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3D alginate hydrogel microspheres with uniform micro-structure for cell culture and CVB3 infection. 三维海藻酸盐水凝胶微球,具有均匀的微观结构,用于细胞培养和CVB3感染。
IF 5.3 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-10 DOI: 10.1007/s00604-026-07865-3
Tianyi Zhang, Yuqing Xu, Yiwei Sun, Kun Ye, Jiarong Liu, Rui Zhang, Sirong Yu, Ziqiao Wang, Min Li, Hua Wang, Hongxing Shen, Xiaoxiang Zhou

An integrated microfluidic platform has been developed for the efficient generation of highly uniform alginate hydrogel microspheres (AHMs) encapsulating HeLa cells, enabling robust three dimensional (3D) cell culture and subsequent infection with Coxsackievirus B3 expressing enhanced green fluorescent protein (CVB3-eGFP). Our results demonstrate that AHMs support high cell viability and facilitated cell proliferation within a biomimetic 3D matrix. By systematically reducing the alginate concentration from 1.0% to 0.6%, we enhanced viral accessibility while maintaining microstructural integrity, thereby significantly improving CVB3-eGFP infection rates, as confirmed by fluorescence imaging and western blot analysis. This study establishes a tunable, reproducible, and physiologically relevant 3D model for studying virus-host interactions, with broad applications in antiviral drug screening and infectious disease modeling.

一个集成的微流控平台已经被开发出来,用于高效地生成高度均匀的海藻酸盐水凝胶微球(AHMs),包被HeLa细胞,实现强大的三维(3D)细胞培养和随后的柯萨奇病毒B3表达增强的绿色荧光蛋白(CVB3-eGFP)感染。我们的研究结果表明,ahm支持高细胞活力和促进细胞增殖的仿生3D基质。通过系统地将海藻酸盐浓度从1.0%降低到0.6%,我们在保持微观结构完整性的同时增强了病毒的可达性,从而显著提高了CVB3-eGFP的感染率,荧光成像和western blot分析证实了这一点。本研究为研究病毒-宿主相互作用建立了一个可调的、可重复的、生理相关的3D模型,在抗病毒药物筛选和传染病建模方面具有广泛的应用。
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引用次数: 0
Controllable synthesis of reticulated covalent organic polymers for the rapid extraction of triazine herbicides in vegetables prior to analysis by high-performance liquid chromatography. 网状共价有机聚合物的可控合成,用于高效液相色谱分析前快速提取蔬菜中三嗪类除草剂。
IF 5.3 2区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-10 DOI: 10.1007/s00604-026-07841-x
Bingnian Yang, Ziqin Peng, Guangping Xia, Guihua Ruan, Yipeng Huang, Ningli Tang
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引用次数: 0
Electrophoresis: An Effective Viability Assessment Method across Cell Domains. 电泳:一种有效的跨细胞域活力评估方法。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-10 DOI: 10.1021/acs.analchem.5c05986
Jesus Espino, Carlos A Mendiola-Escobedo, Alaleh Vaghef-Koodehi, Blanca H Lapizco-Encinas

Cell viability assessments are a critical step in numerous research, clinical and drug development processes. Electrokinetic techniques, such as electrorotation and dielectrophoresis, have shown promise as viability assessment methods, but often under specific and limited conditions. This study explores insulator-based electrokinetic (iEK) systems as a promising analytical alternative, leveraging differences in electromigration to rapidly separate viable and nonviable cells in a microfluidic system. To demonstrate broad efficacy and domain-agnostic discrimination, two prokaryotic bacterial lines (Escherichia coli and Salmonella Typhimurium) and two eukaryotic yeast strains (Saccharomyces cerevisiae ATCC 4098 and ATCC 9080) were studied. This work expands upon previous studies by performing separations in the weak and moderate electric field regimes, thus utilizing the linear and nonlinear regimes of electrophoresis as an adaptive separation mechanism for discriminating viable from nonviable cells. The results confirm that iEK systems can effectively and quantitatively separate viable and nonviable populations across distinct cellular domains (prokaryotic and eukaryotic), achieving high resolution (all Rs > 1.2) and good reproducibility across all conditions tested. This validation establishes iEK electrophoresis as a novel and robust analytical platform for rapid, quantitative cell viability assessment across a variety of disciplines.

