Journal of Chemical Physics最新文献_第4页

Modeling solvation dynamics of transition metal redox ion through on-the-fly multi-objective Bayesian-optimized force field. 通过实时多目标贝叶斯优化力场模拟过渡金属氧化还原离子的溶解动力学。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0225520

Yuchi Chen, Qiangqiang Huang, Te-Huan Liu, Ronggui Yang, Xin Qian

{"title":"Modeling solvation dynamics of transition metal redox ion through on-the-fly multi-objective Bayesian-optimized force field.","authors":"Yuchi Chen, Qiangqiang Huang, Te-Huan Liu, Ronggui Yang, Xin Qian","doi":"10.1063/5.0225520","DOIUrl":"https://doi.org/10.1063/5.0225520","url":null,"abstract":"Modeling solvation dynamics and properties is crucial for developing electrolytes for electrochemical energy storage and conversion devices. This work reports an on-the-fly multi-objective Bayesian optimization (OTF-MOBO) method to parameterize force fields for modeling ionic solvation structures, thermodynamics, and transport properties using molecular dynamics simulations. By leveraging solvation-free energy and solvation radii as training data, we employ the data-driven OTF-MOBO algorithm to actively optimize the force field parameters. The modeling accuracy was evaluated in molecular dynamics simulations until the Pareto front in the parameter space was reached through minimized prediction errors in both solvation-free energy and solvation radii. Using transition metal redox ions (Fe3+/Fe2+, Cr3+/Cr2+, and Cu2+/Cu+) in aqueous solution as examples, we demonstrate that simple force fields combining the Lenard-Jones potential and Coulombic potential can achieve relative error below 2% in both solvation free energy and solvation radii. The optimized force fields can be further extrapolated to predict solvation entropy and diffusivities with relative error below 10% compared with experiments.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347509","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

Molecular influence on nuclear-quadrupole-coupling effects in laser induced alignment. 分子对激光诱导排列中核四极耦合效应的影响。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0231814

Linda V Thesing, Andrey Yachmenev, Rosario González-Férez, Jochen Küpper

引用次数: 0

Nonlinear Langevin functionals for a driven probe. 驱动探针的非线性朗格文函数。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0227674

Juliana Caspers, Matthias Krüger

{"title":"Nonlinear Langevin functionals for a driven probe.","authors":"Juliana Caspers, Matthias Krüger","doi":"10.1063/5.0227674","DOIUrl":"https://doi.org/10.1063/5.0227674","url":null,"abstract":"When a probe particle immersed in a fluid with nonlinear interactions is subject to strong driving, the cumulants of the stochastic force acting on the probe are nonlinear functionals of the driving protocol. We present a Volterra series for these nonlinear functionals by applying nonlinear response theory in a path integral formalism, where the emerging kernels are shown to be expressed in terms of connected equilibrium correlation functions. The first cumulant is the mean force, the second cumulant characterizes the non-equilibrium force fluctuations (noise), and higher order cumulants quantify non-Gaussian fluctuations. We discuss the interpretation of this formalism in relation to Langevin dynamics. We highlight two example scenarios of this formalism. (i) For a particle driven with the prescribed trajectory, the formalism yields the non-equilibrium statistics of the interaction force with the fluid. (ii) For a particle confined in a moving trapping potential, the formalism yields the non-equilibrium statistics of the trapping force. In simulations of a model of nonlinearly interacting Brownian particles, we find that nonlinear phenomena, such as shear-thinning and oscillating noise covariance, appear in third- or second-order response, respectively.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347514","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

Optical force and torque in near-field excitation of C3H6: A first-principles study using RT-TDDFT. 近场激发 C3H6 时的光学力和扭矩：利用 RT-TDDFT 进行的第一原理研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0223371

