The Journal of chemical physics最新文献_第7页

Adiabatic electronic flux in molecules and in condensed matter. 分子和凝聚态物质中的绝热电子通量。

The Journal of chemical physics Pub Date : 2022-05-11 DOI: 10.1063/5.0087883

R. Resta

引用次数: 0

A multiscale time-Laplace method to extract relaxation times from non-stationary dynamic light scattering signals. 从非平稳动态光散射信号中提取松弛时间的多尺度时间-拉普拉斯方法。

The Journal of chemical physics Pub Date : 2022-05-10 DOI: 10.1063/5.0088005

François Liénard, É. Freyssingeas, P. Borgnat

引用次数: 2

Bonding properties of molecular cerium oxides tuned by the 4f-block from ab initio perspective. 由4f-嵌段调整的铈氧化物分子的键合性质。

The Journal of chemical physics Pub Date : 2022-05-10 DOI: 10.1063/5.0090214

Ziyong Chen, J. Yang

引用次数: 4

A local mode study of ring puckering effects in the infrared spectra of cyclopentane. 环戊烷红外光谱中起皱效应的局部模态研究。

The Journal of chemical physics Pub Date : 2022-05-10 DOI: 10.1063/5.0095010

E. Sibert, P. Bernath

引用次数: 1

Femtosecond-to-millisecond mid-IR spectroscopy of photoactive yellow protein uncovers structural micro-transitions of the chromophore's protonation mechanism. 光活性黄色蛋白的飞秒-毫秒中红外光谱揭示了发色团质子化机制的结构微跃迁。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.1063/5.0091918

L. V. van Wilderen, L. Blankenburg, J. Bredenbeck

{"title":"Femtosecond-to-millisecond mid-IR spectroscopy of photoactive yellow protein uncovers structural micro-transitions of the chromophore's protonation mechanism.","authors":"L. V. van Wilderen, L. Blankenburg, J. Bredenbeck","doi":"10.1063/5.0091918","DOIUrl":"https://doi.org/10.1063/5.0091918","url":null,"abstract":"Protein structural dynamics can span many orders of magnitude in time. Photoactive yellow protein's (PYP) reversible photocycle encompasses picosecond isomerization of the light-absorbing chromophore as well as large scale protein backbone motions occurring on a millisecond timescale. Femtosecond-to-millisecond time-resolved mid-infrared spectroscopy is employed here to uncover structural details of photocycle intermediates up to chromophore protonation and the first structural changes leading to the formation of the partially unfolded signaling state pB. The data show that a commonly thought stable transient photocycle intermediate is actually formed after a sequence of several smaller structural changes. We provide residue-specific spectroscopic evidence that protonation of the chromophore on a few hundreds of microseconds timescale is delayed with respect to deprotonation of the nearby E46 residue. That implies that the direct proton donor is not E46 but most likely a water molecule. Such details may assist the ongoing photocycle and protein folding simulation efforts on the complex and wide time-spanning photocycle of the model system PYP.","PeriodicalId":446961,"journal":{"name":"The Journal of chemical physics","volume":"18 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2022-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"117088846","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 2

DFT investigations of KTiOPO4Mx (M = K, Na, and Li) anodes for alkali-ion battery. 用于碱性离子电池的 KTiOPO4Mx（M = K、Na 和 Li）阳极的 DFT 研究。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.2139/ssrn.4035322

Jiajia Huang, Xu Cai, Yanli Li, Zhongpu Fang, Yi Li, Wei-hui Lin, Shuping Huang, Yongfan Zhang

引用次数: 4

Temporal and chirp effects of laser pulses on the spectral line shape in sum-frequency generation vibrational spectroscopy. 和频产生振动光谱中激光脉冲的时间和啁啾效应对谱线形状的影响。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.1063/5.0088506

Hui Wang, Xiao-Hua Hu, Hong-fei Wang

{"title":"Temporal and chirp effects of laser pulses on the spectral line shape in sum-frequency generation vibrational spectroscopy.","authors":"Hui Wang, Xiao-Hua Hu, Hong-fei Wang","doi":"10.1063/5.0088506","DOIUrl":"https://doi.org/10.1063/5.0088506","url":null,"abstract":"Assignment and interpretation of the sum-frequency generation vibrational spectra (SFG-VS) depend on the ability to measure and understand the factors affecting the SFG-VS spectral line shape accurately and reliably. In the past, the formulation of the polarization selection rules for SFG-VS and the development of the sub-wavenumber high-resolution broadband SFG-VS (HR-BB-SFG-VS) have provided solutions for many of these needs. However, despite these advantages, HR-BB-SFG-VS have not been widely adopted. The majority of SFG measurements so far still relies on the picosecond (ps) scanning SFG-VS or the conventional broadband SFG-VS (BB-SFG-VS) with the spectral resolution around (mostly above) 10 cm-1, which also results in less ideal spectral line shape in the SFG spectra due to the temporal and chirp effects of the laser pulses used in experiment. In this study, the temporal and the chirp effects of laser pulses with different profiles in the SFG experiment on the measured SFG-VS spectral line shape are examined through spectral simulation. In addition, the experimental data of a classical model system, i.e., octadecyltrichlorosilane monolayer on glass, obtained from the ps scanning SFG-VS, the BB-SFG-VS, and the HR-BB-SFG-VS measurements are directly compared and examined. These results show that temporal and chirp effects are often significant in the conventional BB-SFG-VS, resulting in line shape distortions and peak position shifts besides spectral broadening. Such temporal and chirp effects are less significant in the ps scanning SFG-VS. For the HR-BB-SFG-VS, spectral broadening and temporal and chirp effects are insignificant, making HR-BB-SFG-VS the choice for accurate and reliable measurement and analysis of SFG-VS.","PeriodicalId":446961,"journal":{"name":"The Journal of chemical physics","volume":"28 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2022-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"129694734","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 5

