Journal of Chemical Physics最新文献_第7页

The physical chemistry of solar fuels catalysis. 太阳能燃料催化的物理化学。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0234241

Karen L Mulfort, Javier J Concepcion, Benjamin Dietzek-Ivanšić, Osamu Ishitani, Junko Yano

引用次数: 0

Monte Carlo simulations of glass-forming liquids beyond Metropolis. 超越 Metropolis 的玻璃态液体蒙特卡罗模拟。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0225978

Ludovic Berthier, Federico Ghimenti, Frédéric van Wijland

引用次数: 0

Ultrafast photoinduced charge carrier dynamics of L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots coupled with gold nanoparticles. 与金纳米粒子耦合的 L-半胱氨酸和油胺稳定 CsPbBr3 包晶石量子点的超快光诱导电荷载流子动力学。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0222815

Mariam Khvichia, Kai-Chun Chou, Sidney Lee, David C Zeitz, Shengli Zou, Yan Li, Jin Z Zhang

{"title":"Ultrafast photoinduced charge carrier dynamics of L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots coupled with gold nanoparticles.","authors":"Mariam Khvichia, Kai-Chun Chou, Sidney Lee, David C Zeitz, Shengli Zou, Yan Li, Jin Z Zhang","doi":"10.1063/5.0222815","DOIUrl":"https://doi.org/10.1063/5.0222815","url":null,"abstract":"We have synthesized L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots (PQDs) and coupled them with gold nanoparticles (AuNPs). The PQDs and AuNPs, as well as their hybrid nanostructures (HNS), were characterized using UV-visible (UV-vis) and photoluminescence (PL) spectroscopy. The UV-vis spectra show absorption bands of the HNS at 503 and 520 nm, attributed mainly to PQDs and AuNPs, respectively. The PQDs show a strong excitonic PL band peaked at 513 nm from PQDs. The HR-TEM results show the formation of hybrid structures between PQDs and AuNPs, which is also supported by the PL quenching of the PQDs by the coupled AuNPs. Ultrafast dynamics of the exciton and charge carriers in the HNS and pristine PQD were studied using femtosecond transient absorption. Multiexponential fitting of the dynamic data revealed the existence of shallow and deep trap states in pristine PQDs and ultrafast electron transfer from PQDs to AuNPs in the HNS. A kinetic model was proposed to account for the key dynamic processes involved and to extract the time for electron transfer from PQDs to AuNPs in the HNS, found to be ∼2 ps. Dynamic processes in pristine PQDs are largely unchanged by HNS formation with AuNPs.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142288182","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

Accurate determination of excitation energy: An equation-of-motion approach over a bi-exponential coupled cluster theory. 激发能量的精确测定：双指数耦合团簇理论的运动方程方法。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0221202

Anish Chakraborty, Pradipta Kumar Samanta, Rahul Maitra

引用次数: 0

The influence of the bounding surface on the structural ordering of short chains of oligoetherimides. 结合表面对低聚醚酰亚胺短链结构排序的影响。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0225850

Alexey Yu Dobrovskiy, Victor M Nazarychev, Sergey V Larin, Sergey V Lyulin

{"title":"The influence of the bounding surface on the structural ordering of short chains of oligoetherimides.","authors":"Alexey Yu Dobrovskiy, Victor M Nazarychev, Sergey V Larin, Sergey V Lyulin","doi":"10.1063/5.0225850","DOIUrl":"https://doi.org/10.1063/5.0225850","url":null,"abstract":"In this study, we have conducted a comparative analysis of the structural ordering of short oligoetherimide chains (dimers) near the bounding surface, depending on the structure of that surface. In order to clarify the possibility of oligoetherimide ordering along the symmetry axes of graphene, two types of bounding surfaces were considered: graphene, with a regular discrete position of interaction centers (carbon atoms), and a smooth, structureless impermeable wall. The chemical structures of the considered dimers consist of two repeating units of BPDA-P3, ODPA-P3, or aBPDA-P3 thermoplastic polyetherimides. Using all-atom molecular dynamics simulations, the process of structural ordering of the dimers near the surface of the graphene or wall was established. The ODPA-P3 and BPDA-P3 dimers form an ordered state near the graphene surface, while the aBPDA-P3 dimers do not demonstrate structural ordering. The simulation results confirmed that the ordering direction of the BPDA-P3 and ODPA-P3 dimers near the graphene surface is chosen randomly. Comparison of the oligoetherimide structure formed near the attracting wall without a symmetrical location of the interaction centers shows the similarity of the ordering of dimers near the graphene surface and the wall. As in the case of the graphene surface, the ordering of oligoetherimide molecules near the structureless wall demonstrates one direction of ordering. Therefore, we confirmed that the key factor for the onset of ordering is the presence of a confining surface, rather than the symmetrical arrangement of interaction centers in the substrate structure.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142288176","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

