structure that features highly doped hard carbon, which significantly enhances carrier transport. Furthermore, first-principles calculations reveal the synergistic effect of hybrid ions in nitrogen-doped hard carbon nanotubes, enhancing the ion adsorption stability in the carbon layer. This study introduces a substantial anode material for HIBs and expands the scope from binary to ternary HIB systems.

混合离子电池（HIBs）的利用有效降低了稀缺锂资源的消耗，并利用混合离子的协同效应，实现了与锂离子电池相当的性能。然而，目前缺乏既具有高安全性又具有优异性能的hib负极材料。在此，我们提出了一种新型结构的封闭硬碳纳米管（HCNTs），掺杂高水平的氮和氧作为HIBs的阳极。与单一碱金属离子电池相比，在Li-Na-K HIBs中，它们具有更好的可逆容量（100 mA/g时为440.1 mA·h·g - 1）和更高的倍率性能（1 A/g时为327.7 mA·h·g - 1）。这些改进可归因于设计了具有高掺杂硬碳的一维结构，这大大增强了载流子输运。此外，第一性原理计算揭示了杂化离子在氮掺杂硬碳纳米管中的协同作用，增强了离子在碳层中的吸附稳定性。本研究为HIB系统引入了一种重要的负极材料，并将其应用范围从二元HIB系统扩展到三元HIB系统。

{"title":"Highly oxygen/nitrogen doped enclosed carbon nanotubes as anode materials for advanced Li+/Na+/K+ hybrid ion batteries","authors":"Shaoyang Dai , Xibing Wu , Dianhui Wang, Qianhui Fu, Peng Liu, Feng Wang, Daosheng Liu, Wenping Liu, Jianqiu Deng","doi":"10.1016/j.jmat.2025.101143","DOIUrl":"10.1016/j.jmat.2025.101143","url":null,"abstract":"<div><div>The utilization of hybrid ion batteries (HIBs) effectively reduces the consumption of scarce Li resources and harnesses the synergistic effect of mixed ions to achieve performance comparable to that of lithium-ion batteries. However, there is currently a lack of anode materials that possess both high safety and excellent performance for HIBs. Herein, we present a novel structure of enclosed hard carbon nanotubes (HCNTs) doped with high levels of nitrogen and oxygen as anodes for HIBs. When utilized in Li<img>Na<img>K HIBs, they exhibit superior reversible capacity (440.1 mA⋅h·g−1 at 100 mA/g) and enhanced rate performance (327.7 mA⋅h·g−1 at 1 A/g) compared to single alkali metal ion batteries. These improvements can be attributed to the design of a one-dimensional structure that features highly doped hard carbon, which significantly enhances carrier transport. Furthermore, first-principles calculations reveal the synergistic effect of hybrid ions in nitrogen-doped hard carbon nanotubes, enhancing the ion adsorption stability in the carbon layer. This study introduces a substantial anode material for HIBs and expands the scope from binary to ternary HIB systems.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101143"},"PeriodicalIF":9.6,"publicationDate":"2025-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145447565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Charge defect design within PbTe grain boundaries to influence the mechanical properties PbTe晶界内电荷缺陷设计对力学性能的影响

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-11-05 DOI: 10.1016/j.jmat.2025.101142

Xuemei Zhang , Jingyu Li , Shuping Guo , Lulu Huang , Mi Qin , Jianbo Zhu , Xiaoqiang Ma , Zhixin Hui , Yongsheng Zhang

Defect engineering is a key strategy for optimizing the thermoelectric (TE) properties of PbTe-based materials, and investigating charged defects in PbTe grain boundaries (GBs) is crucial for understanding its thermoelectric properties. In this study, focusing the PbTe(111)<11

\bar{2}

>/PbTe(111)<

\bar{1} \bar{1}

2> GBs, we perform a high-throughput investigation of the formation energies with various charged point (intrinsic and extrinsic) defects and their effects on the mechanical properties, the shear modulus. The GBs can facilitate the formation of the charged point defects (such as

