Journal of Chemical Physics最新文献_第2页

Water under hydrophobic confinement: entropy and diffusion. 疏水约束下的水：熵和扩散。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0264812

Lorenzo Agosta, Yong Wang, Kersti Hermansson, Mikhail Dzugutov

引用次数: 0

Thermal properties of Na2CO3-NaCl-KCl ternary eutectic salt for high-temperature thermal energy storage: Experimental and deep potential molecular dynamics combined. 高温储热用Na2CO3-NaCl-KCl三元共晶盐的热性能：实验与深势分子动力学相结合。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0281150

Heqing Tian, Tianyu Liu, Wenguang Zhang

{"title":"Thermal properties of Na2CO3-NaCl-KCl ternary eutectic salt for high-temperature thermal energy storage: Experimental and deep potential molecular dynamics combined.","authors":"Heqing Tian, Tianyu Liu, Wenguang Zhang","doi":"10.1063/5.0281150","DOIUrl":"https://doi.org/10.1063/5.0281150","url":null,"abstract":"With the global energy structure transitioning toward decarbonization, molten salts serve as critical media for efficient thermal energy storage and transfer in large-scale utilization of renewable energy. However, the experimental measurements of the thermal properties of high-temperature molten salts suffer severe obstacles due to their strong corrosiveness and toxicity, necessitating high-precision multiscale predictive models. This study focuses on the Na2CO3-NaCl-KCl ternary eutectic molten salt system, integrating experimental measurement with deep potential molecular dynamics simulation to systematically investigate its high-temperature thermal properties. The experimental results show that the melting point, enthalpy of fusion, and specific heat capacity of ternary eutectic salt is 852.65 K, 392.00 J/g, and 1.268 J/(g K), respectively, indicating the outstanding heat storage capacity. Initial datasets generated from first-principle molecular dynamics are optimized using the DP-GEN enhanced sampling strategy, and the simulation results reveal that the density decreased from 1.776 g/cm3 (873 K) to 1.690 g/cm3 (1073 K), with a maximum deviation of 2.68% compared to experimental data. The specific heat capacity is 1.276 J/(g K), exhibiting a negligible error of 0.63% against experimental values. Viscosity declined from 3.117 mPa s (873 K) to 1.755 mPa s (1073 K), consistent with the Stokes-Einstein relationship, while thermal conductivity slightly decreased with rising temperature. This study validates the high accuracy and reliability of the DP model in predicting thermal properties of molten salt and provides theoretical insights for material design and operational optimization of high-temperature molten salt thermal energy storage systems.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144955308","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

Ab initio study of electromigration in liquid GeAsSe alloys for selector devices. 选择器用液态GeAsSe合金电迁移的从头算研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0280879

Matteo Cobelli, Dario Baratella, Paolo Fantini, Marco Bernasconi

引用次数: 0

Developing a neural network machine learning interatomic potential for molecular dynamics simulations of La-Si-P systems. 开发用于La-Si-P系统分子动力学模拟的神经网络机器学习原子间势。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0284672

Ling Tang, Weiyi Xia, Gayatri Viswanathan, Ernesto Soto, Kirill Kovnir, Cai-Zhuang Wang

{"title":"Developing a neural network machine learning interatomic potential for molecular dynamics simulations of La-Si-P systems.","authors":"Ling Tang, Weiyi Xia, Gayatri Viswanathan, Ernesto Soto, Kirill Kovnir, Cai-Zhuang Wang","doi":"10.1063/5.0284672","DOIUrl":"https://doi.org/10.1063/5.0284672","url":null,"abstract":"While molecular dynamics (MD) is a very useful computational method for atomistic simulations, modeling the interatomic interactions for reliable MD simulations of real materials has been a long-standing challenge. In 2007, Behler and Parrinello first proposed and demonstrated an artificial neural network machine learning (ANN-ML) scheme, opening a new paradigm for developing accurate and efficient interatomic potentials for reliable MD simulation studies of the thermodynamics and kinetics of materials. In this paper, we show that an accurate and transferable ANN-ML interatomic potential can be developed for MD simulations of the La-Si-P system. The crucial role of training data in the ML potential development is discussed. The developed ANN-ML potential accurately describes not only the energy vs volume curves for all the known elemental, binary, and ternary crystalline structures in the La-Si-P system but also the structures of La-Si-P liquids with various compositions. Using the developed ANN-ML potential, the melting temperatures of several crystalline phases in the La-Si-P system are predicted by the coexistence of solid-liquid phases from MD simulations. While the ANN-ML model systematically underestimates the melting temperatures of these phases, the overall trend agrees with experiment. The developed ANN-ML potential is also applied to study the nucleation and growth of LaP as a function of different relative concentrations of Si and P in the La-Si-P liquid, and the obtained results are consistent with experimental observations.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144955758","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

