首页 > 最新文献

The Journal of Physical Chemistry C最新文献

英文 中文
Ab-Initio Exploration of Stoichiometric and Nonstoichiometric CsK2Sb Photocathodes for Photoemission Applications 化学计量和非化学计量CsK2Sb光电阴极在光电发射中的应用
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-30 DOI: 10.1021/acs.jpcc.5c06660
Sandip Aryal, , , Gaoxue Wang, , and , Enrique R. Batista*, 

Bialkali antimonide photocathodes, such as cesium potassium antimonide (CsK2Sb), have emerged as strong candidates for next-generation photocathodes in linear accelerators due to their low work function, fast response, high quantum yield, and visible-light sensitivity. However, a critical gap remains in understanding how defects─unavoidable in real materials and responsible for driving nonstoichiometric phases─affect these desirable photoemissive properties. Most theoretical studies have so far considered only perfectly stoichiometric crystals, overlooking the role of imperfections introduced during synthesis. Here, we address this gap using state-of-the-art first-principles calculations to explore both ideal and defected CsK2Sb. For the stoichiometric phase, our results confirm strong absorption in the visible range and a significantly reduced work function compared to metallic photocathodes, consistent with experiments. Moving beyond the ideal case, we identify cesium and potassium vacancies as the most prevalent intrinsic defects. These vacancies might introduce midgap states, reshape the absorption spectrum, and are poised to strongly influence photoemission efficiency. By connecting intrinsic defects to performance, this work advances fundamental understanding of CsK2Sb and provides practical insights for optimizing high-efficiency photocathodes.

双碱锑化光阴极,如铯锑化钾(CsK2Sb),由于其低功函数、快速响应、高量子产率和可见光灵敏度,已成为线性加速器中下一代光电阴极的有力候选材料。然而,在理解缺陷──在真实材料中不可避免的,并负责驱动非化学计量相──如何影响这些理想的光电特性方面,仍然存在一个关键的差距。迄今为止,大多数理论研究只考虑了完美的化学计量晶体,忽视了合成过程中引入的缺陷的作用。在这里,我们使用最先进的第一性原理计算来解决这一差距,以探索理想和缺陷的CsK2Sb。对于化学计量相,我们的结果证实了在可见光范围内的强吸收和与金属光电阴极相比显着降低的功函数,与实验一致。超越理想的情况下,我们确定铯和钾的空缺是最普遍的内在缺陷。这些空位可能会引入中隙态,重塑吸收光谱,并对光发射效率产生强烈影响。通过将内在缺陷与性能联系起来,这项工作推进了对CsK2Sb的基本理解,并为优化高效光电阴极提供了实用的见解。
{"title":"Ab-Initio Exploration of Stoichiometric and Nonstoichiometric CsK2Sb Photocathodes for Photoemission Applications","authors":"Sandip Aryal,&nbsp;, ,&nbsp;Gaoxue Wang,&nbsp;, and ,&nbsp;Enrique R. Batista*,&nbsp;","doi":"10.1021/acs.jpcc.5c06660","DOIUrl":"10.1021/acs.jpcc.5c06660","url":null,"abstract":"<p >Bialkali antimonide photocathodes, such as cesium potassium antimonide (CsK<sub>2</sub>Sb), have emerged as strong candidates for next-generation photocathodes in linear accelerators due to their low work function, fast response, high quantum yield, and visible-light sensitivity. However, a critical gap remains in understanding how defects─unavoidable in real materials and responsible for driving nonstoichiometric phases─affect these desirable photoemissive properties. Most theoretical studies have so far considered only perfectly stoichiometric crystals, overlooking the role of imperfections introduced during synthesis. Here, we address this gap using state-of-the-art first-principles calculations to explore both ideal and defected CsK<sub>2</sub>Sb. For the stoichiometric phase, our results confirm strong absorption in the visible range and a significantly reduced work function compared to metallic photocathodes, consistent with experiments. Moving beyond the ideal case, we identify cesium and potassium vacancies as the most prevalent intrinsic defects. These vacancies might introduce midgap states, reshape the absorption spectrum, and are poised to strongly influence photoemission efficiency. By connecting intrinsic defects to performance, this work advances fundamental understanding of CsK<sub>2</sub>Sb and provides practical insights for optimizing high-efficiency photocathodes.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2327–2340"},"PeriodicalIF":3.2,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089632","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Decoding Supramolecular Order in Naphthalene Diimides through Locally Disordered Entities 通过局部无序实体解码萘二亚胺的超分子秩序
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-30 DOI: 10.1021/acs.jpcc.5c07222
Parth Raval, , , Soumik Sao, , , Triza Pal, , , Tomasz Pawlak, , , Sayan Bhattacharjee, , , Rohit Bhowal, , , Sayantan Khan, , , Deepak Chopra, , , Debangshu Chaudhuri*, , and , G. N. Manjunatha Reddy*, 

Materials design for wider organic electronics greatly benefits from supramolecular chemistry approaches, whereby elucidating structure-driven noncovalent interactions across length scales represents a characterization challenge. Methods probing long-range order often struggle to identify the heterogeneous nature of van der Waals interactions, leaving locally disordered regions and their impact on bulk properties unexamined. This study demonstrates that structural polymorphism in regioisomeric pyridine-substituted naphthalene diimide (PyNDI) assemblies imparts varying degrees of order and disorder. A synergistic combination of X-ray diffraction (XRD) and solid-state nuclear magnetic resonance (ssNMR) spectroscopy, supported by computational modeling, reveals that supramolecular order in ortho (o)- and para (p)-PyNDIs arises from cooperative π-stacking, lone-pair-π interactions, and lamellar interdigitation. In contrast, the meta (m)-isomer exhibits local disorder with different packing motifs that can be iteratively modeled using the structural knowledge obtained from their o- and p-PyNDIs crystalline analogues. The approach uniquely resolves locally disordered motifs by leveraging information obtained from structurally similar, but well-ordered, isomers of π-conjugated assemblies relevant to the optoelectronic paradigm.