V_{Pb}^{2 -}

,

S b_{Pb}^{1 +}

), indicating the accumulations of the defects within the GBs region. Such defect accumulation can strongly increase the phonon scatterings. Furthermore, charge defects within TePbTe GBs lower the shear modulus to <33.1 GPa, due to the weakening interactions between PbTe bonds. The soft bonds around GBs will induce the stronger anharmonicity and further suppress the lattice thermal conductivity. Employing the machine learning method, we establish the relationship between the shear modulus and physical descriptors, which can efficiently screen or design the various purposes of PbTe compounds. Our work bridges the gap in understanding charged defects at grain boundaries in PbTe-based thermoelectric materials and giving rise to the design methodology to achieve high promising thermoelectric performance through charged defect influenced mechanical properties.

缺陷工程是优化PbTe基材料热电性能的关键策略，研究PbTe晶界中的带电缺陷对于理解其热电性能至关重要。在这项研究中，我们以PbTe(111)<11 >/PbTe(111)< 2>； gb为重点，对具有各种电荷点（内在和外在）缺陷的地层能量及其对力学性能和剪切模量的影响进行了高通量研究。GBs可以促进带电点缺陷（如，）的形成，表明缺陷在GBs区域内的积累。这种缺陷的积累会大大增加声子散射。此外，由于Pb-Te键之间的相互作用减弱，Te-PbTe GBs内部的电荷缺陷使剪切模量降低至33.1 GPa。GBs周围的软键会引起更强的非调和性，从而进一步抑制晶格的导热性。利用机器学习方法，建立剪切模量与物理描述符之间的关系，可以有效地筛选或设计各种用途的PbTe化合物。我们的工作填补了理解pbte基热电材料晶界带电缺陷的空白，并提出了通过带电缺陷影响机械性能来实现高前景热电性能的设计方法。

{"title":"Charge defect design within PbTe grain boundaries to influence the mechanical properties","authors":"Xuemei Zhang , Jingyu Li , Shuping Guo , Lulu Huang , Mi Qin , Jianbo Zhu , Xiaoqiang Ma , Zhixin Hui , Yongsheng Zhang","doi":"10.1016/j.jmat.2025.101142","DOIUrl":"10.1016/j.jmat.2025.101142","url":null,"abstract":"<div><div>Defect engineering is a key strategy for optimizing the thermoelectric (TE) properties of PbTe-based materials, and investigating charged defects in PbTe grain boundaries (GBs) is crucial for understanding its thermoelectric properties. In this study, focusing the PbTe(111)<11 <math><mrow><mover><mn>2</mn><mo>¯</mo></mover></mrow></math> >/PbTe(111)<<math><mrow><mover><mn>1</mn><mo>¯</mo></mover><mover><mn>1</mn><mo>¯</mo></mover></mrow></math> 2> GBs, we perform a high-throughput investigation of the formation energies with various charged point (intrinsic and extrinsic) defects and their effects on the mechanical properties, the shear modulus. The GBs can facilitate the formation of the charged point defects (such as <math><mrow><msubsup><mi>V</mi><mtext>Pb</mtext><mrow><mn>2</mn><mo>−</mo></mrow></msubsup></mrow></math>, <math><mrow><mi>S</mi><msubsup><mi>b</mi><mtext>Pb</mtext><mrow><mn>1</mn><mo>+</mo></mrow></msubsup></mrow></math>), indicating the accumulations of the defects within the GBs region. Such defect accumulation can strongly increase the phonon scatterings. Furthermore, charge defects within Te<img>PbTe GBs lower the shear modulus to <33.1 GPa, due to the weakening interactions between Pb<img>Te bonds. The soft bonds around GBs will induce the stronger anharmonicity and further suppress the lattice thermal conductivity. Employing the machine learning method, we establish the relationship between the shear modulus and physical descriptors, which can efficiently screen or design the various purposes of PbTe compounds. Our work bridges the gap in understanding charged defects at grain boundaries in PbTe-based thermoelectric materials and giving rise to the design methodology to achieve high promising thermoelectric performance through charged defect influenced mechanical properties.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101142"},"PeriodicalIF":9.6,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145441956","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Polarization rotation in high-performance KNN-based piezoceramics revealed by an in situ electric field pair distribution function 用原位电场对分布函数揭示高性能knn基压电陶瓷的极化旋转

