Journal of Chemical Physics最新文献_第6页

Sub-ambient water wettability of hydrophilic and hydrophobic SiO2 surfaces. 亲水性和疏水性二氧化硅表面的亚环境水润湿性。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0236994

Jianghui Liu, Haishan Cao

{"title":"Sub-ambient water wettability of hydrophilic and hydrophobic SiO2 surfaces.","authors":"Jianghui Liu, Haishan Cao","doi":"10.1063/5.0236994","DOIUrl":"https://doi.org/10.1063/5.0236994","url":null,"abstract":"The wettability of SiO2 surfaces, crucial for understanding the phase transition processes of water, remains a topic of significant controversy in the literature due to uncertainties in experiments. Molecular dynamics (MD) simulations offer a promising avenue for elucidating these complexities, yet studies specifically addressing water contact angles on hydrophilic and hydrophobic SiO2 surfaces at sub-ambient temperatures are notably absent. In this study, we experimentally measured water contact angles of hydrophilic and hydrophobic SiO2 surfaces at ambient temperature and employed MD to investigate water contact angles on Q3, Q3/Q4, and Q4 SiO2 surfaces across temperatures ranging from 220 to 300 K. We investigated the effects of the distribution of hydroxyl groups, droplet size, and hydroxyl density and found that the hydroxyl density had the largest impact on contact angle. Moreover, hydrogen bond analysis uncovered enhanced water affinities of Q3 and Q3/Q4 SiO2 surfaces at lower temperatures, and the spreading rate of precursor films reduced with decreasing temperature. This comprehensive study sheds light on the intricate interaction between surface properties and water behavior, promoting our understanding of the wettability of SiO2 surfaces.","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":"142604706","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

Collision of cesium atoms on helium nanodroplets: Unraveling mechanisms for surface capture at experimental velocities. 铯原子在氦纳米液滴上的碰撞：揭示实验速度下的表面俘获机制。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0231641

David A Bonhommeau

{"title":"Collision of cesium atoms on helium nanodroplets: Unraveling mechanisms for surface capture at experimental velocities.","authors":"David A Bonhommeau","doi":"10.1063/5.0231641","DOIUrl":"https://doi.org/10.1063/5.0231641","url":null,"abstract":"The collision of cesium atoms on the surface of helium nanodroplets (HNDs) containing 1000 atoms is described by the ZPAD-mPL approach, a zero-point averaged dynamics (ZPAD) method based on a He-He pseudopotential adjusted to better reproduce the total energy of He1000. Four types of collisional patterns were identified depending on the initial projectile speed v0 and impact parameter b. At the lowest speeds (v0 ≲ 250 m s-1), Cs atoms are softly captured by the HND surface, while at the highest ones (v0 ≳ 500-600 m s-1), Cs atoms can travel through the droplet and move away. In between these two extreme cases, Cs atoms can be temporarily submerged in the HND before being expelled to the surface if b = 0 or cross the HND before being captured on its surface. The possibility for Cs capture at experimental velocities and droplet piercings at the highest ones contrasts with time-dependent density functional theory calculations, which predict Cs capture for velocities lower than 75 m s-1, and ring-polymer molecular dynamics (RPMD) or former ZPAD-like methods, which predict soft Cs capture up to 500 m s-1. ZPAD-mPL results are attributed to the liquid but non-superfluid nature of the droplet, which favors energy exchanges with the helium environment, and to low He-He binding energy and HND surface tension, which can stimulate helium ejections, especially at high projectile speeds. Despite the use of a pseudopotential to model He-He interactions, the heliophobicity of Cs atoms is maintained as demonstrated by their ability to remain localized on the HND surface or to be expelled to the HND surface after transient submersion in helium.","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":"142604669","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

Extrinsic fluctuations in the p53 cycle. p53 周期的外部波动。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0227728

