Journal of Chemical Physics最新文献_第6页

Modeling water using multipole response tensors fitted to the monomer geometry. 用适合单体几何的多极响应张量模拟水。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-09-07 DOI: 10.1063/5.0279764

Jonatan Öström, Lars G M Pettersson

引用次数: 0

Extended line list for the B2Σ+-X2Σ+ band system of CaF for use in laser-induced plasma studies. 用于激光诱导等离子体研究的CaF的B2Σ+-X2Σ+波段系统的扩展线列表。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0278000

Ziqiang Zhao, Shilin Hou, Yang Zhao, Pingsai Chu, Ye Tian

{"title":"Extended line list for the B2Σ+-X2Σ+ band system of CaF for use in laser-induced plasma studies.","authors":"Ziqiang Zhao, Shilin Hou, Yang Zhao, Pingsai Chu, Ye Tian","doi":"10.1063/5.0278000","DOIUrl":"https://doi.org/10.1063/5.0278000","url":null,"abstract":"Calcium monofluoride (CaF) is an important species for the sensitive detection of fluorine with laser-induced breakdown spectroscopy (LIBS). A line list for the B2Σ+-X2Σ+ transition system of CaF was calculated and extended from v ≤ 20 to v = 35 using empirical potential functions obtained through a direct-potential fit approach with observed transition frequencies. The line strengths were predicted using the scaled transition dipole moments calculated ab initio. The simulated intensities and transition positions with the present line list agree well with the spectra of high-resolution molecular spectroscopy from the literature and of LIBS from this work. Based on the simulated spectra of the CaF B-X system, the derived temperatures with the LIBS spectra vary across different wavelength regions. For example, with the same spectrum of delay time t = 13 μs, the obtained temperatures with λ ≈ 514-529 nm and λ ≈ 514-570 nm are 4000 and 5500 K, respectively. However, this discrepancy decreases with increasing delay time. For t = 23 μs, the obtained temperatures (3700 ± 200-4000 ± 100 K) are already in agreement within the estimated uncertainties. Self-absorption in the spectrum also influences the simulated temperature. Excluding the influences from self-absorption, the derived temperature (6000 ± 200 K) with the CaF molecular spectrum of λ ≈ 529-542 nm of t = 13 μs is close to the ionization temperature (6600 K) obtained with the Saha-Boltzmann fit from the observed atomic/ionic lines of Ca in the plasma. The present line list can be adopted in plasma diagnostics and in sensitive detections of fluorine with the CaF spectrum in hot environments.","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":"144955693","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

Diffusive transport through nanopores: What the size of a molecule is? 通过纳米孔的扩散传输：分子的大小是多少？

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0284331

Gian Marco Tuveri, Stefan Milenkovic, Matteo Ceccarelli, Igor Bodrenko

引用次数: 0

Halogen anion (Cl-, Br-) and alkali metal cation (Cs+, K+, Rb+) synergistic binding behaviors using a belt shaped dual-functional hydrocarbon receptor. 卤素阴离子（Cl-, Br-）与碱金属阳离子（Cs+, K+, Rb+）在带状双功能烃受体上的协同结合行为。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0287300

Qingqing Yao, Haolin Li, Wenbo Zhang, Yaqin Cui, Yanzhi Liu, Jianbin Zhang, Jinxing Jiang, Zhifeng Li, Kun Yuan

{"title":"Halogen anion (Cl-, Br-) and alkali metal cation (Cs+, K+, Rb+) synergistic binding behaviors using a belt shaped dual-functional hydrocarbon receptor.","authors":"Qingqing Yao, Haolin Li, Wenbo Zhang, Yaqin Cui, Yanzhi Liu, Jianbin Zhang, Jinxing Jiang, Zhifeng Li, Kun Yuan","doi":"10.1063/5.0287300","DOIUrl":"https://doi.org/10.1063/5.0287300","url":null,"abstract":"The belt shaped functionalized hydrocarbon receptors have attracted great interest because of their special \"frustum-like\" configuration, in which the openings at the upper and lower ends (dual-functional sites) are more beneficial when used as ion recognition sites. In this paper, the binding behaviors of the belt shaped dual-functional hydrocarbon receptors for halogen anions (Cl- and Br-) and alkali metal cations (K+, Rb+, and Cs+) were investigated in depth using density functional theory calculations. It is found that anion/cation binding can be enhanced and synergistically regulated by counterion and the corresponding conformational changes of the receptor, which well reflects the electrical complementary matching and mutual reinforcement effects. The nature of the receptor-ion interactions was further elucidated by combining the noncovalent intermolecular interaction with molecular electrostatic potential analysis. The complexation process of Cs+/Cl- with the receptor was dynamically tracked using ab initio molecular dynamics simulation.","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":"144955726","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