更广泛的有机电子学材料设计极大地受益于超分子化学方法,因此阐明跨长度尺度的结构驱动的非共价相互作用代表了表征挑战。探测长程有序的方法往往难以确定范德华相互作用的异质性质,导致局部无序区域及其对体性质的影响未得到检验。本研究表明,区域异构体吡啶取代萘二亚胺(PyNDI)的结构多态性赋予了不同程度的有序和无序。x射线衍射(XRD)和固态核磁共振(ssNMR)的协同组合,在计算模型的支持下,揭示了邻位(o)-和对(p)- pyndi中的超分子有序是由协同π堆积、孤对π相互作用和片层交错形成的。相反,元(m)-异构体表现出具有不同填充基序的局部无序,可以使用从它们的o-和p-PyNDIs晶体类似物中获得的结构知识进行迭代建模。该方法通过利用从与光电范例相关的π共轭组件的结构相似但有序的同分异构体中获得的信息,独特地解决了局部无序基序。
{"title":"Decoding Supramolecular Order in Naphthalene Diimides through Locally Disordered Entities","authors":"Parth Raval,&nbsp;, ,&nbsp;Soumik Sao,&nbsp;, ,&nbsp;Triza Pal,&nbsp;, ,&nbsp;Tomasz Pawlak,&nbsp;, ,&nbsp;Sayan Bhattacharjee,&nbsp;, ,&nbsp;Rohit Bhowal,&nbsp;, ,&nbsp;Sayantan Khan,&nbsp;, ,&nbsp;Deepak Chopra,&nbsp;, ,&nbsp;Debangshu Chaudhuri*,&nbsp;, and ,&nbsp;G. N. Manjunatha Reddy*,&nbsp;","doi":"10.1021/acs.jpcc.5c07222","DOIUrl":"10.1021/acs.jpcc.5c07222","url":null,"abstract":"<p >Materials design for wider organic electronics greatly benefits from supramolecular chemistry approaches, whereby elucidating structure-driven noncovalent interactions across length scales represents a characterization challenge. Methods probing long-range order often struggle to identify the heterogeneous nature of van der Waals interactions, leaving locally disordered regions and their impact on bulk properties unexamined. This study demonstrates that structural polymorphism in regioisomeric pyridine-substituted naphthalene diimide (PyNDI) assemblies imparts varying degrees of order and disorder. A synergistic combination of X-ray diffraction (XRD) and solid-state nuclear magnetic resonance (ssNMR) spectroscopy, supported by computational modeling, reveals that supramolecular order in <i>ortho</i> (<i>o</i>)- and <i>para</i> (<i>p</i>)-PyNDIs arises from cooperative π-stacking, lone-pair-π interactions, and lamellar interdigitation. In contrast, the <i>meta</i> (<i>m</i>)-isomer exhibits local disorder with different packing motifs that can be iteratively modeled using the structural knowledge obtained from their <i>o</i>- and <i>p</i>-PyNDIs crystalline analogues. The approach uniquely resolves locally disordered motifs by leveraging information obtained from structurally similar, but well-ordered, isomers of π-conjugated assemblies relevant to the optoelectronic paradigm.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2223–2233"},"PeriodicalIF":3.2,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the Effect of Varying Chain Length and Wettability on the Charge-Storage Performance in Donor–Acceptor–Donor-Type Electrode-Based Pseudocapacitors 揭示不同链长和润湿性对供体-受体-供体型电极基伪电容器电荷存储性能的影响
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-30 DOI: 10.1021/acs.jpcc.5c07910
Dnyaneshwar D. Ugale, , , Sidhanath V. Bhosale*, , and , Sheshanath V. Bhosale*, 

Pseudocapacitors (PSCs) based on small organic molecule materials have attracted significant research interest due to their structural diversity, tunable redox properties, and ability to support widening the operational potential window, offering higher energy density and rapid power density. Nevertheless, the progress is hindered by their unsatisfactory cycling stability. An approach to tailoring the cycling life of the organic electrode materials for supercapacitors (SCs) is extending π-conjugation of the molecular architecture. To improve the overall performance of the supercapacitor device, the electrode materials, in particular conjugated donor–acceptor–donor (D–A–D)-type molecules, can store both positive and negative charge in a pseudocapacitor device. The D–A–D-type conjugation with good packing could facilitate charge transport and enhance the electrochemical characteristics of the SC cell configurations. In this work, new D–A–D-type 2,7-bis(10-(2-ethylhexyl)-10H-phenothiazin-3-yl) benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (PTZ-NDI-EH) and 2,7-bis(10-(2-hexyldecyl)-10H-phenothiazin-3-yl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (PTZ-NDI-HD) bearing two different alkyl chains are designed and synthesized. The optimized PTZ-NDI-EH and PTZ-NDI-HD active organic electrode materials in combination with conducting graphite foil (GF) exhibit outstanding functionalities such as higher specific capacitance, higher energy density, and longer cycling stability. Such higher PSC performance could be originating from the molecular packing, higher electronic conductivity, and enhanced charge delocalization during the Faradaic reversible redox processes. The higher cycling stability could be attributed to efficient ion transportation. In addition, the alkyl chain length influences the electrochemical properties of PTZ-NDI-EH and PTZ-NDI-HD. The increase in contact angle of PTZ-NDI-HD (higher alkyl chain length) leads to the reduction of the specific capacitance compared to PTZ-NDI-EH (lower alkyl chain length). This provides the basis for the wettability of the electrode in the presence of aqueous electrolytes and their impact on the electrochemical properties. These results indicate that the D–A–D materials design and their applications contribute to the development of high-performance electrical energy storage (EES) devices.