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-10-01 DOI: 10.1016/j.jmat.2025.101130

Yingying Yu , Fanyi Meng , Cheng Yang , Linda Qi , Changhao Zhao , Bo Wu , Mao-Hua Zhang

Understanding the atomic-scale structural dynamics that enable ultrahigh piezoelectric responses in lead-free piezoceramics remains a central challenge in materials science. Here, we employ in situ electric field pair distribution function (PDF) analysis to elucidate the local structural origin of a KNN-based piezoceramic with a nominal composition of 0.964K_0.5Na_0.5Nb_0.965Sb_0.035O₃–0.03(Bi_0.5Na_0.5)_0.9(Ga_0.5Li_0.5)_0.1ZrO₃–0.006BiFeO₃ that has an exceptional piezoelectricity coefficient (d₃₃ > 500 pC/N). Combined Rietveld refinement, PDF fitting, and reverse Monte Carlo simulations revealed the coexistence of long-range tetragonal and orthorhombic phases with local c-type monoclinic symmetry. In situ electric field PDF analyses indicated a reversible polarization rotation between the <001>_PC and <110>_PC directions via a monoclinic plane, with a critical switching field of approximately 0.4 kV/mm. These findings establish polarization rotation, rather than abrupt phase transitions, as the governing mechanism for the enhanced piezoresponse, providing a structural design principle for next-generation lead-free piezoelectrics.

在无铅压电陶瓷中实现超高压电响应的原子尺度结构动力学仍然是材料科学的核心挑战。本文采用原位电场对分布函数（PDF）分析阐明了一种具有优异压电系数（d33 > 500 pC/N）的knn基压电陶瓷的局部结构起源，该陶瓷的名义成分为0.964K0.5Na0.5Nb0.965Sb0.035O3-0.03 (Bi0.5Na0.5)0.9(Ga0.5Li0.5) 0.1ZrO3-0.006BiFeO3。结合Rietveld细化、PDF拟合和反向蒙特卡罗模拟，揭示了具有局部c型单斜对称的长程四方相和正交相共存。原位电场PDF分析表明，在单斜平面上，<001>；PC和<；110>；PC方向之间存在可逆的极化旋转，临界开关场约为0.4 kV/mm。这些发现确立了极化旋转，而不是突然相变，作为增强压电响应的控制机制，为下一代无铅压电材料提供了结构设计原则。

{"title":"Polarization rotation in high-performance KNN-based piezoceramics revealed by an in situ electric field pair distribution function","authors":"Yingying Yu , Fanyi Meng , Cheng Yang , Linda Qi , Changhao Zhao , Bo Wu , Mao-Hua Zhang","doi":"10.1016/j.jmat.2025.101130","DOIUrl":"10.1016/j.jmat.2025.101130","url":null,"abstract":"<div><div>Understanding the atomic-scale structural dynamics that enable ultrahigh piezoelectric responses in lead-free piezoceramics remains a central challenge in materials science. Here, we employ in situ electric field pair distribution function (PDF) analysis to elucidate the local structural origin of a KNN-based piezoceramic with a nominal composition of 0.964K0.5Na0.5Nb0.965Sb0.035O3–0.03(Bi0.5Na0.5)0.9(Ga0.5Li0.5)0.1ZrO3–0.006BiFeO3 that has an exceptional piezoelectricity coefficient (d33 > 500 pC/N). Combined Rietveld refinement, PDF fitting, and reverse Monte Carlo simulations revealed the coexistence of long-range tetragonal and orthorhombic phases with local c-type monoclinic symmetry. In situ electric field PDF analyses indicated a reversible polarization rotation between the <001>PC and <110>PC directions via a monoclinic plane, with a critical switching field of approximately 0.4 kV/mm. These findings establish polarization rotation, rather than abrupt phase transitions, as the governing mechanism for the enhanced piezoresponse, providing a structural design principle for next-generation lead-free piezoelectrics.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 1","pages":"Article 101130"},"PeriodicalIF":9.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195003","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

