Journal of Chemical Physics最新文献_第9页

Macrotransport of active particles in periodic channels and fields: Rectification and dispersion. 活性粒子在周期性通道和场中的宏观传输：整流与分散

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0232614

Zhiwei Peng

{"title":"Macrotransport of active particles in periodic channels and fields: Rectification and dispersion.","authors":"Zhiwei Peng","doi":"10.1063/5.0232614","DOIUrl":"https://doi.org/10.1063/5.0232614","url":null,"abstract":"Transport and dispersion of active particles in structured environments, such as corrugated channels and porous media, are important for the understanding of both natural and engineered active systems. Owing to their continuous self-propulsion, active particles exhibit rectified transport under spatially asymmetric confinement. While progress has been made in experiments and particle-based simulations, a theoretical understanding of the effective long-time transport dynamics in spatially periodic geometries remains less developed. In this paper, we apply generalized Taylor dispersion theory to analyze the long-time effective transport dynamics of active Brownian particles (ABPs) in periodic channels and fields. We show that the long-time transport behavior is governed by an effective advection-diffusion equation. The derived macrotransport equations allow us to characterize the average drift and effective dispersion coefficient. For the case of ABPs subject to a no-flux boundary condition at the channel wall, we show that regardless of activity, the average drift is given by the net diffusive flux along the channel. For ABPs, their activity is the driving mechanism that sustains a density gradient, which ultimately leads to rectified motion along the channel. Our continuum theory is validated against direct Brownian dynamics simulations of the Langevin equations governing the motion of each ABP.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466480","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

All-electron first-principles GWΓ simulations for accurately predicting core-electron binding energies considering first-order three-point vertex corrections. 考虑一阶三点顶点修正的全电子第一原理 GWΓ 模拟，用于准确预测核-电子结合能。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0227580

Kenta Yoneyama, Yoshifumi Noguchi, Kaoru Ohno

{"title":"All-electron first-principles GWΓ simulations for accurately predicting core-electron binding energies considering first-order three-point vertex corrections.","authors":"Kenta Yoneyama, Yoshifumi Noguchi, Kaoru Ohno","doi":"10.1063/5.0227580","DOIUrl":"https://doi.org/10.1063/5.0227580","url":null,"abstract":"In the conventional GW method, the three-point vertex function (Γ) is approximated to unity (Γ ∼ 1). Here, we developed an all-electron first-principles GWΓ method beyond a conventional GW method by considering a first-order three-point vertex function (Γ(1) = 1 + iGGW) in a one-electron self-energy operator. We applied the GWΓ method to simulate the binding energies (BEs) of B1s, C1s, N1s, O1s, and F1s for 19 small-sized molecules. Contrary to the one-shot GW method [or G0W0(LDA)], which underestimates the experimentally determined absolute BEs by about 3.7 eV for B1s, 5.1 eV for C1s, 6.9 eV for N1s, 7.8 eV for O1s, and 5.8 eV for F1s, the GWΓ method successfully reduces these errors by approximately 1-2 eV for all the elements studied here. Notably, the first-order three-point vertex corrections are more significant for heavier elements, following the order of F > O > N > C > B1s. Finally, the computational cost analysis revealed that one term in the GWΓ one-electron self-energy operator, despite being computationally intensive, contributes negligibly (<0.1 eV) to the C1s, N1s, O1s, and F1s.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466452","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

Effect of current collector on the coupled electro-chemo-mechanical performance of graphite electrodes in LiBs. 集流器对锂电池石墨电极耦合电化学机械性能的影响。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0233210

Xiaolin Li, Jiahui Liu, Honghui Gu, Hainan Jiang, Linlin Song, Yaolong He, Dawei Li