基于小有机分子材料的假电容器(PSCs)由于其结构多样性、可调节的氧化还原特性以及支持扩大工作电位窗口的能力,提供更高的能量密度和快速的功率密度,引起了人们的极大研究兴趣。然而,由于其不理想的循环稳定性,这一进展受到阻碍。扩大分子结构的π共轭是提高超级电容器有机电极材料循环寿命的一种途径。为了提高超级电容器器件的整体性能,电极材料,特别是共轭供体-受体-供体(D-A-D)型分子,可以在假电容器器件中同时存储正电荷和负电荷。具有良好填料的d - a - d型共轭可以促进电荷传输,提高SC电池结构的电化学特性。本文设计并合成了新型d - a - d型2,7-二(10-(2-乙基己基)- 10h -吩噻嗪-3-基)苯并[lmn][3,8]菲罗啉-1,3,6,8(2H,7H)-四酮(PTZ-NDI-EH)和2,7-二(10-(2-己基癸基)- 10h -吩噻嗪-3-基)苯并[lmn][3,8]菲罗啉-1,3,6,8(2H,7H)-四酮(PTZ-NDI-HD)。优化后的PTZ-NDI-EH和PTZ-NDI-HD活性有机电极材料与导电石墨箔(GF)结合,表现出更高的比电容、更高的能量密度和更长的循环稳定性。这种更高的PSC性能可能源于分子包装、更高的电子导电性以及法拉第可逆氧化还原过程中电荷离域的增强。较高的循环稳定性可归因于高效的离子运输。此外,烷基链长度对PTZ-NDI-EH和PTZ-NDI-HD的电化学性能也有影响。较高烷基链长度的PTZ-NDI-HD与较低烷基链长度的PTZ-NDI-EH相比,接触角增大导致比电容减小。这为电极在水电解质存在下的润湿性及其对电化学性能的影响提供了基础。这些结果表明,D-A-D材料的设计及其应用有助于高性能电能存储(EES)器件的发展。
{"title":"Unveiling the Effect of Varying Chain Length and Wettability on the Charge-Storage Performance in Donor–Acceptor–Donor-Type Electrode-Based Pseudocapacitors","authors":"Dnyaneshwar D. Ugale,&nbsp;, ,&nbsp;Sidhanath V. Bhosale*,&nbsp;, and ,&nbsp;Sheshanath V. Bhosale*,&nbsp;","doi":"10.1021/acs.jpcc.5c07910","DOIUrl":"10.1021/acs.jpcc.5c07910","url":null,"abstract":"<p >Pseudocapacitors (PSCs) based on small organic molecule materials have attracted significant research interest due to their structural diversity, tunable redox properties, and ability to support widening the operational potential window, offering higher energy density and rapid power density. Nevertheless, the progress is hindered by their unsatisfactory cycling stability. An approach to tailoring the cycling life of the organic electrode materials for supercapacitors (SCs) is extending π-conjugation of the molecular architecture. To improve the overall performance of the supercapacitor device, the electrode materials, in particular conjugated donor–acceptor–donor (D–A–D)-type molecules, can store both positive and negative charge in a pseudocapacitor device. The D–A–D-type conjugation with good packing could facilitate charge transport and enhance the electrochemical characteristics of the SC cell configurations. In this work, new D–A–D-type 2,7-bis(10-(2-ethylhexyl)-10<i>H</i>-phenothiazin-3-yl) benzo[lmn][3,8]phenanthroline-1,3,6,8(2H,7H)-tetraone (PTZ-NDI-EH) and 2,7-bis(10-(2-hexyldecyl)-10H-phenothiazin-3-yl)benzo[lmn][3,8]phenanthroline-1,3,6,8(2<i>H</i>,7<i>H</i>)-tetraone (PTZ-NDI-HD) bearing two different alkyl chains are designed and synthesized. The optimized PTZ-NDI-EH and PTZ-NDI-HD active organic electrode materials in combination with conducting graphite foil (GF) exhibit outstanding functionalities such as higher specific capacitance, higher energy density, and longer cycling stability. Such higher PSC performance could be originating from the molecular packing, higher electronic conductivity, and enhanced charge delocalization during the Faradaic reversible redox processes. The higher cycling stability could be attributed to efficient ion transportation. In addition, the alkyl chain length influences the electrochemical properties of PTZ-NDI-EH and PTZ-NDI-HD. The increase in contact angle of PTZ-NDI-HD (higher alkyl chain length) leads to the reduction of the specific capacitance compared to PTZ-NDI-EH (lower alkyl chain length). This provides the basis for the wettability of the electrode in the presence of aqueous electrolytes and their impact on the electrochemical properties. These results indicate that the D–A–D materials design and their applications contribute to the development of high-performance electrical energy storage (EES) devices.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2107–2118"},"PeriodicalIF":3.2,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089638","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Stable Light-Trapping SERS Substrates with Bioinspired Arrays for Biochemical Sensing 稳定的光捕获SERS基底与生物启发阵列用于生化传感
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-30 DOI: 10.1021/acs.jpcc.5c08632
Maohua Quan, , , Yuting Qiu, , and , Zhou Yang*, 