No-heating deposition of ferroelectric epitaxial Hf0.5Zr0.5O2 films using a sputtering method with precise RF power density and thickness control 采用精确控制射频功率密度和厚度的溅射方法无加热沉积铁电外延Hf0.5Zr0.5O2薄膜

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-09-29 DOI: 10.1016/j.jmat.2025.101129

Takanori Mimura , Yoshiko Nakamura , Yutaro Tsuchiya , Kazuki Okamoto , Hiroshi Funakubo

The no-heating deposition of (111)-oriented epitaxial (Hf_0.5Zr_0.5)O₂ films was successfully achieved on (111) indium tin oxide//(111) yttria-stabilized zirconia substrates using a radio-frequency (RF) magnetron sputtering method. As the RF power density was increased, the crystal phase changed sequentially from the tetragonal, the orthorhombic, and then to the monoclinic phase. A similar trend in the crystal phase was also observed with increasing film thickness. The (Hf_0.5Zr_0.5)O₂ film exhibited ferroelectric properties comparable to the (Y_0.07Hf_0.93)O₂ film previously produced via non-heating film deposition. Upon heat treatment at 1000 °C, the crystal phase of the film transitioned from the orthorhombic phase to the monoclinic phase, indicating that the stability of the orthorhombic phase is low compared with (Y_0.07Hf_0.93)O₂. Therefore, precise control of the RF power density and film thickness is essential for preparing ferroelectric (Hf_0.5Zr_0.5)O₂ films without heating.

采用射频磁控溅射方法，在（111）氧化铟锡//(111)钇稳定氧化锆衬底上成功地制备了（111）取向外延（Hf0.5Zr0.5）O2薄膜。随着射频功率密度的增大，晶相由四方相、正交相、单斜相依次变化。随着薄膜厚度的增加，晶相也有类似的变化趋势。（Hf0.5Zr0.5）O2薄膜的铁电性能与之前通过非加热膜沉积制备的（Y0.07Hf0.93）O2薄膜相当。经1000℃热处理后，膜的晶相由正交相转变为单斜相，表明与（Y0.07Hf0.93）O2相比，正交相的稳定性较低。因此，精确控制射频功率密度和薄膜厚度对于制备不加热的铁电（Hf0.5Zr0.5）O2薄膜至关重要。

{"title":"No-heating deposition of ferroelectric epitaxial Hf0.5Zr0.5O2 films using a sputtering method with precise RF power density and thickness control","authors":"Takanori Mimura , Yoshiko Nakamura , Yutaro Tsuchiya , Kazuki Okamoto , Hiroshi Funakubo","doi":"10.1016/j.jmat.2025.101129","DOIUrl":"10.1016/j.jmat.2025.101129","url":null,"abstract":"<div><div>The no-heating deposition of (111)-oriented epitaxial (Hf0.5Zr0.5)O2 films was successfully achieved on (111) indium tin oxide//(111) yttria-stabilized zirconia substrates using a radio-frequency (RF) magnetron sputtering method. As the RF power density was increased, the crystal phase changed sequentially from the tetragonal, the orthorhombic, and then to the monoclinic phase. A similar trend in the crystal phase was also observed with increasing film thickness. The (Hf0.5Zr0.5)O2 film exhibited ferroelectric properties comparable to the (Y0.07Hf0.93)O2 film previously produced via non-heating film deposition. Upon heat treatment at 1000 °C, the crystal phase of the film transitioned from the orthorhombic phase to the monoclinic phase, indicating that the stability of the orthorhombic phase is low compared with (Y0.07Hf0.93)O2. Therefore, precise control of the RF power density and film thickness is essential for preparing ferroelectric (Hf0.5Zr0.5)O2 films without heating.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 1","pages":"Article 101129"},"PeriodicalIF":9.6,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182941","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

