Journal of Chemical Physics最新文献_第8页

Simplification of solvation shell with water clusters in the simulation of electrochemical nitrogen reduction reaction. 电化学氮还原反应模拟中水簇溶壳的简化。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0230137

Han-Xuan Liu, Zheng-Qing Huang, Xin Gao, Guidong Yang, Chun-Ran Chang

{"title":"Simplification of solvation shell with water clusters in the simulation of electrochemical nitrogen reduction reaction.","authors":"Han-Xuan Liu, Zheng-Qing Huang, Xin Gao, Guidong Yang, Chun-Ran Chang","doi":"10.1063/5.0230137","DOIUrl":"https://doi.org/10.1063/5.0230137","url":null,"abstract":"Electrochemical methods for nitrogen reduction have received extensive attention due to the mild reaction conditions. In order to gain an insight into the mechanism of the electrochemical nitrogen reduction process, theoretical simulations are necessary. However, current simulation studies contain many imprecise approximations that may hinder the real recognition of the reaction process. Although solvation methods have recently been developed to provide efficient descriptions, their further applications are hindered by controversy over modeling of solvents and the enormous computational effort required. In this work, we simplify the solvation conditions by using water clusters and compare them with an accurate water layer model. The results demonstrate that the simplified water clusters can effectively capture protons, simulate the surface electric environment, and enable the calculation of the activation energy of the reaction. This method offers an affordable approach for simulating the surface potentials and solvents and provides a new reference for the theoretical study of the electrochemical nitrogen reduction reaction.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 18","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142620932","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

Simulating the Landau-Zener sweep in deeply sub-Ohmic environments. 模拟深亚欧姆环境中的朗道-齐纳扫描。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0235741

Felix Kahlert, Valentin Link, Richard Hartmann, Walter T Strunz

引用次数: 0

A computer simulation study of a chiral active ring polymer. 手性活性环聚合物的计算机模拟研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0232538

Shalabh K Anand

引用次数: 0

Hydrogen diffusion on Ni(100): A combined machine-learning, ring polymer molecular dynamics, and kinetic Monte Carlo study. 镍（100）上的氢扩散：机器学习、环状聚合物分子动力学和动力学蒙特卡洛综合研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0226314

J Steffen, A Alibakhshi

{"title":"Hydrogen diffusion on Ni(100): A combined machine-learning, ring polymer molecular dynamics, and kinetic Monte Carlo study.","authors":"J Steffen, A Alibakhshi","doi":"10.1063/5.0226314","DOIUrl":"https://doi.org/10.1063/5.0226314","url":null,"abstract":"We introduce a methodological framework coupling machine-learning potentials, ring polymer molecular dynamics (RPMD), and kinetic Monte Carlo (kMC) to draw a comprehensive physical picture of the collective diffusion of hydrogen atoms on metal surfaces. For the benchmark case of hydrogen diffusion on a Ni(100) surface, the hydrogen adsorption and diffusion energetics and its dependence on the local coverage is described via a neural-network potential, where the training data are computed via periodic density functional theory (DFT) and include all relevant optimized diffusion and desorption paths, sampled by nudged elastic band optimizations and molecular dynamics simulations. Nuclear quantum effects, being crucial for processes involving hydrogen at low temperatures, are treated by RPMD. The diffusion rate constants are calculated with a combination of umbrella samplings employed to map the free energy profile and separate samplings of recrossing trajectories to obtain the transmission coefficient. The calculated diffusion rates for different temperatures and local environments are then combined and fitted into a kMC model allowing access to larger time and length scales. Our results demonstrate an outstanding performance for the trained neural network potential in reproducing reference DFT energies and forces. We report the effective diffusion rates for different temperatures and hydrogen surface coverages obtained via this recipe in good agreement with the experimental results. The method combination proposed in this study can be instrumental for a wide range of applications in materials science.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 18","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142621407","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

Influence of temperature and crack-tip speed on crack propagation in elastic solids. 温度和裂纹尖端速度对弹性固体裂纹扩展的影响

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0236699

B N J Persson

引用次数: 0

Propagation gap for shear waves in binary liquids: Analytical and simulation study. 二元液体中剪切波的传播间隙：分析与模拟研究

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0236047

Taras Bryk, Maria Kopcha, Ihor Yidak

引用次数: 0

Reduced density matrix dynamics in multistate harmonic models via time-convolution and time-convolutionless quantum master equations with quantum-mechanical and semiclassical kernels. 通过具有量子力学和半经典核的时间卷积和无时间卷积量子主方程的多态谐波模型中的还原密度矩阵动力学。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0231561

