Journal of Chemical Physics最新文献_第3页

Detecting vibronic excitations of individual pentagon defects with S = 1/2 spin states in graphene nanoribbons. 石墨烯纳米带中S = 1/2自旋态五边形缺陷的振动激发检测。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-14 DOI: 10.1063/5.0297985

Xiaoqing Wang, Xinyong Meng, Ruoting Yin, Yifan Liang, Bin Li, Wei Hu, Qitang Fan, Shijing Tan, Chuanxu Ma, Jinlong Yang, Bing Wang

{"title":"Detecting vibronic excitations of individual pentagon defects with S = 1/2 spin states in graphene nanoribbons.","authors":"Xiaoqing Wang, Xinyong Meng, Ruoting Yin, Yifan Liang, Bin Li, Wei Hu, Qitang Fan, Shijing Tan, Chuanxu Ma, Jinlong Yang, Bing Wang","doi":"10.1063/5.0297985","DOIUrl":"https://doi.org/10.1063/5.0297985","url":null,"abstract":"Non-hexagonal rings represent an important type of topological defects to tailor the electronic, magnetic, and vibrational properties in graphene-based nanomaterials. Despite recent advances of on-surface synthesis, there is still lack of an effective approach to create individual non-hexagonal defects with an open-shell feature in graphene nanoribbons (GNRs) and to decouple the non-hexagons from the metal surfaces for investigating the intrinsic properties. Here, we report an on-surface approach that combines thermally triggered reactions and tip-assisted manipulations to achieve decoupled individual pentagons in bilayer GNR crosses on Au(111) surface. By combining scanning tunneling microscopy/spectroscopy (STM/STS) with non-contact atomic force microscopy (nc-AFM), we can confirm the pentagonal structures with single-bond resolution and the open-shell character with S = 1/2 from the Kondo resonance in on-surface synthesized topological GNRs. By utilizing the tip-assisted manipulation, we construct the bilayer GNR cross with the methyl-group sandwiched individual pentagon on top of a pristine all-hexagonal GNR segment, which effectively decouples the pentagon from the metallic surface. The open-shell nature of the single pentagon defect can be directly confirmed by the presence of well-defined singly occupied and unoccupied molecular orbitals (SOMO and SUMO), supported by first-principles calculations. Benefiting from the decoupled nature, we also observe vibronic peaks associated with the resonant electron tunneling into SOMO and SUMO, which can be well attributed to the vibrational excitations of the local D and D' modes in defective graphene. These findings demonstrate a versatile manner to explore the intrinsic electronic, vibrational, and magnetic properties of individual defects in graphene nanostructures.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 14","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145274718","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

Seniority-zero states are mean-field wavefunctions. 资历为零的状态是平均场波函数。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-14 DOI: 10.1063/5.0296924

Marco Martínez González, Daniel F Calero-Osorio, Michelle Richer, Cassandra Masschelein, Shuoyang Wang, Paul A Johnson, Stijn De Baerdemacker, Paul W Ayers

引用次数: 0

Real-time dynamics with bead-Fourier path integrals. I. Bead-Fourier CMD. 实时动态与头-傅立叶路径积分。1 .珠-傅里叶CMD。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-14 DOI: 10.1063/5.0278955

Nathan London, Mohammad R Momeni

{"title":"Real-time dynamics with bead-Fourier path integrals. I. Bead-Fourier CMD.","authors":"Nathan London, Mohammad R Momeni","doi":"10.1063/5.0278955","DOIUrl":"https://doi.org/10.1063/5.0278955","url":null,"abstract":"Developing new methods for the accurate and efficient calculations of real-time quantum correlation functions is deemed one of the most challenging problems of modern condensed matter theory. Many popular methods, such as centroid molecular dynamics (CMD), make use of Feynman path integrals (PIs) to efficiently introduce nuclear quantum effects into classical dynamical simulations. Conventional CMD methods use the discretized form of the PI formalism to represent a quantum particle using a series of replicas, or \"beads,\" connected with harmonic springs to create an imaginary time ring polymer. The alternative Fourier PI methodology, instead, represents the imaginary time path using a Fourier sine series. Presented as an intermediary between the two formalisms, bead-Fourier PIs (BF-PIs) have been shown to reduce the number of beads needed to converge equilibrium properties by including a few terms of the Fourier series. Here, a new CMD method is presented where the effective potential is calculated using BF-PIs as opposed to the typical bead PIs. We demonstrate the accuracy and efficiency of this new BF-CMD method for a series of 1D model systems and show that at low temperatures, one can achieve between a fourfold and eightfold reduction in the number of beads with the addition of a single Fourier component. The developed methodology is general and can be extended to other closely related methods, such as ring polymer molecular dynamics, as well as non-adiabatic PI methods.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 14","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145280419","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