In Raman spectroscopy, the optimal signal is obtained when the sample is irradiated by a laser at normal incidence. Ensuring both signal stability and high sensitivity for capturing analyte molecules on nonflat or tilted substrates remains difficult, especially in the process of rapid testing. Here, 3D hemispherical polydimethylsiloxane (PDMS) substrate with bioinspired compound-eye structure was fabricated by utilizing the liquid–liquid interface self-assembly and transfer technique. Using Au monolayer films decorated PDMS substrate as a surface-enhanced Raman scattering (SERS) substrate. The rotational symmetry of the bioinspired SERS substrate architecture enables stable SERS performance even under substrate tilting from 0 to 75°, demonstrating excellent suitability for field-based detection applications. The hemispherical SERS substrate demonstrated a minimum detectable urea concentration of 10–5 M, which is significantly lower than the minimum urea level (10–3 M) in the tear fluid of the body.

在拉曼光谱中,当样品被正入射激光照射时获得最佳信号。确保在非平坦或倾斜的衬底上捕获分析物分子的信号稳定性和高灵敏度仍然是困难的,特别是在快速测试过程中。利用液-液界面自组装和转移技术,制备了具有仿生复眼结构的三维半球形聚二甲基硅氧烷(PDMS)底物。采用金单层膜装饰PDMS衬底作为表面增强拉曼散射衬底。生物启发的SERS基板结构的旋转对称性即使在基板倾斜从0到75°的情况下也能实现稳定的SERS性能,证明了出色的现场检测应用适用性。半球形SERS底物显示最低可检测尿素浓度为10-5 M,显著低于人体泪液中最低尿素水平(10-3 M)。
{"title":"Stable Light-Trapping SERS Substrates with Bioinspired Arrays for Biochemical Sensing","authors":"Maohua Quan,&nbsp;, ,&nbsp;Yuting Qiu,&nbsp;, and ,&nbsp;Zhou Yang*,&nbsp;","doi":"10.1021/acs.jpcc.5c08632","DOIUrl":"10.1021/acs.jpcc.5c08632","url":null,"abstract":"<p >In Raman spectroscopy, the optimal signal is obtained when the sample is irradiated by a laser at normal incidence. Ensuring both signal stability and high sensitivity for capturing analyte molecules on nonflat or tilted substrates remains difficult, especially in the process of rapid testing. Here, 3D hemispherical polydimethylsiloxane (PDMS) substrate with bioinspired compound-eye structure was fabricated by utilizing the liquid–liquid interface self-assembly and transfer technique. Using Au monolayer films decorated PDMS substrate as a surface-enhanced Raman scattering (SERS) substrate. The rotational symmetry of the bioinspired SERS substrate architecture enables stable SERS performance even under substrate tilting from 0 to 75°, demonstrating excellent suitability for field-based detection applications. The hemispherical SERS substrate demonstrated a minimum detectable urea concentration of 10<sup>–5</sup> M, which is significantly lower than the minimum urea level (10<sup>–3</sup> M) in the tear fluid of the body.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2287–2293"},"PeriodicalIF":3.2,"publicationDate":"2026-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effect of Gold Nanoparticle Size and DNA Concentration on DNA-Nanoparticles Complexation: A Molecular Dynamics Study 金纳米颗粒大小和DNA浓度对DNA-纳米颗粒络合的影响:分子动力学研究
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-29 DOI: 10.1021/acs.jpcc.5c07253
J. Hingies Monisha, , , Vasumathi Velachi*, , and , Prabal K. Maiti, 

Ensuring the stability of the AuNP-gene complex until it reaches the target sites is a crucial factor for the success of gene therapy. Although different AuNP sizes and AuNP-to-DNA ratios are investigated for specific therapeutic needs, their role in the stability and packaging of AuNP-DNA complex remains unclear. In this study, we employ all-atom molecular dynamics simulations to investigate the influence of cationic ligand-functionalized AuNP (CAuNP) size and CAuNP-to-DNA ratio on DNA wrapping and binding affinity. The obtained results show that a single DNA interacting with smaller CAuNPs exhibits greater bending and wrapping due to their higher curvature. However, when two DNAs bind to smaller CAuNPs, electrostatic repulsion prevents the effective wrapping, which leads the DNAs to twist from their original orientation. Such behavior is not observed with larger CAuNPs since their increased size may mitigate repulsive forces. Further, the analysis on axial bending angle reveals that smaller AuNPs induce sharper DNA bending and larger AuNPs promote smoother bending. In addition, the potential of mean force (PMF) analysis confirms a stronger DNA binding affinity for larger AuNPs, with affinity decreasing when two DNAs attach to a single CAuNP. Our results from the DNA loading capacity calculations provide insights into the maximum number of DNA molecules that can be loaded onto CAuNPs of a given size. These findings offer key insights into optimizing the size of AuNP and DNA-to-AuNP ratios for the development of efficient gene delivery systems.