DFT insights on iron-based layered perovskites as oxygen catalysts 铁基层状钙钛矿作为氧催化剂的DFT研究

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-09-26 DOI: 10.1016/j.jmat.2025.101128

M. Elena Arroyo-de Dompablo, Marianela Gomez-Toledo

Density Functional Theory (DFT)-derived electronic descriptors are key to accelerating the design of effective ORR/OER catalysts. The O 2p-band center, in particular, is a robust descriptor of catalytic activity in perovskite oxides. This study examines the O 2p-band center in Fe⁴⁺ perovskite-type layered oxides, focusing on the Ruddlesden Popper (RP) phases Sr₂FeO₄ and Sr₃Fe₂O_7, as well as the high-Tc superconductor YSr₂Cu₂FeO_8. The analysis emphasizes trends driven by compositional modifications. The O 2p-band centers of Sr_2–2xLa_2xFeO₄ and Sr_3–3xLa_3xFe₂O₇ (0 < x < 1) correlate linearly with the Fe oxidation state, and span a wide energy range (−1.2 eV to −4.7 eV with PBE+U; −1.9 eV to −4.7 eV with SCAN). Partial substitution of Fe with 3d transition metals (TM) in Sr₂Fe_7/8xM_1/8O₄ shifts the O 2p band center, with the more electronegative TMs bringing it closer to the Fermi level. RP–Sr₂FeO₄ exhibits remarkable tunability of the O 2p-band center, enabling the compositionally driven design of oxygen catalysts with potentially improved activity–stability balance. In contrast, YSr₂Cu₂FeO_7+δ (0 < δ < 1) shows no correlation between the O 2p-band center and Fe oxidation states, likely due to a change in Fe coordination from octahedral (δ = 1) to tetrahedral (δ = 0). The O 2p-center values (−0.9 eV to −1.3 eV with PBE+U; −1.5 eV to −2 eV with SCAN) suggest that YSr₂Cu₂FeO_7+δ could potentially catalyze the ORR/OER, though stability over operation time remains a challenge.

密度泛函理论（DFT）衍生的电子描述符是加速设计有效ORR/OER催化剂的关键。特别是o2p -带中心，是钙钛矿氧化物催化活性的有力描述符。本研究考察了Fe4+钙钛矿型层状氧化物中的O 2p-带中心，重点研究了Ruddlesden Popper （RP）相Sr2FeO4和Sr3Fe2O7，以及高tc超导体YSr2Cu2FeO8。分析强调由成分变化驱动的趋势。Sr2-2xLa2xFeO4和Sr3-3xLa3xFe2O7的O - 2p波段中心（0 < x < 1）与Fe氧化态呈线性相关，且能量范围较宽（PBE+U为-1.2 eV至-4.7 eV； SCAN为-1.9 eV至-4.7 eV）。在Sr2Fe7/8xM1/8O4中，三维过渡金属（TM）部分取代Fe使o2p带中心移位，电负性越强的TM使其更接近费米能级。RP-Sr2FeO4表现出明显的o2o -波段中心可调性，使氧催化剂的组成驱动设计具有潜在的改善活性-稳定性平衡。相比之下，YSr2Cu2FeO7+δ (0 < δ < 1)在O 2p-带中心和铁氧化态之间没有相关性，可能是由于铁的配位从八面体（δ = 1）转变为四面体（δ = 0）。o2o中心值（PBE+U为-0.9 ~ -1.3 eV； SCAN为-1.5 ~ -2 eV）表明，YSr2Cu2FeO7+δ可能催化ORR/OER，但稳定性仍是一个挑战。