Unique proton transfer and hydrogen evolution reaction at semi-disordered interfaces in confined spaces. 在受限空间半无序界面上独特的质子转移和析氢反应。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-14 DOI: 10.1063/5.0288299

Shu-Qiang He, Mao Su, Chenyu Tang, Yi-Feng Zheng, Si-Yan Gao, Haiping Fang, Yue-Yu Zhang

{"title":"Unique proton transfer and hydrogen evolution reaction at semi-disordered interfaces in confined spaces.","authors":"Shu-Qiang He, Mao Su, Chenyu Tang, Yi-Feng Zheng, Si-Yan Gao, Haiping Fang, Yue-Yu Zhang","doi":"10.1063/5.0288299","DOIUrl":"https://doi.org/10.1063/5.0288299","url":null,"abstract":"Nanoconfinement effect holds significant research implications across multiple disciplines, with interfacial interactions-particularly at solid-water interfaces-playing a central role in the field of confined spaces. The semi-disordered nature of solid-liquid interfaces under confinement critically influences various dynamic processes, such as crystallization, electrochemistry, and catalysis. Building on these insights, we employed ab initio molecular dynamics simulations to systematically investigate interfacial reactions in graphene-confined environments, with a focus on the water-CaCl semi-disordered interface to elucidate the underlying atomic-scale mechanisms. In particular, the non-uniform electronic density distribution at the CaCl semi-disordered interface governs the spatial arrangement, structural ordering, and stability of interfacial water molecules. Furthermore, our simulations revealed that strong Coulomb interactions drive pronounced proton transfer and peculiar hydrogen evolution reactions at the interface. Finally, combining machine learning techniques, we developed a set of potential functions with density functional theory accuracy to describe Ca-Cl systems with unconventional stoichiometry. These functions will support in-depth research on Ca-Cl systems with unconventional stoichiometry. These findings provide fundamental insights into interfacial phenomena under confinement and offer critical implications for the design of energy storage systems, batteries, and iontronic devices.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 14","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145286357","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

Spectral diffusion of single Ag-In-Zn-S quantum dots elucidates the photoluminescence mechanism. 单个Ag-In-Zn-S量子点的光谱扩散阐明了其光致发光机理。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0290296

Adam Ćwilich, Patrycja Kowalik, Karolina Sulowska, Pushkar Joshi, Piotr Bujak, Sebastian Maćkowski, Adam Pron, Łukasz Kłopotowski

{"title":"Spectral diffusion of single Ag-In-Zn-S quantum dots elucidates the photoluminescence mechanism.","authors":"Adam Ćwilich, Patrycja Kowalik, Karolina Sulowska, Pushkar Joshi, Piotr Bujak, Sebastian Maćkowski, Adam Pron, Łukasz Kłopotowski","doi":"10.1063/5.0290296","DOIUrl":"https://doi.org/10.1063/5.0290296","url":null,"abstract":"Alloyed Ag-In-Zn-S colloidal quantum dots (QDs) have recently emerged as bright fluorophores with properties compatible with various applications. Although the synthetic procedures are well developed and allow achieving near-unity photoluminescence quantum yields, further development of these nanostructures is hindered by poor understanding of the light emission mechanism. In this work, we employ a tool of single particle spectroscopy-studies of spectral diffusion-to elucidate the nature of the luminescent excited state. By analyzing temporal fluctuations and correlations of the photoluminescence intensity, peak position, and linewidth, we show that this state comprises an electron delocalized over the QD volume and a hole localized at a midgap trap state. We thus challenge the view prevailing in the literature that the photoluminescence in alloyed Ag-In-Zn-S QDs occurs via a donor-acceptor pair recombination mechanism. Furthermore, our single dot measurements reveal various contributions to the photoluminescence line broadening.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 13","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145238632","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