确保aunp基因复合物的稳定性,直到它到达目标位点是基因治疗成功的关键因素。尽管不同的AuNP大小和AuNP与dna的比例被研究用于特定的治疗需求,但它们在AuNP- dna复合物的稳定性和包装中的作用仍不清楚。在这项研究中,我们采用全原子分子动力学模拟来研究阳离子配体功能化的AuNP (CAuNP)大小和CAuNP与DNA的比例对DNA包裹和结合亲和力的影响。所得结果表明,单个DNA与较小的CAuNPs相互作用,由于其更高的曲率而表现出更大的弯曲和包裹。然而,当两个dna与较小的CAuNPs结合时,静电斥力会阻止有效的包裹,从而导致dna从原来的方向扭曲。这种行为在较大的CAuNPs中没有观察到,因为它们的增大可能会减轻排斥力。此外,对轴向弯曲角的分析表明,较小的AuNPs诱导DNA弯曲更尖锐,而较大的AuNPs促进弯曲更平滑。此外,平均力电位(PMF)分析证实了对较大的aunp具有更强的DNA结合亲和力,当两个DNA与单个CAuNP结合时,亲和力降低。我们的DNA装载能力计算结果提供了可以装载到给定大小的CAuNPs上的最大DNA分子数量的见解。这些发现为优化AuNP的大小和dna与AuNP的比率提供了关键的见解,以开发有效的基因传递系统。
{"title":"Effect of Gold Nanoparticle Size and DNA Concentration on DNA-Nanoparticles Complexation: A Molecular Dynamics Study","authors":"J. Hingies Monisha,&nbsp;, ,&nbsp;Vasumathi Velachi*,&nbsp;, and ,&nbsp;Prabal K. Maiti,&nbsp;","doi":"10.1021/acs.jpcc.5c07253","DOIUrl":"10.1021/acs.jpcc.5c07253","url":null,"abstract":"<p >Ensuring the stability of the AuNP-gene complex until it reaches the target sites is a crucial factor for the success of gene therapy. Although different AuNP sizes and AuNP-to-DNA ratios are investigated for specific therapeutic needs, their role in the stability and packaging of AuNP-DNA complex remains unclear. In this study, we employ all-atom molecular dynamics simulations to investigate the influence of cationic ligand-functionalized AuNP (CAuNP) size and CAuNP-to-DNA ratio on DNA wrapping and binding affinity. The obtained results show that a single DNA interacting with smaller CAuNPs exhibits greater bending and wrapping due to their higher curvature. However, when two DNAs bind to smaller CAuNPs, electrostatic repulsion prevents the effective wrapping, which leads the DNAs to twist from their original orientation. Such behavior is not observed with larger CAuNPs since their increased size may mitigate repulsive forces. Further, the analysis on axial bending angle reveals that smaller AuNPs induce sharper DNA bending and larger AuNPs promote smoother bending. In addition, the potential of mean force (PMF) analysis confirms a stronger DNA binding affinity for larger AuNPs, with affinity decreasing when two DNAs attach to a single CAuNP. Our results from the DNA loading capacity calculations provide insights into the maximum number of DNA molecules that can be loaded onto CAuNPs of a given size. These findings offer key insights into optimizing the size of AuNP and DNA-to-AuNP ratios for the development of efficient gene delivery systems.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2360–2374"},"PeriodicalIF":3.2,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Catalytic Capability of Graphene/Cu Heterostructures for Oxygen Evolution Reaction Activated by the Synergistic Effect of Defects and Strain 石墨烯/Cu异质结构在缺陷和应变协同作用下催化析氧反应的性能
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1021/acs.jpcc.5c04627
Jing Xu, , , Wanlin Guo, , and , Yufeng Guo*, 

Developing catalysts based on graphene heterostructures is an attractive aspect for advancing the application of graphene. Our extensive first-principles calculations and ab initio molecular dynamics simulations reveal that the catalytic capability of graphene/Cu heterostructures for the electrochemical oxygen evolution reaction (OER) can be activated and significantly enhanced by the synergistic effect of introducing Stone–Wales (SW) defects into graphene and applying biaxial compressive strains to the heterostructures. The overpotential of the SW-defected graphene/Cu heterostructure for the OER decreases to 0.39 V under a biaxial compressive strain of −3%, which is lower than most theoretical overpotentials obtained when using graphene heterostructures as catalysts. The alteration and improvement in the catalytic capability of SW-defected graphene/Cu heterostructures under compressive strains are mainly attributed to the facilitated desorption of intermediates on graphene, the decreased reaction activation energy, and the charge transfer from the SW defect sites to the Cu substrates.