Exploring run-and-tumble movement in confined settings through simulation. 通过模拟探索封闭环境中的奔跑和翻滚运动。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0221781

Dario Javier Zamora, Roberto Artuso

{"title":"Exploring run-and-tumble movement in confined settings through simulation.","authors":"Dario Javier Zamora, Roberto Artuso","doi":"10.1063/5.0221781","DOIUrl":"https://doi.org/10.1063/5.0221781","url":null,"abstract":"Motion in bounded domains is a fundamental concept in various fields, including billiard dynamics and random walks on finite lattices, and has important applications in physics, ecology, and biology. An important universal property related to the average return time to the boundary, the Mean Path Length Theorem (MPLT), has been proposed theoretically and experimentally confirmed in various contexts. We investigated a wide range of mechanisms that lead to deviations from this universal behavior, such as boundary effects, reorientation, and memory processes. This study investigates the dynamics of run-and-tumble particles within a confined two-dimensional circular domain. Through a combination of theoretical approaches and numerical simulations, we validate the MPLT under uniform and isotropic particle inflow conditions. This research demonstrates that although the MPLT is generally applicable for different step length distributions, deviations occur for non-uniform angular distributions, non-elastic boundary conditions, or memory processes. These results underline the crucial influence of boundary interactions and angular dynamics on the behavior of particles in confined spaces. Our results provide new insights into the geometry and dynamics of motion in confined spaces and contribute to a better understanding of a broad spectrum of phenomena ranging from the motion of bacteria to neutron transport. This type of analysis is crucial in situations where inhomogeneity occurs, such as multiple real-world scenarios within a limited domain.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142288166","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

RASPA3: A Monte Carlo code for computing adsorption and diffusion in nanoporous materials and thermodynamics properties of fluids. RASPA3：用于计算纳米多孔材料中的吸附和扩散以及流体热力学特性的蒙特卡罗代码。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0226249

Y A Ran, S Sharma, S R G Balestra, Z Li, S Calero, T J H Vlugt, R Q Snurr, D Dubbeldam

{"title":"RASPA3: A Monte Carlo code for computing adsorption and diffusion in nanoporous materials and thermodynamics properties of fluids.","authors":"Y A Ran, S Sharma, S R G Balestra, Z Li, S Calero, T J H Vlugt, R Q Snurr, D Dubbeldam","doi":"10.1063/5.0226249","DOIUrl":"https://doi.org/10.1063/5.0226249","url":null,"abstract":"We present RASPA3, a molecular simulation code for computing adsorption and diffusion in nanoporous materials and thermodynamic and transport properties of fluids. It implements force field based classical Monte Carlo/molecular dynamics in various ensembles. In this article, we introduce the new additions and changes compared to RASPA2. RASPA3 is rewritten from the ground up in C++23 with speed and code readability in mind. Transition-matrix Monte Carlo is added to compute the density of states and free energies. The Monte Carlo code for rigid molecules is based on quaternions, and the atomic positions needed in the energy evaluation are recreated from the center of mass position and quaternion orientation. The expanded ensemble methodology for fractional molecules, with a scaling parameter λ between 0 and 1, now also keeps track of analytic expressions of dU/dλ, allowing independent verification of the chemical potential using thermodynamic integration. The source code is freely available under the MIT license on GitHub. Using this code, we compare four Monte Carlo (MC) insertion/deletion techniques: unbiased Metropolis MC, Configurational-Bias Monte Carlo (CBMC), Continuous Fractional Component MC (CFCMC), and CB/CFCMC. We compare particle distribution shapes, acceptance ratios, accuracy and speed of isotherm computation, enthalpies of adsorption, and chemical potentials, over a wide range of loadings and systems, for the grand canonical ensemble and for the Gibbs ensemble.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142288174","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

Film swelling and contaminant adsorption at polymer coated surfaces: Insights from density functional theory. 聚合物涂层表面的薄膜膨胀和污染物吸附：密度泛函理论的启示。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-21 DOI: 10.1063/5.0225085