Understanding the heterogeneous nucleation of ice on silver iodide using deep potential molecular dynamics. 用深势分子动力学研究碘化银上冰的非均相成核。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0288279

Yaochen Yu, Haiyang Niu

{"title":"Understanding the heterogeneous nucleation of ice on silver iodide using deep potential molecular dynamics.","authors":"Yaochen Yu, Haiyang Niu","doi":"10.1063/5.0288279","DOIUrl":"https://doi.org/10.1063/5.0288279","url":null,"abstract":"Ice nucleation is one of the most unique and widespread phase transitions on Earth. Due to the relatively low phase transition energy barrier to overcome and the ubiquitous existence of foreign substrates, ice nucleation primarily occurs heterogeneously in nature. Despite extensive studies, our understanding of the molecular-scale heterogeneous nucleation process under the influence of silver iodide (AgI) substrate interactions, one of the most efficient ice nucleating agents, remains limited. Using a deep neural network potential, we perform molecular dynamics simulations with ab initio accuracy to investigate the heterogeneous nucleation of ice on AgI. By analyzing the free energy surface of water molecules at the AgI-water interface, we systematically elucidate the mechanism behind the formation of an ice-like hexagonal layer on AgI. The reconstruction of the metastable, disordered hydrogen bond network into this ice-like hexagonal layer facilitates ice nucleation and contributes to the asynchronous crystallization manner. Furthermore, we find that the influence of the AgI substrate propagates through the highly dynamical and collaborative hydrogen bond network, leading to a pre-ordered region at the ice-water interface that reduces the ice growth rate to approximately one-third compared to ice homogeneous nucleation conditions. These findings provide new insights into the early stages of ice heterogeneous nucleation on the AgI surface and expand our understanding of the role substrates play in this process.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 13","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145232795","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

Conformation-specific reactions of Criegee intermediates. Criegee中间体的构象特异性反应。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0278251

Chen-An Chung, Tang-Yu Kao, Yuan-Pern Lee

引用次数: 0

Interfacial charge transfer and oxygen activation in phosphorus-doped g-C3N4/MoS2 quantum dot heterostructures: A first-principles and photocatalytic study. 磷掺杂g-C3N4/MoS2量子点异质结构的界面电荷转移和氧活化：第一性原理和光催化研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0293379

Tianzhu Yu, Zhaoxiong Yan, Changle Li, Xianfeng Yang, Mei Jin, Zhihua Xu

{"title":"Interfacial charge transfer and oxygen activation in phosphorus-doped g-C3N4/MoS2 quantum dot heterostructures: A first-principles and photocatalytic study.","authors":"Tianzhu Yu, Zhaoxiong Yan, Changle Li, Xianfeng Yang, Mei Jin, Zhihua Xu","doi":"10.1063/5.0293379","DOIUrl":"https://doi.org/10.1063/5.0293379","url":null,"abstract":"A phosphorus-doped graphitic carbon nitride (PCN)/MoS2 quantum dots (QDs) heterostructure was synthesized via an evaporation-induced self-assembly process. X-ray photoelectron spectroscopy and work function analysis revealed strong interfacial electronic interactions. Density functional theory calculations indicated that interfacial charge migration was dominated by a diffusion-driven mechanism. Incorporation of MoS2 QDs modulated the electronic structure of PCN, significantly enhancing O2 adsorption and promoting the generation of reactive oxygen species (1O2 and ·O2-) under simulated solar irradiation. These electronic modifications improved the photocatalytic response, as demonstrated by the enhanced degradation of Rhodamine B and tetracycline (TC), with pollutant removal efficiencies of 99.5% and 90.0%, respectively, substantially exceeding those of pristine PCN. Application to real printing and dyeing wastewater demonstrated the material's practical potential, with the degradation products of TC exhibiting substantially reduced biotoxicity to aquatic organisms. This study provides mechanistic insights into charge transport and interfacial oxygen activation in g-C3N4-based heterostructures, offering a rational strategy for the design of advanced photocatalysts for solar-driven environmental remediation.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 13","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145238708","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