Glassy dynamics and a growing structural length scale in supercooled nanoparticles. 过冷纳米颗粒的玻璃动力学和不断增长的结构长度尺度。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0280451

Weikai Qi, Shreya Tiwary, Richard K Bowles

引用次数: 0

Predicting energetic and entropic driving forces with coarse-grained models. 用粗粒度模型预测能量和熵驱动力。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0281108

Lucus M Mussi, W G Noid

{"title":"Predicting energetic and entropic driving forces with coarse-grained models.","authors":"Lucus M Mussi, W G Noid","doi":"10.1063/5.0281108","DOIUrl":"https://doi.org/10.1063/5.0281108","url":null,"abstract":"Low resolution coarse-grained (CG) models provide exceptional computational efficiency for simulating soft materials. Consequently, many studies employ CG models to determine free energy surfaces along order parameters or reaction coordinates of interest. However, because CG models average over atomic details, it is challenging to determine the energetic and entropic contributions to the resulting free energy surfaces. In this work, we present a rigorous and predictive CG framework for computing these energetic and entropic driving forces based upon simulations at a single temperature. This dual approach employs distinct variational principles to independently approximate the exact CG interaction potential, W(R), and its energetic component, EW(R). This dual approach determines the free energy surface, aφ(x), along an order parameter, φ(x), via simulations with W(R). The dual approach then determines the energetic driving force, ūφ(x), by evaluating EW(R) for the sampled configurations. The entropic driving force, s̄φ(x), is indirectly inferred, s̄φ(x)=ūφ(x)-aφ(x)/T. Importantly, this entropic contribution reflects both the CG configuration distribution and the atomic details that have been eliminated from the CG model. We demonstrate that the dual approach reasonably describes the energetic and entropic driving forces between a pair of nonpolar solutes in a polar solvent. In contrast, naïvely estimating energetics with the CG interaction potential provides a qualitatively incorrect description for these driving forces.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144955938","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

The coadsorption of chlorine and oxygen on Ag(111): Detection of electrophilic oxygen in the ClO and ClO3 quasimolecules. Ag（111）上氯和氧的共吸附：ClO和ClO3准分子中亲电氧的检测。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0277774

Boris V Andryushechkin, Vladimir M Shevlyuga, Nikita S Komarov, Tatiana V Pavlova, Konstantin N Eltsov, Valerii I Bukhtiyarov

{"title":"The coadsorption of chlorine and oxygen on Ag(111): Detection of electrophilic oxygen in the ClO and ClO3 quasimolecules.","authors":"Boris V Andryushechkin, Vladimir M Shevlyuga, Nikita S Komarov, Tatiana V Pavlova, Konstantin N Eltsov, Valerii I Bukhtiyarov","doi":"10.1063/5.0277774","DOIUrl":"https://doi.org/10.1063/5.0277774","url":null,"abstract":"The coadsorption of chlorine and oxygen on the Ag(111) surface has been studied with low-temperature scanning tunneling microscopy in combination with density functional theory (DFT) calculations. The coadsorption systems were created in two ways: either by the oxidation of the chlorinated Ag(111) surface or by chlorination of the oxidized sample. Depending on the stoichiometry, a series of new well-ordered coadsorbed structures containing both oxygen and chlorine atoms has been discovered. The DFT analysis has shown that all the structures correspond to the reconstruction of the silver (111) surface. Moreover, the reconstruction is formed by silver triangles with atoms occupying either fcc or hcp positions. Most chlorine and oxygen atoms occupy nearly fourfold positions similar to those in the p(4 × 4)-O and (3 × 3)-Cl reconstructions. A characteristic feature of all coadsorbed structures is the presence of bright objects, which we associate with ClO3 and ClO quasimolecules. Using DFT, we calculated the O 1s binding energies for all oxygen atoms in the structures. The binding energy of oxygen atoms in the nearly fourfold positions is 528 eV [as in the Ag(111)-p(4 × 4)-O phase], while the binding energies of oxygen atoms in ClO3 and ClO quasimolecules are 531 and 530 eV, respectively, indicating their electrophilic nature.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144956013","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