Laura J Douglas Frink, Frank van Swol, Anthony P Malanoski, Dimiter N Petsev

{"title":"Film swelling and contaminant adsorption at polymer coated surfaces: Insights from density functional theory.","authors":"Laura J Douglas Frink, Frank van Swol, Anthony P Malanoski, Dimiter N Petsev","doi":"10.1063/5.0225085","DOIUrl":"https://doi.org/10.1063/5.0225085","url":null,"abstract":"Designing coatings and films that can protect surfaces is important in a wide variety of applications from corrosion prevention to anti-fouling. These systems are challenging from a modeling perspective because they are invariably multicomponent, which quickly leads to an expansive design space. At a minimum, the system has a substrate, a film (often composed of a polymeric material), a ubiquitous carrier solvent, which may be either a vapor or liquid phase, and one or more contaminants. Each component has an impact on the effectiveness of coating. This paper focuses on films that are used as a barrier to surface contamination, but the results also extend to surface coatings that are designed to extract a low density species from the fluid phase as in liquid chromatography. A coarse-grained model is developed using Yukawa potentials that encompasses both repulsive and attractive interactions among the species. Classical density functional theory calculations are presented to show how contaminant adsorption is controlled by the molecular forces in the system. Two specific vectors through the parameter space are considered to address likely experimental manipulations that change either the solvent or the polymer in a system. We find that all the adsorption results can be unified by considering an appropriate combination of molecular parameters. As a result, these calculations provide a link between molecular interactions and film performance and may serve to guide the rational design of films.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142288167","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 significance of fuzzy boundaries of the barrier regions in single-molecule measurements of failed barrier crossing attempts. 单分子测量穿越势垒失败尝试中势垒区模糊边界的重要性。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-14 DOI: 10.1063/5.0227497

Alexander M Berezhkovskii, Dmitrii E Makarov

{"title":"The significance of fuzzy boundaries of the barrier regions in single-molecule measurements of failed barrier crossing attempts.","authors":"Alexander M Berezhkovskii, Dmitrii E Makarov","doi":"10.1063/5.0227497","DOIUrl":"10.1063/5.0227497","url":null,"abstract":"A recent ground-breaking experimental study [Lyons et al., Phys. Rev. X 14(1), 011017 (2024)] reports on measuring the temporal duration and the spatial extent of failed attempts to cross an activation barrier (i.e., \"loops\") for a folding transition in a single molecule and for a Brownian particle trapped within a bistable potential. Within the model of diffusive dynamics, however, both of these quantities are, on average, exactly zero because of the recrossings of the barrier region boundary. That is, an observer endowed with infinite spatial and temporal resolution would find that finite loops do not exist (or, more precisely, form a set of measure zero). Here we develop a description of the experiment that takes the \"fuzziness\" of the boundaries caused by finite experimental resolution into account and show how the experimental uncertainty of localizing the point, in time and space, where the barrier is crossed leads to observable distributions of loop times and sizes. Although these distributions generally depend on the experimental resolution, this dependence, in certain cases, may amount to a simple resolution-dependent factor and, therefore, the experiments do probe inherent properties of barrier crossing dynamics.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11387013/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142154244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Beyond the "spine of hydration": Chiral SFG spectroscopy detects DNA first hydration shell and base pair structures. 超越 "水合脊柱"：手性 SFG 光谱检测 DNA 第一水合壳和碱基对结构。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-07 DOI: 10.1063/5.0220479

Ethan A Perets, Daniel Konstantinovsky, Ty Santiago, Pablo E Videla, Matthew Tremblay, Luis Velarde, Victor S Batista, Sharon Hammes-Schiffer, Elsa C Y Yan

{"title":"Beyond the \"spine of hydration\": Chiral SFG spectroscopy detects DNA first hydration shell and base pair structures.","authors":"Ethan A Perets, Daniel Konstantinovsky, Ty Santiago, Pablo E Videla, Matthew Tremblay, Luis Velarde, Victor S Batista, Sharon Hammes-Schiffer, Elsa C Y Yan","doi":"10.1063/5.0220479","DOIUrl":"10.1063/5.0220479","url":null,"abstract":"Experimental methods capable of selectively probing water at the DNA minor groove, major groove, and phosphate backbone are crucial for understanding how hydration influences DNA structure and function. Chiral-selective sum frequency generation spectroscopy (chiral SFG) is unique among vibrational spectroscopies because it can selectively probe water molecules that form chiral hydration structures around biomolecules. However, interpreting chiral SFG spectra is challenging since both water and the biomolecule can produce chiral SFG signals. Here, we combine experiment and computation to establish a theoretical framework for the rigorous interpretation of chiral SFG spectra of DNA. We demonstrate that chiral SFG detects the N-H stretch of DNA base pairs and the O-H stretch of water, exclusively probing water molecules in the DNA first hydration shell. Our analysis reveals that DNA transfers chirality to water molecules only within the first hydration shell, so they can be probed by chiral SFG spectroscopy. Beyond the first hydration shell, the electric field-induced water structure is symmetric and, therefore, precludes chiral SFG response. Furthermore, we find that chiral SFG can differentiate chiral subpopulations of first hydration shell water molecules at the minor groove, major groove, and phosphate backbone. Our findings challenge the scientific perspective dominant for more than 40 years that the minor groove \"spine of hydration\" is the only chiral water structure surrounding the DNA double helix. By identifying the molecular origins of the DNA chiral SFG spectrum, we lay a robust experimental and theoretical foundation for applying chiral SFG to explore the chemical and biological physics of DNA hydration.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11377083/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142125875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0