Connecting shear thinning and dynamic heterogeneity in supercooled liquids by localized elasticity. 用局部弹性理论连接过冷液体的剪切减薄与动态非均质性。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0282802

Ke-Qi Zeng, Dong-Xu Yu, Zhe Wang

引用次数: 0

Analyzing the internal interface in localized high-concentration electrolytes. 局部高浓度电解液内部界面分析。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0285201

Anne Hockmann, Monika Schönhoff, Diddo Diddens

{"title":"Analyzing the internal interface in localized high-concentration electrolytes.","authors":"Anne Hockmann, Monika Schönhoff, Diddo Diddens","doi":"10.1063/5.0285201","DOIUrl":"https://doi.org/10.1063/5.0285201","url":null,"abstract":"We present molecular dynamics simulations on localized high-concentration electrolytes (LHCE) based on the conducting salt lithium bis(fluorosulfonyl)imide (LiFSI) or lithium bis(trifluoromethanesulfonyl)imide dissolved in the solvent 1,2-dimethoxyethane and diluted to two different degrees with the diluent 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether. Due to the immiscibility of the conducting salt phase (salt + solvent) and the diluent phase, LHCEs feature a complex microstructure of two phases forming an internal interface. In this study, we not only investigate the lithium coordination structure in the conducting salt phase but also the size and composition of its interface to the diluent phase by Voronoi tessellations. Furthermore, we investigate the influence on the ion transport by evaluating Onsager coefficients. We show that an LHCE containing the surface-active anion TFSI- creates an anion-rich internal interface, leading to enhanced ion dissociation and anticorrelated ion movement. On the other hand, the smaller FSI- anion with a more localized charge distribution and less amphiphilic character shows no enrichment at the internal interface, but rather a depletion. By increasing LiFSI concentration, we even observe a solvent-rich internal interface due to a large and branched Li-anion network. Furthermore, the less diffuse interface and enlarged Li-anion network lead to lower ion-ion anticorrelations and a stronger convective flux of the conducting salt phase, which is compensated by a flux of the diluent phase, especially in the higher concentrated LiFSI based LHCE.","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":"144955754","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

Interfacial stability and strain-modulated electronic properties in LaAlO3/SrTiO3 (110) heterostructures: A first-principles study. LaAlO3/SrTiO3（110）异质结构的界面稳定性和应变调制电子特性：第一性原理研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0277966

Yaqin Wang, Yuling Li, Fangxu Wu, Demin Liu, Le Yuan, Mei Bi, Xiaolong Weng, Kesong Yang

{"title":"Interfacial stability and strain-modulated electronic properties in LaAlO3/SrTiO3 (110) heterostructures: A first-principles study.","authors":"Yaqin Wang, Yuling Li, Fangxu Wu, Demin Liu, Le Yuan, Mei Bi, Xiaolong Weng, Kesong Yang","doi":"10.1063/5.0277966","DOIUrl":"https://doi.org/10.1063/5.0277966","url":null,"abstract":"Perovskite oxide interfaces exhibit functional properties that are absent in their bulk counterparts. Compared to the well-studied LaAlO3/SrTiO3 (001) interface, the LaAlO3/SrTiO3 (110) interface remains relatively unexplored. Here, we investigate the interfacial properties of n-type LaAlO3/SrTiO3 (110) heterostructures, including cleavage energy, two-dimensional electron gas (2DEG) formation, and the effects of biaxial strain, using first-principles density functional theory calculations. Our results reveal that the (110) interface has a higher cleavage energy than the (001) interface, indicating stronger interfacial bonding interactions. In addition, we find that a critical LaAlO3 thickness of five unit cells is required to induce 2DEG formation in the (110) heterostructure, compared to four unit cells in the (001) system. Notably, biaxial strain in the (110) heterostructure induces behavior opposite to that observed in the (001) system. Compressive strain reduces the polarization strength in the LaAlO3 film, lowering the critical thickness required for 2DEG formation, whereas tensile strain enhances polarization, increasing the critical thickness for 2DEG formation. This contrasting strain response in the (110) and (001) heterostructures can be explained by their distinct crystallographic orientations at the interface. These findings provide new insights into strain-dependent interfacial phenomena and offer valuable guidance for designing functional perovskite oxide interfaces.","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":"144955873","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