{"title":"Effect of current collector on the coupled electro-chemo-mechanical performance of graphite electrodes in LiBs.","authors":"Xiaolin Li, Jiahui Liu, Honghui Gu, Hainan Jiang, Linlin Song, Yaolong He, Dawei Li","doi":"10.1063/5.0233210","DOIUrl":"https://doi.org/10.1063/5.0233210","url":null,"abstract":"The current collector, one of the main components in the manufacture of composite electrodes, is mainly used to enhance the mechanical stability and improve the performance and cycle performance of the electrodes. During the electrochemical reaction, the lithium diffusion can induce compressive stress and affect the mechanical performance, lifespan, and performance of batteries. Therefore, this study analyzed the influence of copper foil on the mechanical response and degradation performance of electrodes. In addition, a mathematical model was developed to analyze the effect of copper foil on the stress-strain behavior of the electrodes. The results indicated that the stress and modulus of the graphite electrodes have a non-linear increase with the lithiation process. Based on those findings, utilizing a thinner and more compliant current collector could effectively mitigate the in-plane strain and the stress within electrodes. Thus, developing a thinner and softer copper foil could simultaneously enhance the mechanical properties and specific density of composite electrodes for the next-generation LiBs.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466460","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

Grassmann time-evolving matrix product operators: An efficient numerical approach for fermionic path integral simulations. 格拉斯曼时变矩阵积算子：费米子路径积分模拟的高效数值方法。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0226167

Xiansong Xu, Chu Guo, Ruofan Chen

{"title":"Grassmann time-evolving matrix product operators: An efficient numerical approach for fermionic path integral simulations.","authors":"Xiansong Xu, Chu Guo, Ruofan Chen","doi":"10.1063/5.0226167","DOIUrl":"https://doi.org/10.1063/5.0226167","url":null,"abstract":"Developing numerical exact solvers for open quantum systems is a challenging task due to the non-perturbative and non-Markovian nature when coupling to structured environments. The Feynman-Vernon influence functional approach is a powerful analytical tool to study the dynamics of open quantum systems. Numerical treatments of the influence functional including the quasi-adiabatic propagator technique and the tensor-network-based time-evolving matrix product operator method have proven to be efficient in studying open quantum systems with bosonic environments. However, the numerical implementation of the fermionic path integral suffers from the Grassmann algebra involved. In this work, we present a detailed introduction to the Grassmann time-evolving matrix product operator method for fermionic open quantum systems. In particular, we introduce the concepts of Grassmann tensor, signed matrix product operator, and Grassmann matrix product state to handle the Grassmann path integral. Using the single-orbital Anderson impurity model as an example, we review the numerical benchmarks for structured fermionic environments for real-time nonequilibrium dynamics, real-time and imaginary-time equilibration dynamics, and its application as an impurity solver. These benchmarks show that our method is a robust and promising numerical approach to study strong coupling physics and non-Markovian dynamics. It can also serve as an alternative impurity solver to study strongly correlated quantum matter with dynamical mean-field theory.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466472","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

Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry. 高精度热化学背景下的等级还原 CCSD(T) 前景。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0230899

Tingting Zhao, James H Thorpe, Devin A Matthews

{"title":"Prospects for rank-reduced CCSD(T) in the context of high-accuracy thermochemistry.","authors":"Tingting Zhao, James H Thorpe, Devin A Matthews","doi":"10.1063/5.0230899","DOIUrl":"https://doi.org/10.1063/5.0230899","url":null,"abstract":"Obtaining sub-chemical accuracy (1 kJ mol-1) for reaction energies of medium-sized gas-phase molecules is a longstanding challenge in the field of thermochemical modeling. The perturbative triples correction to coupled-cluster single double triple [CCSD(T)] constitutes an important component of all high-accuracy composite model chemistries that obtain this accuracy but can be a roadblock in the calculation of medium to large systems due to its O(N7) scaling, particularly in HEAT-like model chemistries that eschew separation of core and valence correlation. This study extends the work of Lesiuk [J. Chem. Phys. 156, 064103 (2022)] with new approximate methods and assesses the accuracy of five different approximations of (T) in the context of a subset of molecules selected from the W4-17 dataset. It is demonstrated that all of these approximate methods can achieve sub-0.1 kJ mol-1 accuracy with respect to canonical, density-fitted (T) contributions with a modest number of projectors. The approximation labeled Z̃T appears to offer the best trade-off between cost and accuracy and shows significant promise in an order-of-magnitude reduction in the computational cost of the CCSD(T) component of high-accuracy model chemistries.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466503","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