细胞活力评估是众多研究、临床和药物开发过程中的关键步骤。电动技术,如电旋和电泳术,已经显示出作为活力评估方法的希望,但通常在特定和有限的条件下。本研究探索了基于绝缘体的电动力学(iEK)系统作为一种有前途的分析替代方案,利用电迁移的差异来快速分离微流体系统中的活细胞和非活细胞。为了证明广泛的功效和不区分领域,研究了两种原核细菌(大肠杆菌和鼠伤寒沙门氏菌)和两种真核酵母菌(酿酒酵母菌ATCC 4098和ATCC 9080)。这项工作扩展了先前的研究,在弱和中等电场条件下进行分离,从而利用电泳的线性和非线性制度作为一种适应性分离机制来区分活细胞和非活细胞。结果证实,iEK系统可以在不同的细胞结构域(原核和真核)中有效和定量地分离有活力和无活力的种群,在所有测试条件下实现高分辨率(所有Rs > 1.2)和良好的再现性。该验证建立了iEK电泳作为一种新的、强大的分析平台,用于快速、定量地评估各种学科的细胞活力。
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引用次数: 0
Guiding Similarity Search in Chemical Fragment Spaces with Weighted Fingerprints. 基于加权指纹的化学碎片空间相似性搜索。
IF 5.3 2区 化学 Q1 CHEMISTRY, MEDICINAL Pub Date : 2026-02-10 DOI: 10.1021/acs.jcim.5c02952
Justin Lübbers, Malte Schokolowski, Uta Lessel, Alexander Weber, Matthias Rarey

The introduction of chemical fragment spaces as a way to model large chemical spaces led to readily available compound libraries several orders of magnitude larger than seen before. The possibility of efficient similarity search based on molecular fingerprint comparison in such chemical fragment spaces was introduced by the SpaceLight algorithm for the first time. In this work, we introduce weighted SpaceLight, an enhancement that allows the algorithm to focus the search on important areas of a query molecule, increasing the local similarity while increasing variability in other areas, ultimately providing more structural control over the results. Due to the size of chemical fragment spaces, such customization methodologies become crucial to avoid millions of hits which have to be postfiltered. We demonstrate how weighted SpaceLight produces more molecules that preserve selected substructures during similarity search and how it can be adapted for different search scenarios. Combining global fingerprint similarity with a focus on specific substructures bridges the gap between existing search methods like SpaceLight and SpaceMACS and offers a new level of control for chemical space exploration in drug discovery.

引入化学碎片空间作为模拟大型化学空间的一种方式,导致了现成的化合物库比以前看到的大几个数量级。SpaceLight算法首次引入了基于分子指纹比对的化学碎片空间高效相似性搜索的可能性。在这项工作中,我们引入了加权SpaceLight,这是一种增强,允许算法将搜索集中在查询分子的重要区域,增加局部相似性,同时增加其他区域的可变性,最终提供对结果的更多结构控制。由于化学碎片空间的大小,这种定制方法对于避免数百万次必须经过后过滤的命中至关重要。我们演示了加权SpaceLight如何在相似性搜索过程中产生更多保留所选子结构的分子,以及如何适应不同的搜索场景。将全球指纹相似性与对特定子结构的关注相结合,弥补了现有搜索方法(如SpaceLight和SpaceMACS)之间的差距,并为药物发现中的化学空间探索提供了新的控制水平。
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引用次数: 0
A molecularly imprinted electrochemical sensor based on dual functional monomers for selective determination of nimodipine. 基于双功能单体的分子印迹电化学传感器选择性测定尼莫地平。
IF 2.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-10 DOI: 10.1039/d5ay01486g
Ying Wang, Xuyuan Sun, Minmin Liu, Zhengyuan Dai, Xiaoyu Yang, Li Li, Yaping Ding