Rotational excitation of NS+ by H2 revisited: A new global potential energy surface and rate coefficients. H2对NS+的旋转激发:一个新的全局势能面和速率系数。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.1063/5.0089745

C. Bop, Y. Kalugina, F. Lique

{"title":"Rotational excitation of NS+ by H2 revisited: A new global potential energy surface and rate coefficients.","authors":"C. Bop, Y. Kalugina, F. Lique","doi":"10.1063/5.0089745","DOIUrl":"https://doi.org/10.1063/5.0089745","url":null,"abstract":"Due to the lack of specific collisional data, the abundance of NS+ in cold dense interstellar clouds was determined using collisional rate coefficients of CS as a substitute. To better understand the chemistry of sulfur in the interstellar medium, further abundance modeling using the actual NS+ collisional rate coefficients is needed. For this purpose, we have computed the first full 4D potential energy surface of the NS+-H2 van der Waals complex using the explicitly correlated coupled cluster approach with single, double, and non-iterative triple excitation in conjunction with the augmented-correlation consistent-polarized valence triple zeta basis set. The potential energy surface exhibits a global minimum of 848.24 cm-1 for a planar configuration of the complex. The long-range interaction energy, described using multipolar moments, is sensitive to the orientation of H2 up to radial distances of ∼50 a0. From this new interaction potential, we derived excitation cross sections, induced by collision with ortho- and para-H2, for the 15 low-lying rotational levels of NS+ using the quantum mechanical close-coupling approach. By thermally averaging these data, we determined downward rate coefficients for temperatures up to 50 K. By comparing them with the previous NS+-H2 data, we demonstrated that reduced dimensional approaches are not suited for this system. In addition, we found that the CS collisional data underestimate our results by up to an order of magnitude. The differences clearly indicate that the abundance of NS+, in cold dense clouds retrieved from observational spectra, must be reassessed using these new collisional rate coefficients.","PeriodicalId":446961,"journal":{"name":"The Journal of chemical physics","volume":"10 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2022-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"128085881","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 1

Polymer informatics for QSPR prediction of tensile mechanical properties. Case study: Strength at break. 聚合物信息学用于拉伸力学性能的QSPR预测。案例研究:休息时的力量。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.1063/5.0087392

F. Cravero, M. Díaz, I. Ponzoni

{"title":"Polymer informatics for QSPR prediction of tensile mechanical properties. Case study: Strength at break.","authors":"F. Cravero, M. Díaz, I. Ponzoni","doi":"10.1063/5.0087392","DOIUrl":"https://doi.org/10.1063/5.0087392","url":null,"abstract":"The artificial intelligence-based prediction of the mechanical properties derived from the tensile test plays a key role in assessing the application profile of new polymeric materials, especially in the design stage, prior to synthesis. This strategy saves time and resources when creating new polymers with improved properties that are increasingly demanded by the market. A quantitative structure-property relationship (QSPR) model for tensile strength at break is presented in this work. The QSPR methodology applied here is based on machine learning tools, visual analytics methods, and expert-in-the-loop strategies. From the whole study, a QSPR model composed of five molecular descriptors that achieved a correlation coefficient of 0.9226 is proposed. We applied visual analytics tools at two levels of analysis: a more general one in which models are discarded for redundant information metrics and a deeper one in which a chemistry expert can make decisions on the composition of the model in terms of subsets of molecular descriptors, from a physical-chemical point of view. In this way, with the present work, we close a contribution cycle to polymer informatics, providing QSPR models oriented to the prediction of mechanical properties related to the tensile test.","PeriodicalId":446961,"journal":{"name":"The Journal of chemical physics","volume":"74 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2022-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"124806944","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 1

Note: Reproducibility of potential energy surfaces of organic/metal interfaces on the example of PTCDA on Ag(111). 注:以Ag(111)上PTCDA为例，有机/金属界面势能面再现性。

The Journal of chemical physics Pub Date : 2022-05-09 DOI: 10.1063/5.0094163

Lukas Hörmann, A. Jeindl, O. Hofmann

引用次数: 1