Sum frequency dual null angle approach and its use in surface hyperpolarizability ratio measurements. 和频双零角法及其在表面超极化率测量中的应用。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0286254

Aruna Kumarasiri, Peter Yang, Dennis Hore

引用次数: 0

Surface local strain and diatomic iron doping synergistically promote the plasmonic photoelectrochemical nitrogen reduction reaction. 表面局部应变和双原子铁掺杂协同促进等离子体光电化学氮还原反应。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0281781

Tairui Wu, Ziwei Ma, Jiazheng Wang, Jianzhang Zhou, Deyin Wu

{"title":"Surface local strain and diatomic iron doping synergistically promote the plasmonic photoelectrochemical nitrogen reduction reaction.","authors":"Tairui Wu, Ziwei Ma, Jiazheng Wang, Jianzhang Zhou, Deyin Wu","doi":"10.1063/5.0281781","DOIUrl":"https://doi.org/10.1063/5.0281781","url":null,"abstract":"Utilizing single/dual atom catalysts as well as the crystallographic plane effect to promote the nitrogen reduction reaction (NRR) has attracted extensive attention. However, there are few works to combine the two effects with the surface plasmon resonance effect based on the first-principles periodic slab models. Our calculated results can be summarized as three points. First, we investigated the adsorption Gibbs free energy (ΔG) of *N2 and *NNH on Au(100), Au(110), and Au(111) facets with single or dual Fe atoms doped. The strongest end-on and side-on adsorption occur at single and dimer Fe atoms doped Au(100) surfaces, respectively. More importantly, the N2 side-on adsorption configuration significantly reduces the ΔG of the first hydrogenation step. Second, we investigated the reason why there is a lower adsorption ΔG for the N2 side-on adsorption on dimer-Fe-doped Au(100). It was discovered that the interatomic distance of the Fe dimer exhibits a strong correlation with adsorption strength. When the Fe dimer is doped on the Au(100) surface, the dimer will relax due to local strain, enabling a stronger N2 side-on adsorption. Finally, we compared the photon absorption capacity between side-on and end-on nitrogen adsorption configurations, revealing that the latter exhibits enhanced light absorption capability at lower photon energies and across broader wavelength ranges. This theoretical research highlights the superiority of the N2 side-on adsorption configuration in plasmonic photoelectrochemical NRR and shows the influence of surface local strain and dynamic relaxation for side-on adsorption, which could be referenced to design efficient side-on adsorption catalysts.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144956079","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

Analyzing energy transfer with density-functional theory in real time: Time scales for the energy transfer between B850 bacteriochlorophylls. 用密度泛函理论实时分析能量传递：B850细菌叶绿素之间能量传递的时间尺度。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0279181

I Schelter, J M Foerster, R Richter, N Schild, S Kümmel

{"title":"Analyzing energy transfer with density-functional theory in real time: Time scales for the energy transfer between B850 bacteriochlorophylls.","authors":"I Schelter, J M Foerster, R Richter, N Schild, S Kümmel","doi":"10.1063/5.0279181","DOIUrl":"https://doi.org/10.1063/5.0279181","url":null,"abstract":"We present techniques that allow for predicting energy transfer in multichromophoric systems based on density-functional-theory calculations in real-time. Our work respects that the time-dependent density is the basic quantity in density-functional theory. In the approach that we discuss here, the simulations are done for a complete multimolecular system, i.e., do not require an a priori decomposition into subsystems. Yet, our analysis tools allow one to reliably extract energy-transfer times between different regions or constituents of the multimolecular system, the structure of transition densities, and the relative degree of excitation of constituents. We demonstrate our approach by analyzing the excitation-energy transfer between six bacteriochlorophyll molecules from the B850 ring of the light-harvesting complex 2 of the purple bacterium Rhodoblastus acidophilus. Our analysis shows that energy is transferred through this system on a time scale of ∼45 fs. The spectral analysis reveals that mainly two supermolecular excitations drive the energy transfer in this system.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"163 8","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144955712","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