As a core medication for the prevention and treatment of cerebral vasospasm, especially after aneurysmal subarachnoid hemorrhage, real-time monitoring of nimodipine (NMD) concentration helps evaluate the adequacy of drug therapy and holds great significance for ensuring patient life and health. Herein, based on dual functional monomers, a molecularly imprinted electrochemical sensor (MIECS) for the detection of NMD with nitrogen-doped multi-walled carbon nanotubes (N-CNTs) and Fe-MOFs was developed. Fe-MOFs provided a large specific surface area, offering more space for generating imprinting sites, while N-CNTs enhanced the conductivity of the electrode. 2-Amino-5-mercapto-1,3,4-thiadiazole (AMT) and o-phenylenediamine (o-PD) served as dual functional monomers and NMD as the template molecule. A molecularly imprinted polymer (MIP) membrane was prepared on the electrode surface by electropolymerization. Compared to single functional monomers, the dual functional monomers exhibited better selectivity and specificity in NMD recognition. Under optimal experimental conditions, the response of the MIECS to NMD showed a linear relationship ranging from 10-14 M to 10-8 M, with a detection limit of 2.97 × 10-15 M. Satisfactory recovery rates were obtained in the detection of human serum and tablets. This multi-parametric enhancement establishes a new paradigm for therapeutic drug monitoring in clinical neurology and pharmaceutical quality control.

尼莫地平(NMD)作为预防和治疗脑血管痉挛,特别是动脉瘤性蛛网膜下腔出血后脑血管痉挛的核心药物,实时监测其浓度有助于评估药物治疗的充分性,对保障患者生命健康具有重要意义。本文基于双功能单体,开发了一种用于检测氮掺杂多壁碳纳米管(N-CNTs)和Fe-MOFs的NMD的分子印迹电化学传感器(MIECS)。fe - mof提供了较大的比表面积,为产生印迹位点提供了更多的空间,而N-CNTs增强了电极的导电性。以2-氨基-5-巯基-1,3,4-噻二唑(AMT)和邻苯二胺(o-PD)为双功能单体,NMD为模板分子。采用电聚合方法在电极表面制备了分子印迹聚合物(MIP)膜。与单功能单体相比,双功能单体在NMD识别中表现出更好的选择性和特异性。在最佳实验条件下,mecs对NMD的响应在10-14 M ~ 10-8 M范围内呈线性关系,检出限为2.97 × 10-15 M,对人血清和片剂的检测回收率满意。这种多参数增强为临床神经病学和药物质量控制中的治疗药物监测建立了新的范例。
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引用次数: 0
Complexation of Plutonium and Other Actinides in Different Oxidation States with Gluconate at Low pH Values─A CE-ICP-MS Study. 低pH下不同氧化态的钚和其他锕系元素与葡萄糖酸盐的络合作用─CE-ICP-MS研究
IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2026-02-10 DOI: 10.1021/acs.inorgchem.5c04403
Janik Lohmann, Felix Sprunk, Diana Velikotrav, Alexander Wiebe, Julia Zemke, Tobias Reich