Self-assembled hemimicelles of perfluoroalkylalkanes: How chain length, shape, and dipole determine internal structure. A new (geometrical + electrostatic) model. 全氟烷基烷烃的自组装半束：链长、形状和偶极子如何决定内部结构。一个新的（几何+静电）模型。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0291300

Pedro Silva, Gonçalo M C Silva, Pedro Morgado, Marie-Claude Fauré, Michel Goldmann, Eduardo J M Filipe

{"title":"Self-assembled hemimicelles of perfluoroalkylalkanes: How chain length, shape, and dipole determine internal structure. A new (geometrical + electrostatic) model.","authors":"Pedro Silva, Gonçalo M C Silva, Pedro Morgado, Marie-Claude Fauré, Michel Goldmann, Eduardo J M Filipe","doi":"10.1063/5.0291300","DOIUrl":"https://doi.org/10.1063/5.0291300","url":null,"abstract":"Perfluoroalkylalkanes form nanostructured Langmuir films comprising discrete surface aggregates or hemimicelles. The aggregates are formed by a large number of molecules (∼2000-3000), are highly monodisperse and round-shaped, and display a characteristic pit in their center. In this study, the influence of the hydrogenated and the perfluorinated chain lengths on the size of the hemimicelles was probed by a systematic atomistic molecular dynamics simulation study and further rationalized in terms of a model that describes the internal structure of the hemimicelles. The model, while set on geometrical considerations, was developed using quantitative information obtained from the molecular dynamics simulations performed using an atomistic force field that includes detailed electrostatic and dispersive intramolecular and intermolecular interactions. These interactions are therefore intrinsically incorporated in the model, which is consequently designated geometrical + electrostatic (G+E model). Eleven PFAA molecules (F8Hm: F8H14, F8H16, F8H18, F8H20; FnH16: F6H16, F8H16, F10H16, F12H16; F10Hm: F10H14, F10H18, F10H20) and the corresponding hemimicelles were studied, covering a representative range of molecular structures. The results of both the molecular dynamics simulations and the new model reproduce the available experimental data within the respective uncertainties. The results provide a rational basis for a complete understanding of the self-assembly process of PFAA molecules into discrete hemimicelles, well-founded in physical principles and molecular properties.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 13","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145232724","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

Practical considerations for accurate estimation of diffusion parameters from single-particle tracking in living cells. 从活细胞中单粒子跟踪准确估计扩散参数的实际考虑。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-10-07 DOI: 10.1063/5.0284172

Aishani Ghosal, Yu-Huan Wang, Nguyen Nguyen, Laura Troyer, Sangjin Kim

{"title":"Practical considerations for accurate estimation of diffusion parameters from single-particle tracking in living cells.","authors":"Aishani Ghosal, Yu-Huan Wang, Nguyen Nguyen, Laura Troyer, Sangjin Kim","doi":"10.1063/5.0284172","DOIUrl":"10.1063/5.0284172","url":null,"abstract":"Advances in fluorescence microscopy have enabled high-resolution tracking of individual biomolecules in living cells. However, accurate estimation of diffusion parameters from single-particle trajectories remains challenging due to static and dynamic localization errors inherent in these measurements. While previous studies have characterized how such errors affect mean-squared displacement (MSD) analysis, practical guidelines for minimizing them during data acquisition and correcting them during analysis are still lacking. Here, we combine theoretical modeling and simulations to evaluate how exposure time and sampling rate influence the accuracy of MSD-based inference under fractional Brownian motion (FBM), a canonical model of anomalous diffusion. We demonstrate that decoupling exposure and sampling times enables escape from the error-prone regime, thus improving inference accuracy, and that incorporating an offset in nonlinear MSD fitting substantially improves the estimation of the anomalous diffusion exponent. We validate this framework using trajectories of cytoplasmic particles in Escherichia coli, recovering consistent diffusion parameters across multiple datasets. We further prove that the framework extends beyond FBM to general cases of subdiffusion, thereby offering practical strategies to improve both experimental design and data analysis in single-particle tracking of live or synthetic systems.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 13","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145232784","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