{"title":"DFT insights on iron-based layered perovskites as oxygen catalysts","authors":"M. Elena Arroyo-de Dompablo, Marianela Gomez-Toledo","doi":"10.1016/j.jmat.2025.101128","DOIUrl":"10.1016/j.jmat.2025.101128","url":null,"abstract":"<div><div>Density Functional Theory (DFT)-derived electronic descriptors are key to accelerating the design of effective ORR/OER catalysts. The O 2p-band center, in particular, is a robust descriptor of catalytic activity in perovskite oxides. This study examines the O 2p-band center in Fe4+ perovskite-type layered oxides, focusing on the Ruddlesden Popper (RP) phases Sr2FeO4 and Sr3Fe2O7, as well as the high-Tc superconductor YSr2Cu2FeO8. The analysis emphasizes trends driven by compositional modifications. The O 2p-band centers of Sr2–2xLa2xFeO4 and Sr3–3xLa3xFe2O7 (0 < x < 1) correlate linearly with the Fe oxidation state, and span a wide energy range (−1.2 eV to −4.7 eV with PBE+U; −1.9 eV to −4.7 eV with SCAN). Partial substitution of Fe with 3d transition metals (TM) in Sr2Fe7/8xM1/8O4 shifts the O 2p band center, with the more electronegative TMs bringing it closer to the Fermi level. RP–Sr2FeO4 exhibits remarkable tunability of the O 2p-band center, enabling the compositionally driven design of oxygen catalysts with potentially improved activity–stability balance. In contrast, YSr2Cu2FeO7+δ (0 < δ < 1) shows no correlation between the O 2p-band center and Fe oxidation states, likely due to a change in Fe coordination from octahedral (δ = 1) to tetrahedral (δ = 0). The O 2p-center values (−0.9 eV to −1.3 eV with PBE+U; −1.5 eV to −2 eV with SCAN) suggest that YSr2Cu2FeO7+δ could potentially catalyze the ORR/OER, though stability over operation time remains a challenge.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101128"},"PeriodicalIF":9.6,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145141167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Multi-functional design of ultra-high temperature ceramics coatings 超高温陶瓷涂料的多功能设计

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-09-15 DOI: 10.1016/j.jmat.2025.101127

Yanfei Liu , Ruize Zhang , Shaopu Liu , Jieliang Zhao , Xiaojun Tang , Yanbo Liu

Ultra-high temperature ceramics (UHTCs) exhibit ultra-high melting points and relatively high mechanical performance, making them ideal coating materials for extreme environment applications like hypersonic vehicles. Recently, novel design strategies of UHTCs coatings have been proposed, mainly including the composition and structural design. In this article, state-of-the-art approaches including multilayer and gradient UHTC coatings for enhanced mechanical and ablation resistance, surface engineering for the improvement of coating adhesion, materials and microstructural design for thermal insulation, laser ablation protection, and drag reduction were reviewed. Furthermore, advanced designing and fabrication techniques for UHTC coatings are also prospected, which can provide insights for the development of next-generation multi-functional UHTC coatings for harsh conditions.

超高温陶瓷（UHTCs）具有超高熔点和相对较高的机械性能，使其成为高超声速飞行器等极端环境应用的理想涂层材料。近年来，人们提出了新的超高温涂层设计策略，主要包括成分设计和结构设计。本文综述了用于增强机械和抗烧蚀性能的多层和梯度UHTC涂层、用于改善涂层附着力的表面工程、用于隔热、激光烧蚀保护和减阻的材料和微结构设计等最新方法。展望了UHTC涂料的先进设计和制造技术，为开发下一代多功能恶劣条件下的UHTC涂料提供了参考。

引用次数: 0

Negative thermal expansion ScF3 ceramic for electronic packaging applications 负热膨胀ScF3陶瓷电子封装应用