Using a coupling between capillary electrophoresis and ICP-MS (CE-ICP-MS), the gluconate (GLU) complexation of plutonium in the major oxidation states (III)-(VI) as well as Am(III), Th(IV), Np(V), and U(VI) was investigated at pH ≤ 4. CE-ICP-MS enabled the determination of the Pu oxidation state by comparing its electrophoretic mobility to that of a redox-analogous actinide (An). For the Am(III)/Pu(III) pair, the complex formation constants of three successive binary [An(GLU)x]3-x (x = 1-3) complexes could be determined. For Np(V)/Pu(V), the complex formation constants of the first binary [AnO2(GLU)](aq) complex were determined in accordance with previous literature for Np(V), and those of the second [AnO2(GLU)2]- complex were estimated. For U(VI)/Pu(VI), the constants of the [AnO2(GLU)]+, [AnO2(GLU-H)](aq), and [AnO2(GLU-H)(GLU)]- complexes were also determined in accordance with previous literature for U(VI). Plutonium in the oxidation states (III), (V), and (VI) behaved very similarly to the redox analogues. This was not the case for Th(IV)/Pu(IV). Here, the first five binary [Th(GLU)x]4-x (x = 1-5) complexes were determined for Th(IV), whereas mixed Pu-OH-GLU complexes were proposed for Pu(IV). The comparison of the first complex formation constants of the binary An-GLU complexes suggests a different bonding motif between An3+/4+ and AnO2+/2+, with AnO2+/2+ forming the weaker complexes.

采用毛细管电泳与ICP-MS (CE-ICP-MS)耦合的方法,在pH≤4的条件下,研究了钚在主要氧化态(III)-(VI)以及Am(III)、Th(IV)、Np(V)和U(VI)下的葡萄糖酸盐(GLU)络合反应。CE-ICP-MS通过比较其与氧化还原类似的锕系元素(An)的电泳迁移率来测定Pu的氧化态。对于Am(III)/Pu(III)对,可以确定三个连续二元[An(GLU)x]3-x (x = 1-3)配合物的形成常数。对于Np(V)/Pu(V),根据前人关于Np(V)的文献确定了第一个二元[AnO2(GLU)](aq)配合物的形成常数,并估计了第二个[AnO2(GLU)2]-配合物的形成常数。对U(VI)/Pu(VI)进行了[AnO2(GLU)]+、[AnO2(GLU- h)](aq)和[AnO2(GLU- h)(GLU)]-配合物的常数测定。钚在氧化态(III)、(V)和(VI)下的表现与氧化还原类似物非常相似。Th(IV)/Pu(IV)的情况并非如此。在这里,确定了Th(IV)的前五个二元[Th(GLU)x]4-x (x = 1-5)配合物,而Pu(IV)的混合Pu- oh -GLU配合物。对二元An-GLU配合物的第一络合物形成常数的比较表明,An3+/4+和AnO2+/2+之间的键基序不同,其中AnO2+/2+形成较弱的配合物。
{"title":"Complexation of Plutonium and Other Actinides in Different Oxidation States with Gluconate at Low pH Values─A CE-ICP-MS Study.","authors":"Janik Lohmann, Felix Sprunk, Diana Velikotrav, Alexander Wiebe, Julia Zemke, Tobias Reich","doi":"10.1021/acs.inorgchem.5c04403","DOIUrl":"https://doi.org/10.1021/acs.inorgchem.5c04403","url":null,"abstract":"<p><p>Using a coupling between capillary electrophoresis and ICP-MS (CE-ICP-MS), the gluconate (GLU) complexation of plutonium in the major oxidation states (III)-(VI) as well as Am(III), Th(IV), Np(V), and U(VI) was investigated at pH ≤ 4. CE-ICP-MS enabled the determination of the Pu oxidation state by comparing its electrophoretic mobility to that of a redox-analogous actinide (An). For the Am(III)/Pu(III) pair, the complex formation constants of three successive binary [An(GLU)<sub><i>x</i></sub>]<sup>3-<i>x</i></sup> (<i>x</i> = 1-3) complexes could be determined. For Np(V)/Pu(V), the complex formation constants of the first binary [AnO<sub>2</sub>(GLU)]<sub>(aq)</sub> complex were determined in accordance with previous literature for Np(V), and those of the second [AnO<sub>2</sub>(GLU)<sub>2</sub>]<sup>-</sup> complex were estimated. For U(VI)/Pu(VI), the constants of the [AnO<sub>2</sub>(GLU)]<sup>+</sup>, [AnO<sub>2</sub>(GLU<sub>-H</sub>)]<sub>(aq)</sub>, and [AnO<sub>2</sub>(GLU<sub>-H</sub>)(GLU)]<sup>-</sup> complexes were also determined in accordance with previous literature for U(VI). Plutonium in the oxidation states (III), (V), and (VI) behaved very similarly to the redox analogues. This was not the case for Th(IV)/Pu(IV). Here, the first five binary [Th(GLU)<sub><i>x</i></sub>]<sup>4-<i>x</i></sup> (<i>x</i> = 1-5) complexes were determined for Th(IV), whereas mixed Pu-OH-GLU complexes were proposed for Pu(IV). The comparison of the first complex formation constants of the binary An-GLU complexes suggests a different bonding motif between An<sup>3+/4+</sup> and AnO<sub>2</sub><sup>+/2+</sup>, with AnO<sub>2</sub><sup>+/2+</sup> forming the weaker complexes.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":" ","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146148454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Relocation of Endocytic Leaflet DNA Probes for Asymmetric and Week-Long Lysosomal Labeling. 内噬小叶DNA探针的重新定位用于不对称和长达一周的溶酶体标记。
IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1021/jacs.5c21974
An Yan, Yuhan Kong, Yuxing Shang, Yifan Ge, Hang Xing, Di Li