Risa Amano, Daisuke Nishizawa, Tetsuya Taketsugu, Takeshi Iwasa

{"title":"Optical force and torque in near-field excitation of C3H6: A first-principles study using RT-TDDFT.","authors":"Risa Amano, Daisuke Nishizawa, Tetsuya Taketsugu, Takeshi Iwasa","doi":"10.1063/5.0223371","DOIUrl":"https://doi.org/10.1063/5.0223371","url":null,"abstract":"Optical trapping is an effective tool for manipulating micrometer-sized particles, although its application to nanometer-sized particles remains difficult. The field of optical trapping has advanced significantly, incorporating more advanced techniques such as plasmonic structures. However, single-molecule trapping remains a challenge. To achieve a deeper understanding of optical forces acting on molecular systems, a first-principles approach to analyze the optical force on molecules interacting with a plasmonic field is crucial. In our study, the optical force and torque induced by the near-field excitation of C3H6 were investigated using real-time time-dependent density functional theory calculations on real-space grids. The near field from the scanning tunneling probe was adopted as the excitation source for the molecule. The optical force was calculated using the polarization charges induced in the molecule based on Lorentz force. While the optical force and torque calculated as functions of the light energy were in moderate agreement with the oscillator strengths obtained from the far-field excitation of C3H6, a closer correspondence was achieved with the power spectrum of the induced dipole moment using near-field excitation. Time-domain analysis of the optical force suggests that the simultaneous excitation of multiple excited states generally weakens the force because of mismatches between the directions of the induced polarization and the electric field. This study revealed a subtle damping mechanism for the optical force arising from intrinsic electronic states and the influence of beating.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347516","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

Imaging study of O3 photodissociation in the Huggins band. 哈金斯波段中 O3 光解离的成像研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0230902

Nicholas J Shuber, Megan E Fast, Simon W North

{"title":"Imaging study of O3 photodissociation in the Huggins band.","authors":"Nicholas J Shuber, Megan E Fast, Simon W North","doi":"10.1063/5.0230902","DOIUrl":"https://doi.org/10.1063/5.0230902","url":null,"abstract":"We report a velocity-mapped ion imaging study of the photodissociation of O3 in the Huggins band. The O(3PJ) images show evidence for three electronic channels producing O2(X3Σg-), O2(a1∆g), and O2(b1Σg+) state fragments, with the latter two arising from the spin-forbidden photodissociation of O3. Forward convolution simulations of the derived total translational energy distributions permit extraction of the vibrational state distribution for each O2 electronic state. All these distributions peak near v = 0 and decrease monotonically with the vibrational state. The wavelength-dependent branching of the three electronic channels has been determined and is approximately constant over the wavelength region studied (322-328 nm). We have observed that the O2 electronic state branching ratios depend on the coincident O(3PJ) spin-orbit state, and the O2(b1Σg+) state is particularly sensitive. These results are qualitatively consistent with previous calculations on the coupling of the initially excited state to dissociative states by Rosenwaks and Grebenshchikov [J. Phys. Chem. A. 114, 9809-9819 (2010)]. The spatial anisotropy of the three dissociation channels has been determined through analysis of the O(3P0) angular distributions. The results are consistent with recent calculations but differ from previous experimental reports. The experimental results provide detailed information on the dissociation dynamics and should motivate new calculations.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347503","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

Temperature behavior of the velocity autocorrelation function in large MD models of water. 大型水 MD 模型中速度自相关函数的温度行为。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0227272

A V Anikeenko, Yu I Naberukhin

{"title":"Temperature behavior of the velocity autocorrelation function in large MD models of water.","authors":"A V Anikeenko, Yu I Naberukhin","doi":"10.1063/5.0227272","DOIUrl":"https://doi.org/10.1063/5.0227272","url":null,"abstract":"Velocity autocorrelation functions (VACFs) were calculated using the molecular dynamics method in the TIP4P/2005 and SPC/E water models of 157 464 molecules at temperatures ranging from 250 to 370 K. The large size of the models and the high accuracy of the calculations allow us to reliably compute the long-time tails of the VACFs, showing that they systematically change shape from hydrodynamic (argon-like) at high temperatures to that typical of supercooled liquids at low temperatures. These tails in the range of 2-10 ps can be well fitted by a combination of two power functions: At-3/2 - Bt-β (A, B > 0, β ≈ 2). It is found that the amplitude of the hydrodynamic asymptote, A, approaches zero as the temperature decreases, thereby rendering the negative power-law decay,-Bt-2, the dominant term within the specified time interval. The presence of a negative -Bt-2 decay in the time interval of 2-10 ps determines the specific shape of the VACF long-time tail of water, distinguishing it from ordinary simple liquids. The amplitude B, which is always non-zero, demonstrates a slight increase with rising temperature. At medium temperatures, weak but well-defined damped oscillations are observed on the VACF in the 0.5-2 ps interval.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347521","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

Investigation on the vibrational relaxation and ultrafast electronic dynamics of S1 state in 2,4-difluoroanisole. 关于 2,4-二氟苯甲醚 S1 态振动弛豫和超快电子动力学的研究。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0231264

Ling Cao, Yanmei Wang, Xin Lu, Song Zhang

引用次数: 0

Influence of interstitial cluster families on post-synthesis defect manipulation and purification of oxides using submerged surfaces. 间隙团簇家族对合成后缺陷处理和利用浸没表面提纯氧化物的影响。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0230224