开发基于石墨烯异质结构的催化剂是推进石墨烯应用的一个有吸引力的方面。我们广泛的第一性原理计算和从头算分子动力学模拟表明,石墨烯/Cu异质结构对电化学析氧反应(OER)的催化能力可以通过在石墨烯中引入Stone-Wales (SW)缺陷和在异质结构上施加双轴压缩应变的协同效应被激活并显著增强。在- 3%的双轴压缩应变下,sw缺陷的石墨烯/Cu异质结构对OER的过电位降至0.39 V,低于使用石墨烯异质结构作为催化剂时获得的大多数理论过电位。SW缺陷石墨烯/Cu异质结构在压缩应变下催化性能的改变和提高主要是由于中间产物在石墨烯上的脱附、反应活化能的降低以及SW缺陷部位的电荷向Cu基体的转移。
{"title":"Catalytic Capability of Graphene/Cu Heterostructures for Oxygen Evolution Reaction Activated by the Synergistic Effect of Defects and Strain","authors":"Jing Xu,&nbsp;, ,&nbsp;Wanlin Guo,&nbsp;, and ,&nbsp;Yufeng Guo*,&nbsp;","doi":"10.1021/acs.jpcc.5c04627","DOIUrl":"10.1021/acs.jpcc.5c04627","url":null,"abstract":"<p >Developing catalysts based on graphene heterostructures is an attractive aspect for advancing the application of graphene. Our extensive first-principles calculations and <i>ab initio</i> molecular dynamics simulations reveal that the catalytic capability of graphene/Cu heterostructures for the electrochemical oxygen evolution reaction (OER) can be activated and significantly enhanced by the synergistic effect of introducing Stone–Wales (SW) defects into graphene and applying biaxial compressive strains to the heterostructures. The overpotential of the SW-defected graphene/Cu heterostructure for the OER decreases to 0.39 V under a biaxial compressive strain of −3%, which is lower than most theoretical overpotentials obtained when using graphene heterostructures as catalysts. The alteration and improvement in the catalytic capability of SW-defected graphene/Cu heterostructures under compressive strains are mainly attributed to the facilitated desorption of intermediates on graphene, the decreased reaction activation energy, and the charge transfer from the SW defect sites to the Cu substrates.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2139–2147"},"PeriodicalIF":3.2,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Scandia as the Oxygen Vacancy Stabilizer to Boost the Ionic Conductivity of Sc–Y-Codoped Zirconia 钪作为氧空位稳定剂提高sc - y共掺杂氧化锆的离子电导率
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1021/acs.jpcc.5c08205
Shu-Hui Guan, , , Yi-Wen Wei, , , Cheng Shang*, , and , Zhi-Pan Liu*, 

Scandia (Sc) and yttria (Y) codoped zirconia (ScYSZ) emerged as a promising candidate for high-performance solid electrolyte materials utilized in intermediate-temperature solid oxide fuel cells (IT-SOFCs). While it exhibits a record-high ionic conductivity (∼0.10 S/cm at 800 °C), the physical origin of the superior performance remains poorly understood, limiting the further optimization and the application in IT-SOFC. Here, we construct the Sc–Y–Zr–O global neural network potential and explore systematically the thermodynamic landscape of ScYSZ across 65 different compositions (6.7–14.3 mol % dopants). From millions of candidate structures, we identify a thermodynamically stable cubic phase region at Sc/Y < 1 with Y2O3 ≥ 8 mol %. Large-scale molecular dynamics simulations further show that ScYSZ at Sc2O3 = 3 mol % and Y2O3 = 8 mol % yields an exceptional ionic conductivity of 0.13 S/cm at 800 °C, surpassing conventional 8 mol % Y-stabilized zirconia (YSZ) by an order of magnitude. Our analysis reveals that the presence of Sc not only increases the Ov concentration by allowing ⟨111⟩ Ov–Ov pairs but also reduces the oxygen migration barriers markedly. Our results not only pinpoint the optimal ScYSZ composition for IT-SOFC applications theoretically but also establish a general framework for the rational design of advanced solid electrolyte materials.

钪(Sc)和氧化钇(Y)共掺杂氧化锆(ScYSZ)是中温固体氧化物燃料电池(IT-SOFCs)中高性能固体电解质材料,具有广阔的应用前景。虽然它表现出创纪录的高离子电导率(在800°C时为~ 0.10 S/cm),但优异性能的物理来源仍然知之甚少,限制了进一步的优化和在it - sofc中的应用。在此,我们构建了Sc-Y-Zr-O全局神经网络电位,并系统地探索了65种不同成分(6.7-14.3 mol %掺杂剂)下ScYSZ的热力学景观。从数以百万计的候选结构中,我们确定了Sc/Y <; 1的热力学稳定的立方相区域,Y2O3≥8mol %。大规模分子动力学模拟进一步表明,ScYSZ在Sc2O3 = 3 mol %和Y2O3 = 8 mol %时,在800°C时的离子电导率为0.13 S/cm,比传统的8 mol % y稳定氧化锆(YSZ)高出一个数量级。我们的分析表明,Sc的存在不仅通过允许⟨111⟩的Ov - Ov对增加Ov浓度,而且还显着降低了氧迁移障碍。我们的研究结果不仅从理论上确定了IT-SOFC应用的最佳ScYSZ成分,而且为合理设计先进的固体电解质材料建立了一个总体框架。
{"title":"Scandia as the Oxygen Vacancy Stabilizer to Boost the Ionic Conductivity of Sc–Y-Codoped Zirconia","authors":"Shu-Hui Guan,&nbsp;, ,&nbsp;Yi-Wen Wei,&nbsp;, ,&nbsp;Cheng Shang*,&nbsp;, and ,&nbsp;Zhi-Pan Liu*,&nbsp;","doi":"10.1021/acs.jpcc.5c08205","DOIUrl":"10.1021/acs.jpcc.5c08205","url":null,"abstract":"<p >Scandia (Sc) and yttria (Y) codoped zirconia (ScYSZ) emerged as a promising candidate for high-performance solid electrolyte materials utilized in intermediate-temperature solid oxide fuel cells (IT-SOFCs). While it exhibits a record-high ionic conductivity (∼0.10 S/cm at 800 °C), the physical origin of the superior performance remains poorly understood, limiting the further optimization and the application in IT-SOFC. Here, we construct the Sc–Y–Zr–O global neural network potential and explore systematically the thermodynamic landscape of ScYSZ across 65 different compositions (6.7–14.3 mol % dopants). From millions of candidate structures, we identify a thermodynamically stable cubic phase region at Sc/Y &lt; 1 with Y<sub>2</sub>O<sub>3</sub> ≥ 8 mol %. Large-scale molecular dynamics simulations further show that ScYSZ at Sc<sub>2</sub>O<sub>3</sub> = 3 mol % and Y<sub>2</sub>O<sub>3</sub> = 8 mol % yields an exceptional ionic conductivity of 0.13 S/cm at 800 °C, surpassing conventional 8 mol % Y-stabilized zirconia (YSZ) by an order of magnitude. Our analysis reveals that the presence of Sc not only increases the O<sub>v</sub> concentration by allowing ⟨111⟩ O<sub>v</sub>–O<sub>v</sub> pairs but also reduces the oxygen migration barriers markedly. Our results not only pinpoint the optimal ScYSZ composition for IT-SOFC applications theoretically but also establish a general framework for the rational design of advanced solid electrolyte materials.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2129–2138"},"PeriodicalIF":3.2,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
How Artificial Intelligence Can Advance Electrochemical Science and Identify Water Molecule Orientation on Platinum Electrodes 人工智能如何推进电化学科学和识别铂电极上的水分子取向
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1021/acs.jpcc.5c08343
Yitao He*,  and , Jiří Červenka*, 