Visualization of lysosomes in living cells is essential for understanding their physiological functions; yet, most probes that target the lysosomal interior often disrupt luminal chemistry, exhibit signal leakage, and fail to support long-term imaging. To address these challenges, we developed RELAY (Relocation of Endocytic Leaflet tAg to modifY organelles), a topology-preserving labeling strategy to transfer the inner-leaflet tags on the plasma membrane to the cytosol-facing outer leaflet of lysosomes. RELAY employs liposome-cell membrane fusion to anchor fluorescent DNA probes with phosphorothioate (PS) backbones on the cytoplasmic inner leaflet of the plasma membrane, followed by endocytic trafficking that preserves the membrane topology and relocates the probes onto the lysosomal outer surface. Because this labeling occurs on the lysosomal exterior that is protected from luminal degradation and the PS backbone resists nuclease degradation, RELAY enables highly stable asymmetric labeling that sustains week-long lysosome imaging in living cells. Using this approach, we visualized lysosomal dynamics during cellular senescence and discovered random, unidirectional, intercellular lysosomal transfer in cell-cell communications via tunnelling nanotubes. Holding the capability for prolonged, high-fidelity visualization of lysosomes, RELAY facilitates the exploration of their biological functions.

活细胞中溶酶体的可视化对理解其生理功能至关重要;然而,大多数靶向溶酶体内部的探针通常会破坏腔内化学,表现出信号泄漏,并且不能支持长期成像。为了解决这些挑战,我们开发了RELAY (Relocation of Endocytic leaftag To modifY organelles),这是一种保持拓扑结构的标记策略,可将质膜上的内小叶标签转移到溶酶体面向细胞质的外小叶上。RELAY采用脂质体-细胞膜融合将带有硫代酸盐(PS)骨架的荧光DNA探针固定在质膜的细胞质内小叶上,然后进行内吞运输,保留膜拓扑结构并将探针重新定位到溶酶体外表面。由于这种标记发生在不受腔内降解保护的溶酶体表面,并且PS主链抵抗核酸酶降解,RELAY能够实现高度稳定的不对称标记,维持活细胞中溶酶体长达一周的成像。利用这种方法,我们可视化了细胞衰老过程中的溶酶体动力学,并通过隧道纳米管发现了细胞间通讯中随机、单向的细胞间溶酶体转移。RELAY具有对溶酶体进行长时间高保真可视化的能力,有助于探索其生物学功能。
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引用次数: 0
A Layer-Based Model for Frictional Sliding of Pillar Arrays. 基于层的柱阵摩擦滑动模型。
IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1021/acs.langmuir.5c05261
Jasreen Kaur, Xuemei Xiao, Preetika Karnal, Chung Yuen Hui, Anand Jagota