Manuel Eduardo Hernández-García, Mariana Gómez-Schiavon, Jorge Velázquez-Castro

{"title":"Extrinsic fluctuations in the p53 cycle.","authors":"Manuel Eduardo Hernández-García, Mariana Gómez-Schiavon, Jorge Velázquez-Castro","doi":"10.1063/5.0227728","DOIUrl":"https://doi.org/10.1063/5.0227728","url":null,"abstract":"Fluctuations are inherent to biological systems, arising from the stochastic nature of molecular interactions, and influence various aspects of system behavior, stability, and robustness. These fluctuations can be categorized as intrinsic, stemming from the system's inherent structure and dynamics, and extrinsic, arising from external factors, such as temperature variations. Understanding the interplay between these fluctuations is crucial for obtaining a comprehensive understanding of biological phenomena. However, studying these effects poses significant computational challenges. In this study, we used an underexplored methodology to analyze the effect of extrinsic fluctuations in stochastic systems using ordinary differential equations instead of solving the master equation with stochastic parameters. By incorporating temperature fluctuations into reaction rates, we explored the impact of extrinsic factors on system dynamics. We constructed a master equation and calculated the equations for the dynamics of the first two moments, offering computational efficiency compared with directly solving the chemical master equation. We applied this approach to analyze a biological oscillator, focusing on the p53 model and its response to temperature-induced extrinsic fluctuations. Our findings underscore the impact of extrinsic fluctuations on the nature of oscillations in biological systems, with alterations in oscillatory behavior depending on the characteristics of extrinsic fluctuations. We observed an increased oscillation amplitude and frequency of the p53 concentration cycle. This study provides valuable insights into the effects of extrinsic fluctuations on biological oscillations and highlights the importance of considering them in more complex systems to prevent unwanted scenarios related to health issues.","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":"142604673","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

Open quantum dynamics with variational non-Gaussian states and the truncated Wigner approximation. 具有变异非高斯状态和截断维格纳近似的开放量子动力学。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0226268

Liam J Bond, Bas Gerritsen, Jiří Minář, Jeremy T Young, Johannes Schachenmayer, Arghavan Safavi-Naini

引用次数: 0

Non-adiabatic coupling matrix elements in a magnetic field: Geometric gauge dependence and Berry phase. 磁场中的非绝热耦合矩阵元素：几何量规依赖性和贝里相位。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0229854

Tanner Culpitt, Erik I Tellgren, Laurens D M Peters, Trygve Helgaker

{"title":"Non-adiabatic coupling matrix elements in a magnetic field: Geometric gauge dependence and Berry phase.","authors":"Tanner Culpitt, Erik I Tellgren, Laurens D M Peters, Trygve Helgaker","doi":"10.1063/5.0229854","DOIUrl":"https://doi.org/10.1063/5.0229854","url":null,"abstract":"Non-adiabatic coupling matrix elements (NACMEs) are important in quantum chemistry, particularly for molecular dynamics methods such as surface hopping. However, NACMEs are gauge dependent. This presents a difficulty for their calculation in general, where there are no restrictions on the gauge function except that it be differentiable. These cases are relevant for complex-valued electronic wave functions, such as those that arise in the presence of a magnetic field or spin-orbit coupling. In addition, the Berry curvature and Berry force play an important role in molecular dynamics in a magnetic field and are also relevant in the context of spin-orbit coupling. For methods such as surface hopping, excited-state Berry curvatures will also be of interest. With this in mind, we have developed a scheme for the calculation of continuous, differentiable NACMEs as a function of the molecular geometry for complex-valued wave functions. We demonstrate the efficacy of the method using the H2 molecule at the full configuration-interaction (FCI) level of theory. In addition, ground- and excited-state Berry curvatures are computed for the first time using FCI theory. Finally, Berry phases are computed directly in terms of diagonal NACMEs.","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":"142621415","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

Semiclassical instanton theory for reaction rates at any temperature: How a rigorous real-time derivation solves the crossover temperature problem. 任何温度下反应速率的半经典瞬子理论：严格的实时推导如何解决交叉温度问题。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0237368