Electrochemistry lies at the heart of modern energy technologies, yet connecting atomic-level insights to macroscopic performance remains an enduring challenge. Quantum-based simulations, such as density functional theory, have illuminated many fundamental processes, but their reach is limited by the complexity of real electrochemical environments. Bridging these scales requires a new conceptual framework that can expose the hidden connections between theory and experiment. Here, we argue that the thoughtful integration of artificial intelligence (AI) can transform electrochemical research by unifying theory, experiment, and data-driven inference. AI-assisted frameworks can accelerate convergence between computation and experiment, revealing hidden physical relationships and enabling closed-loop discovery. Realizing this vision will require developing transparent, interpretable AI models that earn the same scientific trust as human reasoning, unlocking deeper understanding and innovation across the electrochemical sciences.

电化学是现代能源技术的核心,但将原子水平的见解与宏观性能联系起来仍然是一个持久的挑战。基于量子的模拟,如密度泛函理论,已经阐明了许多基本过程,但它们的范围受到实际电化学环境的复杂性的限制。弥合这些尺度需要一个新的概念框架,可以揭示理论和实验之间隐藏的联系。在这里,我们认为人工智能(AI)的深思熟虑的整合可以通过统一理论,实验和数据驱动的推理来改变电化学研究。人工智能辅助框架可以加速计算和实验之间的融合,揭示隐藏的物理关系,实现闭环发现。实现这一愿景需要开发透明、可解释的人工智能模型,以获得与人类推理相同的科学信任,从而在电化学科学中开启更深层次的理解和创新。
{"title":"How Artificial Intelligence Can Advance Electrochemical Science and Identify Water Molecule Orientation on Platinum Electrodes","authors":"Yitao He*,&nbsp; and ,&nbsp;Jiří Červenka*,&nbsp;","doi":"10.1021/acs.jpcc.5c08343","DOIUrl":"10.1021/acs.jpcc.5c08343","url":null,"abstract":"<p >Electrochemistry lies at the heart of modern energy technologies, yet connecting atomic-level insights to macroscopic performance remains an enduring challenge. Quantum-based simulations, such as density functional theory, have illuminated many fundamental processes, but their reach is limited by the complexity of real electrochemical environments. Bridging these scales requires a new conceptual framework that can expose the hidden connections between theory and experiment. Here, we argue that the thoughtful integration of artificial intelligence (AI) can transform electrochemical research by unifying theory, experiment, and data-driven inference. AI-assisted frameworks can accelerate convergence between computation and experiment, revealing hidden physical relationships and enabling closed-loop discovery. Realizing this vision will require developing transparent, interpretable AI models that earn the same scientific trust as human reasoning, unlocking deeper understanding and innovation across the electrochemical sciences.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2082–2090"},"PeriodicalIF":3.2,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpcc.5c08343","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056993","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optical Reflection of Crystals of Dye Molecules and Strong Coupling between Light and Matter 染料分子晶体的光学反射与光与物质的强耦合
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1021/acs.jpcc.5c08141
Rens Cuijpers, , , Wietse F. M. van Geel, , , Dorothée S. Mader, , , K. Danique Grevink, , , Matthijs van Velzen, , , Martin Lutz, , and , Stefan C. J. Meskers*, 

Materials consisting of organic dye molecules play an important role as pigments, as active layer in organic light emitting diodes or solar cells, and as bistable medium in optical transistors and switches. Yet there is currently no working protocol to accurately predict one of the most basic optical properties of these solids: their reflection spectrum. Here we develop a method to calculate the reflection spectrum of crystals of dye molecules based on the crystal structure and optical absorption of the dye in solution. We treat the interaction between light and matter in the crystals as strong. Electromagnetic four-potentials are gauged consistently, and their boundary conditions at the reflecting interface are derived. Finally, we include both excitonic and charge transfer interactions between molecules in the crystals. We test our approach on a large data set of reflection spectra and crystal structures including several industrial pigments.