Bioinspired micropatterned surfaces have been studied as a way to enhance or control interfacial mechanical properties. Here, we study friction for the relative sliding of two interdigitated pillar surfaces. The overall frictional force originates from individual pillar-pillar interactions across the interface as well as the interpillar coupling within each substrate. In this study, we develop a layer-based physical model to simulate the contact and sliding behavior of these pillar arrays. The system is modeled as comprising four layers of nodes, with uniform shear displacement applied to the top layer, while the bottom one is held fixed. Nodes in the inner two layers represent the joints between the pillars and the substrate. The model predicts shear friction force and reveals underlying deformation mechanisms at various misorientations and height overlaps, in good agreement with measured friction in sliding experiments.

仿生微图案表面作为一种增强或控制界面力学性能的方法已被研究。在这里,我们研究了两个互指柱表面相对滑动的摩擦。整体摩擦力来自于单个柱-柱之间的相互作用以及每个衬底内部柱间的耦合。在这项研究中,我们开发了一个基于层的物理模型来模拟这些柱阵列的接触和滑动行为。系统建模为由四层节点组成,顶层采用均匀剪切位移,底层保持固定。内两层的节点代表柱与衬底之间的接缝。该模型预测了剪切摩擦力,揭示了不同方向和高度重叠下的潜在变形机制,与滑动实验中测量的摩擦力吻合良好。
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引用次数: 0
Analytical Nuclear Gradients for the Multiconfigurational Self-Consistent Field Method Coupled with the Polarizable Fluctuating Charges Model. 耦合极化波动电荷模型的多构型自洽场法的解析核梯度。
IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-10 Epub Date: 2026-01-27 DOI: 10.1021/acs.jctc.5c01890
Francesco Mazza, Marco Trinari, Chiara Sepali, Chiara Cappelli

The multiscale model combining the multiconfigurational self-consistent field (MCSCF) method with the fully atomistic polarizable Fluctuating Charges (FQ) force field (Sepali, C.; et al. J. Chem. Theory Comput. 2024, 20, 9954-9967) is here extended to the calculation of analytical nuclear gradients. The gradients are derived from first-principles, implemented in the OpenMolcas package, and validated against numerical references. The resulting MCSCF/FQ nuclear gradients are employed to simulate vibronic absorption spectra of aromatic molecules in aqueous solution, namely benzene and phenol. By integrating this approach with molecular dynamics simulations, both solute conformational flexibility and the dynamical aspects of solvation are properly captured. The computed spectra reproduce experimental profiles and relative band intensities with remarkable accuracy, demonstrating the capability of the MCSCF/FQ model to simultaneously describe the multireference character of the solute and its interaction with the solvent environment.

将多构型自洽场(MCSCF)方法与全原子极化波动电荷(FQ)力场相结合的多尺度模型(Sepali, C.;等)。j .化学。理论计算。2024,20,9954-9967)在这里扩展到解析核梯度的计算。梯度是从第一性原理推导出来的,在OpenMolcas包中实现,并根据数值参考进行验证。利用所得的MCSCF/FQ核梯度模拟了水溶液中芳香族分子(即苯和苯酚)的振动吸收光谱。通过将这种方法与分子动力学模拟相结合,溶质构象灵活性和溶剂化的动力学方面都得到了适当的捕获。计算得到的光谱以极高的精度再现了实验剖面和相对波段强度,证明了MCSCF/FQ模型能够同时描述溶质的多参比特征及其与溶剂环境的相互作用。
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引用次数: 0
Benchmarking Density Functional Theory for Accurate Calculation of Nitride Band Gaps. 精确计算氮化物带隙的基准密度泛函理论。
IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-10 Epub Date: 2026-01-27 DOI: 10.1021/acs.jctc.5c01703
Chris E Mohn, Helmer Fjellvåg, Ponniah Vajeeston, Martin Valldor, Kristin Bergum