Computational screening of single-atom catalysts supported on triazine-based graphite carbon nitride for 1,2-dichloroethane dechlorination. 三嗪基石墨氮化碳负载单原子1,2-二氯乙烷脱氯催化剂的计算筛选

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0288228

Huanglan Xue, Yu Huang, Yi Li, Yongfan Zhang, Wei Lin

{"title":"Computational screening of single-atom catalysts supported on triazine-based graphite carbon nitride for 1,2-dichloroethane dechlorination.","authors":"Huanglan Xue, Yu Huang, Yi Li, Yongfan Zhang, Wei Lin","doi":"10.1063/5.0288228","DOIUrl":"https://doi.org/10.1063/5.0288228","url":null,"abstract":"In this study, we systematically investigated the performance of eight transition metal atom-loaded triazine-based graphitic carbon nitride (TM@TGCN) for the catalysis of 1,2-dichloroethane (1,2-DCE) dechlorination reaction (DCEDR) by density functional theory calculations. Through the five-step screening method, the suitable catalysts, respectively, applicable to the generation of vinyl chloride (CH2CHCl), ethylene (CH2CH2), and ethane (CH3CH3) were finally determined. The limiting potential of Fe@TGCN for reducing 1,2-DCE to CH3CH3 is lower, at -0.47 V (gauche-C2H4Cl2) and -0.50 V (trans-C2H4Cl2), respectively. The activity mechanism indicates that Fe@TGCN is at the vertex of the volcano plot, confirming that the intensity of its interaction with the reactants is in optimal equilibrium. In addition, we further examined the influence of hydroxyl modification on the selectivity of DCEDR. The results show that hydroxyl modification significantly weakens the adsorption strength of intermediates (such as *CH2CH2Cl) through a steric hindrance effect and electron delocalization, as well as reduces the desorption energy of CH2CH2 and enhances its selectivity. This study provides theoretical guidance for the rational design of DCEDR electrocatalysts and reveals the key role of ligand modification strategies in regulating the reaction pathway.","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":"144955506","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

Coherent modified Redfield approach to describe photoinduced proton-coupled electron transfer. 描述光致质子耦合电子转移的相干修正红场方法。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2025-08-28 DOI: 10.1063/5.0286825

Charulatha Venkataraman

{"title":"Coherent modified Redfield approach to describe photoinduced proton-coupled electron transfer.","authors":"Charulatha Venkataraman","doi":"10.1063/5.0286825","DOIUrl":"https://doi.org/10.1063/5.0286825","url":null,"abstract":"Coherent modified Redfield theory is employed to describe photoinduced proton-coupled electron transfer for a model Hamiltonian. This formalism is an extension of Redfield theory to capture weak to moderate system-bath coupling strengths, and the dynamics is secular and non-Markovian. In the model Hamiltonian, the electron is coupled to the proton and a phonon bath and is initially photoinduced from the ground electronic site to a donor site. At small bath reorganization energies, the system parameters, such as the energy bias between the donor and acceptor sites and overlaps of the vibronic states, play a crucial role in influencing the population decay and isotope effect. The energy bias decides the spacing between adjacent pairs of donor-acceptor levels as well as the energetically favorable acceptor states for the non-adiabatic transition. For the models we considered, the overlaps of the donor-acceptor wavefunctions of the proton are larger than those of deuterium. When the population is initially distributed over several donor vibrational states, the H/D population decays faster for the case that has the smaller adjacent donor-acceptor spacing. The donor population decay shows an inverse isotope effect when this spacing is smaller for deuterium than for protons. These models demonstrate a subtle balance between the spacing and overlaps in deciding the rate of population decay. Weak electron-phonon coupling leads to coherent oscillations in the electronic population decay and proton wavepacket dynamics. Larger coupling strengths lead to wavepacket localization and the transition to incoherent population decay.","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":"144955556","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

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