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-09-09 DOI: 10.1016/j.jmat.2025.101126

Jin Cheng , Hongye Wang , Xinwei Xu , Naichao Chen , Zhan Zeng , Xiaoyu Li , Biao Guo , Binfeng Zhao , Hong Wang

To meet the demands of miniaturization and integration in modern electronic packaging, developing materials with low coefficient of thermal expansion (CTE) is essential to reduce thermal stress and enhance device reliability. In this study, the dense negative thermal expansion ceramic ScF₃ was prepared with a CTE of −8.86 × 10⁻⁶/°C. The ScF₃ ceramic was cold sintered at 150 °C, exhibiting a low permittivity of 5.3 and a high quality factor (Q×f) of 14,700 GHz. By incorporating ScF₃ to the hexagonal boron nitride (BN) ceramic, the CTE of ScF₃BN composite ceramic was adjusted to 3.36 × 10⁻⁶/°C, establishing compatibility with silicon-based chips. And finite element simulations verified that ScF₃BN composite significantly reduces thermal stress compared to Li₂MoO₄ or Al₂O₃ ceramics. Furthermore, this work demonstrates the potential of cold-sintered ScF₃ to regulate thermal expansion in packaging substrates, paving the way for improved performance in next-generation electronic devices.

为了满足现代电子封装小型化和集成化的要求，开发低热膨胀系数（CTE）材料是降低热应力和提高器件可靠性的必要条件。本研究以-8.86×10-6 /°C的CTE制备了致密负热膨胀陶瓷ScF3。ScF3陶瓷在150°C下进行冷烧结，其介电常数低至5.3，质量因子（Q×f）高达14,700 GHz。通过将ScF3掺入六方氮化硼（BN）陶瓷中，将ScF3-BN复合陶瓷的CTE调节到3.36×10-6 /°C，建立了与硅基芯片的相容性。有限元模拟验证了ScF3-BN复合材料与Li2MoO4或Al2O3陶瓷相比显著降低了热应力。此外，这项工作证明了冷烧结ScF3调节封装基板热膨胀的潜力，为提高下一代电子器件的性能铺平了道路。

{"title":"Negative thermal expansion ScF3 ceramic for electronic packaging applications","authors":"Jin Cheng , Hongye Wang , Xinwei Xu , Naichao Chen , Zhan Zeng , Xiaoyu Li , Biao Guo , Binfeng Zhao , Hong Wang","doi":"10.1016/j.jmat.2025.101126","DOIUrl":"10.1016/j.jmat.2025.101126","url":null,"abstract":"<div><div>To meet the demands of miniaturization and integration in modern electronic packaging, developing materials with low coefficient of thermal expansion (CTE) is essential to reduce thermal stress and enhance device reliability. In this study, the dense negative thermal expansion ceramic ScF3 was prepared with a CTE of −8.86 × 10−6/°C. The ScF3 ceramic was cold sintered at 150 °C, exhibiting a low permittivity of 5.3 and a high quality factor (Q×f) of 14,700 GHz. By incorporating ScF3 to the hexagonal boron nitride (BN) ceramic, the CTE of ScF3<img>BN composite ceramic was adjusted to 3.36 × 10−6/°C, establishing compatibility with silicon-based chips. And finite element simulations verified that ScF3<img>BN composite significantly reduces thermal stress compared to Li2MoO4 or Al2O3 ceramics. Furthermore, this work demonstrates the potential of cold-sintered ScF3 to regulate thermal expansion in packaging substrates, paving the way for improved performance in next-generation electronic devices.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101126"},"PeriodicalIF":9.6,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017631","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

HfO2-based thin films and devices 基于hfo2的薄膜和器件

IF 9.6 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Journal of Materiomics

Pub Date : 2025-09-08 DOI: 10.1016/j.jmat.2025.101125

Xiaoguang Li, Min Hyuk Park, Ji-Yan Dai, Yuewei Yin

引用次数: 0