Heonjae Jeong, Edmund G Seebauer

{"title":"Influence of interstitial cluster families on post-synthesis defect manipulation and purification of oxides using submerged surfaces.","authors":"Heonjae Jeong, Edmund G Seebauer","doi":"10.1063/5.0230224","DOIUrl":"https://doi.org/10.1063/5.0230224","url":null,"abstract":"Injection of interstitial atoms by specially prepared surfaces submerged in liquid water near room temperature offers an attractive approach for post-synthesis defect manipulation and isotopic purification in device structures. However, this approach can be limited by trapping reactions that form small defect clusters. The compositions and dissociation barriers of such clusters remain mostly unknown. This communication seeks to address this gap by measuring the dissociation energies of oxygen interstitial traps in rutile TiO2 and wurtzite ZnO exposed to liquid water. Isotopic self-diffusion measurements using 18O, combined with progressive annealing protocols, suggest the traps are small interstitial clusters with dissociation energies ranging from 1.3 to 1.9 eV. These clusters may comprise a family incorporating various numbers, compositions, and configurations of O and H atoms; however, in TiO2, native interstitial clusters left over from initial synthesis may also play a role. Families of small clusters are probably common in semiconducting oxides and have several consequences for post-synthesis defect manipulation and purification of semiconductors using submerged surfaces.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347505","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

Dissociative electron attachment and Ar+ reaction with chromium hexacarbonyl, 296-400 K. 离解电子附着和 Ar+与六羰基铬的反应，296-400 K。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0232322

Thomas M Miller, Virginia G Rodriguez, Shaun G Ard, Albert A Viggiano, Nicholas S Shuman

引用次数: 0

Measurement and assignment of J = 5 to 9 rotational energy levels in the 9070-9370 cm-1 range of methane using optical frequency comb double-resonance spectroscopy. 使用光频梳双共振光谱法测量和分配甲烷 9070-9370 cm-1 范围内的 J = 5 至 9 旋转能级。

IF 3.1 2区化学

Journal of Chemical Physics Pub Date : 2024-09-28 DOI: 10.1063/5.0223447

Adrian Hjältén, Vinicius Silva de Oliveira, Isak Silander, Andrea Rosina, Michael Rey, Lucile Rutkowski, Grzegorz Soboń, Kevin K Lehmann, Aleksandra Foltynowicz

{"title":"Measurement and assignment of J = 5 to 9 rotational energy levels in the 9070-9370 cm-1 range of methane using optical frequency comb double-resonance spectroscopy.","authors":"Adrian Hjältén, Vinicius Silva de Oliveira, Isak Silander, Andrea Rosina, Michael Rey, Lucile Rutkowski, Grzegorz Soboń, Kevin K Lehmann, Aleksandra Foltynowicz","doi":"10.1063/5.0223447","DOIUrl":"https://doi.org/10.1063/5.0223447","url":null,"abstract":"We use optical-optical double-resonance spectroscopy with a continuous wave (CW) pump and a cavity-enhanced frequency comb probe to measure the energy levels of methane in the upper part of the triacontad polyad (P6) with higher rotational quantum numbers than previously assigned. A high-power CW optical parametric oscillator, tunable around 3000 cm-1, is consecutively locked to the P(7, A2), Q(7, A2), R(7, A2), and Q(6, F2) transitions in the ν3 band, and a comb covering the 5800-6100 cm-1 range probes sub-Doppler ladder-type transitions from the pumped levels with J' = 6 to 8, respectively. We report 118 probe transitions in the 3ν3 ← ν3 spectral range with uncertainties down to 300 kHz (1 × 10-5 cm-1), reaching 84 unique final states in the 9070-9370 cm-1 range with rotational quantum numbers J between 5 and 9. We assign these states using combination differences and by comparison with theoretical predictions from a new ab initio-based effective Hamiltonian and dipole moment operator. This is the first line-by-line experimental verification of theoretical predictions for these hot-band transitions, and we find a better agreement of transition wavenumbers with the new calculations compared to the TheoReTS/HITEMP and ExoMol databases. We also compare the relative intensities and find an overall good agreement with all three sets of predictions. Finally, we report the wavenumbers of 27 transitions in the 2ν3 spectral range, observed as V-type transitions from the ground state, and compare them to the new Hamiltonian, HITRAN2020, ExoMol, and the WKMLC line lists.","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.1,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142347508","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