Effective modeling of open quantum systems by low-rank discretization of structured environments. 通过结构化环境的低阶离散化对开放量子系统进行有效建模。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0232232

Hideaki Takahashi, Raffaele Borrelli

引用次数: 0

Thermal conductivity in modified sodium silicate glasses is governed by modal phase changes. 改性硅酸钠玻璃的导热性受模态相变的影响。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0230354

Philip Rasmussen, Søren S Sørensen

{"title":"Thermal conductivity in modified sodium silicate glasses is governed by modal phase changes.","authors":"Philip Rasmussen, Søren S Sørensen","doi":"10.1063/5.0230354","DOIUrl":"https://doi.org/10.1063/5.0230354","url":null,"abstract":"The thermal conductivity of glasses is well-known to be significantly harder to theoretically describe compared to crystalline materials. Because of this fact, the fundamental understanding of thermal conductivity in glasses remain extremely poor when moving beyond the case of simple glasses, e.g., glassy SiO2, and into so-called \"modified\" oxide glasses, that is, glasses where other oxides (e.g., alkali oxides) have been added to break up the network and alter, e.g., elastic and thermal properties. This lack of knowledge is apparent despite how modified glasses comprise the far majority of known glasses. In the present work, we study an archetypical series of sodium silicate [xNa2O-(100 - x)SiO2] glasses. Analyses of modal contributions reveal how increasing Na2O content induces increasing vibrational localization with a change of vibrations to be less ordered and a related general decrease in modal contributions to thermal conductivity. We find the vibrational phases (acoustic vs optical) of sodium vibrations to be relatively disordered compared to the network-forming silicon and oxygen species, explaining how increasing Na2O content decreases thermal conductivity. Our work sheds new light on the fundamentals of glassy heat transfer as well as the interplay between thermal conduction and modal characteristics in glasses.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466512","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

Differentially heterogeneous hydration environment of the familial mutants of α-synuclein. α-突触核蛋白家族突变体的异质性水合环境。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0230853

Leena Aggarwal, Sayan Karmakar, Parbati Biswas

{"title":"Differentially heterogeneous hydration environment of the familial mutants of α-synuclein.","authors":"Leena Aggarwal, Sayan Karmakar, Parbati Biswas","doi":"10.1063/5.0230853","DOIUrl":"10.1063/5.0230853","url":null,"abstract":"The behavior of hydration water around familial Parkinson's disease linked mutants of α-synuclein may be linked to the early-onset of Parkinson's disease. For the first time, this study compares the local structure and dynamics of hydration water around different segments of some of the natural mutants of α-synuclein, i.e., E46K, G51D, A30P, and A53E, with that of the wild-type protein through explicit water MD simulations. The results show that the C-terminal segments of the fast aggregating mutants such as E46K and A30P are less exposed to water, while those of the slow aggregating ones such as A53E and G51D are more exposed to water relative to that of the wild-type protein. In addition, the water molecules are found to be more ordered around the C-terminal segment of the A53E and G51D mutants as compared to the wild-type protein. This is due to an increase in the overall charge of α-syn upon A53E and G51D mutations. The translational and rotational motions of water molecules in the hydration shell of the C-terminal segment of A53E and G51D mutants are found to be faster relative to that of the wild-type protein. This study validates the differential hydration environment around the C-terminal segment for the causative and protective mutants of α-synuclein.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142466457","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

Construction of Ag-modified ZnO/g-C3N4 heterostructure for enhanced photocatalysis performance. 构建银改性 ZnO/g-C3N4 异质结构以提高光催化性能。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0226195

Shanshan Liu, Shaoli Cheng, Jiale Zheng, Junhui Liu, Mingju Huang

引用次数: 0

Surface weak ferromagnet coupling induced giant room-temperature spontaneous exchange bias in antiferromagnet Fe3BO6 polycrystals. 反铁磁体 Fe3BO6 多晶体中表面弱铁磁耦合诱导的巨型室温自发交换偏置。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-10-21 DOI: 10.1063/5.0225163

Lifeng Wang, Ling Cai, Xiong He, Fanli Yang, Jie Chen, Lizhi Yi, Min Liu, Yunli Xu, Zhengcai Xia, Liqing Pan

引用次数: 0