Joseph E Lawrence

{"title":"Semiclassical instanton theory for reaction rates at any temperature: How a rigorous real-time derivation solves the crossover temperature problem.","authors":"Joseph E Lawrence","doi":"10.1063/5.0237368","DOIUrl":"https://doi.org/10.1063/5.0237368","url":null,"abstract":"Instanton theory relates the rate constant for tunneling through a barrier to the periodic classical trajectory on the upturned potential energy surface, whose period is τ = ℏ/(kBT). Unfortunately, the standard theory is only applicable below the \"crossover temperature,\" where the periodic orbit first appears. This paper presents a rigorous semiclassical (ℏ → 0) theory for the rate that is valid at any temperature. The theory is derived by combining Bleistein's method for generating uniform asymptotic expansions with a real-time modification of Richardson's flux-correlation function derivation of instanton theory. The resulting theory smoothly connects the instanton result at low temperature to the parabolic correction to Eyring transition state theory at high-temperature. Although the derivation involves real time, the final theory only involves imaginary-time (thermal) properties, consistent with the standard version of instanton theory. Therefore, it is no more difficult to compute than the standard theory. The theory is illustrated with application to model systems, where it is shown to give excellent numerical results. Finally, the first-principles approach taken here results in a number of advantages over previous attempts to extend the imaginary free-energy formulation of instanton theory. In addition to producing a theory that is a smooth (continuously differentiable) function of temperature, the derivation also naturally incorporates hyperasymptotic (i.e., multi-orbit) terms and provides a framework for further extensions of the theory.","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":"142620833","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

Brownian dynamics simulation of the structural evolution in monodisperse hard-sphere suspensions during drying and sedimentation processes. 对单分散硬球悬浮液在干燥和沉积过程中的结构演变进行布朗动力学模拟。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0238549

Yeji Kim, Young Ki Lee

{"title":"Brownian dynamics simulation of the structural evolution in monodisperse hard-sphere suspensions during drying and sedimentation processes.","authors":"Yeji Kim, Young Ki Lee","doi":"10.1063/5.0238549","DOIUrl":"https://doi.org/10.1063/5.0238549","url":null,"abstract":"The drying behavior of monodisperse colloidal films, with a focus on the influence of process variables on film microstructures, is explored via Brownian dynamics (BD) simulations. In our model, hard-sphere colloidal particles are dispersed in a Newtonian liquid with an initial particle volume fraction of 0.1. The effects of the drying rate and sedimentation on the evolving microstructures are systematically investigated using two dimensionless numbers: the Péclet number (Pe), which represents the competition between evaporation and diffusion, and the sedimentation number (Ns), which reflects the relative influence of sedimentation on evaporation. First, we analyze the local particle volume fraction and film structure at various Pe and Ns. As Pe increases, particle accumulation occurs near the liquid-gas interface, whereas a high Ns promotes dense packing near the substrate owing to sedimentation. The BD simulation results, viz. the local volume fraction profiles and drying regime maps, are in good agreement with those of the continuum model proposed by Wang and Brady. Structural analysis of the dried films reveals that at a low Pe (Pe = 0.1), a face-centered cubic (FCC) structure dominates, primarily independent of the sedimentation effects. In contrast, a high Pe leads to hexagonal close-packed or amorphous structure formation. Notably, at intermediate drying rates (Pe = 10), an increase in Ns promotes additional FCC ordering in the final film structure. Our study provides new insights into the hitherto underexplored role of sedimentation in the structural evolution of drying colloidal films, revealing the mechanisms of drying-induced assembly in colloidal 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":"142621390","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

Cooperative lattice theory for CO2 adsorption in diamine-appended metal-organic framework at humid direct air capture conditions. 在潮湿的直接空气捕获条件下，二氨基金属有机框架中二氧化碳吸附的合作晶格理论。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0228985

Bennett D Marshall, Pavel Kortunov, Aaron Peters, Hilda Vroman

引用次数: 0

Nonlinear conductivity of aqueous electrolytes: Beyond the first Wien effect. 水性电解质的非线性电导率：超越第一维恩效应

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0226773

Hélène Berthoumieux, Vincent Démery, Anthony C Maggs

引用次数: 0

Chirality of plasmonic structures and materials. 等离子结构和材料的手性。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-11-14 DOI: 10.1063/5.0244919

Lucas V Besteiro, Yongmin Liu, Hiromi Okamoto

引用次数: 0