由有机染料分子组成的材料在有机发光二极管或太阳能电池中起着颜料、有源层、光晶体管和开关中的双稳介质等重要作用。然而,目前还没有可行的方案来准确预测这些固体最基本的光学性质之一:它们的反射光谱。本文提出了一种基于晶体结构和染料在溶液中的光吸收来计算染料分子晶体反射光谱的方法。我们认为晶体中光与物质之间的相互作用很强。对电磁四势进行了一致性测量,并推导了其在反射界面处的边界条件。最后,我们将晶体中分子之间的激子相互作用和电荷转移相互作用都包括在内。我们在包括几种工业颜料的反射光谱和晶体结构的大型数据集上测试了我们的方法。
{"title":"Optical Reflection of Crystals of Dye Molecules and Strong Coupling between Light and Matter","authors":"Rens Cuijpers,&nbsp;, ,&nbsp;Wietse F. M. van Geel,&nbsp;, ,&nbsp;Dorothée S. Mader,&nbsp;, ,&nbsp;K. Danique Grevink,&nbsp;, ,&nbsp;Matthijs van Velzen,&nbsp;, ,&nbsp;Martin Lutz,&nbsp;, and ,&nbsp;Stefan C. J. Meskers*,&nbsp;","doi":"10.1021/acs.jpcc.5c08141","DOIUrl":"10.1021/acs.jpcc.5c08141","url":null,"abstract":"<p >Materials consisting of organic dye molecules play an important role as pigments, as active layer in organic light emitting diodes or solar cells, and as bistable medium in optical transistors and switches. Yet there is currently no working protocol to accurately predict one of the most basic optical properties of these solids: their reflection spectrum. Here we develop a method to calculate the reflection spectrum of crystals of dye molecules based on the crystal structure and optical absorption of the dye in solution. We treat the interaction between light and matter in the crystals as strong. Electromagnetic four-potentials are gauged consistently, and their boundary conditions at the reflecting interface are derived. Finally, we include both excitonic and charge transfer interactions between molecules in the crystals. We test our approach on a large data set of reflection spectra and crystal structures including several industrial pigments.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2255–2265"},"PeriodicalIF":3.2,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Compression Rate Dependence and Hierarchical Mechanism in the Pressure-Induced Polymerization of Acrylamide: Insights from Ab Initio Molecular Dynamics 压力诱导丙烯酰胺聚合的压缩率依赖性和层次机制:从头算分子动力学的见解
IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1021/acs.jpcc.5c06506
Rashid Rafeek V Valappil, , , Sayan Maity, , , Ashwini Anshu, , , Lavanya M. Ramaniah*, , and , Varadharajan Srinivasan*, 

Varying the rate at which pressure is applied to a crystal is known to yield different pressure-induced polymorphic structures in experiments. In this work, we investigate the effect of pressure increase rate on pressure-induced polymerization in crystalline acrylamide, using room temperature constant pressure ab initio molecular dynamics simulations. Simulations performed with two different compression rates revealed very different structural evolutions of the system at lower pressures. Fast (nonequilibrated) pressure increase yields disordered (polymer) structures with unanticipated linkages for pressures up to 67 GPa. On the other hand, slow (quasi-static) pressure increase gives no new structures until 64 GPa. At pressures greater than 67 GPa, both pathways converge toward an ordered 3-dimensional polymer through a hierarchical mechanism involving 1-dimensional polymeric intermediates. The structural and electronic details of the mechanisms leading to polymerization are discussed.

在实验中,已知改变施加于晶体的压力速率会产生不同的压力诱导的多晶结构。在这项工作中,我们研究了压力增加速率对结晶丙烯酰胺压力诱导聚合的影响,采用室温恒压从头算分子动力学模拟。用两种不同的压缩率进行的模拟显示,在较低压力下,系统的结构演变非常不同。当压力高达67gpa时,快速(非平衡)的压力增加会产生无序(聚合物)结构,并产生意想不到的联系。另一方面,缓慢的(准静态)压力增加在64 GPa之前不会产生新的结构。在大于67 GPa的压力下,这两种途径通过涉及一维聚合物中间体的分层机制向有序的三维聚合物收敛。讨论了聚合机理的结构和电子细节。
{"title":"Compression Rate Dependence and Hierarchical Mechanism in the Pressure-Induced Polymerization of Acrylamide: Insights from Ab Initio Molecular Dynamics","authors":"Rashid Rafeek V Valappil,&nbsp;, ,&nbsp;Sayan Maity,&nbsp;, ,&nbsp;Ashwini Anshu,&nbsp;, ,&nbsp;Lavanya M. Ramaniah*,&nbsp;, and ,&nbsp;Varadharajan Srinivasan*,&nbsp;","doi":"10.1021/acs.jpcc.5c06506","DOIUrl":"10.1021/acs.jpcc.5c06506","url":null,"abstract":"<p >Varying the rate at which pressure is applied to a crystal is known to yield different pressure-induced polymorphic structures in experiments. In this work, we investigate the effect of pressure increase rate on pressure-induced polymerization in crystalline acrylamide, using room temperature constant pressure <i>ab initio</i> molecular dynamics simulations. Simulations performed with two different compression rates revealed very different structural evolutions of the system at lower pressures. Fast (nonequilibrated) pressure increase yields disordered (polymer) structures with unanticipated linkages for pressures up to 67 GPa. On the other hand, slow (quasi-static) pressure increase gives no new structures until 64 GPa. At pressures greater than 67 GPa, both pathways converge toward an ordered 3-dimensional polymer through a hierarchical mechanism involving 1-dimensional polymeric intermediates. The structural and electronic details of the mechanisms leading to polymerization are discussed.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 6","pages":"2316–2326"},"PeriodicalIF":3.2,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070603","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
The Journal of Physical Chemistry C
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1