Xiang Sun, Zengkui Liu

{"title":"Reduced density matrix dynamics in multistate harmonic models via time-convolution and time-convolutionless quantum master equations with quantum-mechanical and semiclassical kernels.","authors":"Xiang Sun, Zengkui Liu","doi":"10.1063/5.0231561","DOIUrl":"https://doi.org/10.1063/5.0231561","url":null,"abstract":"In this work, we explore the electronic reduced density matrix (RDM) dynamics using time-convolution (TC) and time-convolutionless (TCL) quantum master equations (QMEs) that are based on perturbative electronic couplings within the framework of multistate harmonic (MSH) models. The MSH model Hamiltonian consistently incorporates the electronic-vibrational correlations between all pairs of states by satisfying the pairwise reorganization energies directly obtained from all-atom simulations, representing the globally heterogeneous environments that couple to the multiple states differently. We derive the exact quantum-mechanical and a hierarchy of semiclassical approximate expressions for the kernels in TC and TCL QMEs that project the full RDM for general shifted harmonic systems, including the MSH model. These QMEs are applied to simulate RDM dynamics of photoinduced charge transfer (PICT) in organic photovoltaic carotenoid-porphyrin-fullerene triad solvated in tetrahydrofuran solution and the excitation energy transfer (EET) dynamics in photosynthetic Fenna-Matthews-Olson complexes from C. tepidum and P. aestuarii. Our results show that while both TC and TCL QMEs capture similar phenomena in PICT and EET processes, TC QME generally provides more accurate results than TCL QME, particularly in the initial oscillation of EET population dynamics. This study highlights the effectiveness of the TC and TCL QMEs in modeling RDM dynamics of nonadiabatic processes, offering insights for realistic condensed phase systems.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 18","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142620614","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

Energy relaxation of N2O in gaseous, supercritical, and liquid xenon and SF6. 气态、超临界、液态氙和 SF6 中 N2O 的能量弛豫。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0235760

Kai Töpfer, Shyamsunder Erramilli, Lawrence D Ziegler, Markus Meuwly

{"title":"Energy relaxation of N2O in gaseous, supercritical, and liquid xenon and SF6.","authors":"Kai Töpfer, Shyamsunder Erramilli, Lawrence D Ziegler, Markus Meuwly","doi":"10.1063/5.0235760","DOIUrl":"https://doi.org/10.1063/5.0235760","url":null,"abstract":"Rotational and vibrational energy relaxation (RER and VER) of N2O embedded in xenon and SF6 environments ranging from the gas phase to the liquid, including the supercritical regime, is studied at a molecular level. Calibrated intermolecular interactions from high-level electronic structure calculations, validated against experiments for the pure solvents, were used to carry out classical molecular dynamics simulations corresponding to experimental state points for near-critical isotherms. The computed RER rates in low-density solvents of krotXe=(3.67±0.25)×1010 s-1 M-1 and krotSF6=(1.25±0.12)×1011 s-1 M-1 compare well with the rates determined by the analysis of two-dimensional infrared experiments. Simulations find that an isolated binary collision description is successful up to solvent concentrations of ∼4 M. For higher densities, including the supercritical regime, the simulations do not correctly describe RER, probably due to the neglect of solvent-solute coupling in the analysis of the rotational motion. For VER, the near-quantitative agreement between simulations and pump-probe experiments captures the solvent density-dependent trends.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 18","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142621405","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

Improvement on the screening of nonlinear commutator operations in selective coupled-cluster using Lagrangian. 利用拉格朗日改进选择性耦合簇中非线性换向器运算的筛选。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0231739

Suhita Basumallick, Enhua Xu, Seiichiro L Ten-No

引用次数: 0

Learning glass transition temperatures via dimensionality reduction with data from computer simulations: Polymers as the pilot case. 通过计算机模拟数据的降维学习玻璃化转变温度：以聚合物为试点案例。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0229161

Artem Glova, Mikko Karttunen

{"title":"Learning glass transition temperatures via dimensionality reduction with data from computer simulations: Polymers as the pilot case.","authors":"Artem Glova, Mikko Karttunen","doi":"10.1063/5.0229161","DOIUrl":"https://doi.org/10.1063/5.0229161","url":null,"abstract":"Machine learning methods provide an advanced means for understanding inherent patterns within large and complex datasets. Here, we employ the principal component analysis (PCA) and the diffusion map (DM) techniques to evaluate the glass transition temperature (Tg) from low-dimensional representations of all-atom molecular dynamic simulations of polylactide (PLA) and poly(3-hydroxybutyrate) (PHB). Four molecular descriptors were considered: radial distribution functions (RDFs), mean square displacements (MSDs), relative square displacements (RSDs), and dihedral angles (DAs). By applying Gaussian Mixture Models (GMMs) to analyze the PCA and DM projections and by quantifying their log-likelihoods as a density-based metric, a distinct separation into two populations corresponding to melt and glass states was revealed. This separation enabled the Tg evaluation from a cooling-induced sharp increase in the overlap between log-likelihood distributions at different temperatures. Tg values derived from the RDF and MSD descriptors using DM closely matched the standard computer simulation-based dilatometric and dynamic Tg values for both PLA and PHB models. This was not the case for PCA. The DM-transformed DA and RSD data resulted in Tg values in agreement with experimental ones. Overall, the fusion of atomistic simulations and DMs complemented with the GMMs presents a promising framework for computing Tg and studying the glass transition in a unified way across various molecular descriptors for glass-forming materials.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 18","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142604685","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