We benchmark exchange-correlation functionals for the calculation of fundamental band gaps of inorganic nitrides. These include conventional functionals such as the local density approximation (LDA), the generalized-gradient (Perdew-Burke-Ernzerhof) approximation (PBE), simple Slater exchange functionals (SLOC), specialized LDA/GGA-derived high local exchange (HLE16) and Armiento-Kümmel semilocal (AK13) functionals, meta-GGA functionals including TASK, the modified Becke-Johnson functional (mBJ), and Heyd-Scuseria-Ernzerhof (HSE06) hybrid functional, as well as quasiparticle GW theory. Since inorganic nitrides remain strongly under-represented in previous extensive benchmark studies, the current subdatabase contributes towards building a future large-scale balanced materials compilation of band gaps to benchmark theory. From a literature survey, we carefully collect 25 binary and 11 ternary nitrides with a focus on semiconductors spanning the periodic table, including ionic Li3N, antibixbyite-structured X3N2 (X = Be, Mg, Ca), early transition metals and lanthanides (e.g., ScN, YN, and LaN), ultrahard Th3P4-type structured M3N4 (M = Zr, Hf) compounds, promising photocatalysts Ta3N5, different polymorphs of III-V reference covalent nitrides (BN, AlN, GaN), and many M3N4 polymorphs (M = C, Si, and Ge) such as spinel-structured phases. Consistent with previous extensive benchmark tests, conventional LDA/PBE unsystematically largely underestimate band gaps with mean absolute errors (MAE) of >1.0 eV and mean absolute percentage errors (MAPE) of about 50%. Simple Slater exchange functional, SLOC, the GGA-derived AK13LDA and HLE16 functionals show improvement over LDA/PBE with MAE of 0.5-0.6 eV (MAPE ∼ 20-25%) with mBJ and HSE06 being the most accurate, with MAE = 0.30 and 0.28 eV (MAPE 12.1% and 11.1%), respectively. Strategies for the development of machine learning and the choice of appropriate exchange-correlation functionals for high-throughput large-scale material screening are discussed in light of these results.

我们将交换相关函数作为计算无机氮化物基本带隙的基准。这些包括传统的泛函,如局部密度近似(LDA)、广义梯度(Perdew-Burke-Ernzerhof)近似(PBE)、简单的Slater交换泛函(SLOC)、专门的LDA/ gga衍生的高局部交换(HLE16)和armiento - k mmel半局部(AK13)泛函、元gga泛函(包括TASK)、改进的Becke-Johnson泛函(mBJ)和Heyd-Scuseria-Ernzerhof (HSE06)混合泛函,以及准粒子GW理论。由于无机氮化物在以前广泛的基准研究中仍然严重不足,目前的子数据库有助于建立未来大规模平衡材料的带隙基准理论汇编。从文献调查中,我们仔细收集了25种二元和11种三元氮化物,重点关注半导体元素周期表,包括离子Li3N,抗碳素体结构的X3N2 (X = Be, Mg, Ca),早期过渡金属和镧系元素(例如,ScN, YN和LaN),超硬th3p4型结构的M3N4 (M = Zr, Hf)化合物,有前途的光催化剂Ta3N5, III-V参考共价氮化物(BN, AlN, GaN)的不同多晶型,以及许多M3N4多晶型(M = C, Si, Si)。和Ge),如尖晶石结构相。与之前广泛的基准测试一致,传统的LDA/PBE在很大程度上非系统地低估了带隙,平均绝对误差(MAE)为100 eV,平均绝对百分比误差(MAPE)约为50%。简单Slater交换功能,SLOC, gga衍生的AK13LDA和HLE16功能比LDA/PBE表现出改善,MAE为0.5-0.6 eV (MAPE ~ 20-25%),其中mBJ和HSE06最准确,MAE分别为0.30和0.28 eV (MAPE分别为12.1%和11.1%)。根据这些结果,讨论了机器学习发展策略和选择合适的交换相关函数进行高通量大规模材料筛选。
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引用次数: 0
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