Physical Chemistry Chemical Physics最新文献_第3页

Magneto-optical properties of heavily Fe-doped GaAs: a density functional approach 重度铁掺杂砷化镓的磁光特性：一种密度泛函方法

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp03101f

Juliana Zarpellon, Dante Homero Mosca, J Varalda

引用次数: 0

Control of interlayer friction in two-dimensional ferromagnetic CrBr3 二维铁磁性 CrBr3 的层间摩擦控制

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp01520g

Xinyue Bi, Yushu Xu, Xinqi Zhang, Junqin Shi, Tengfei Cao, Feng Zhou, W. M. Liu, Xiaoli Fan

{"title":"Control of interlayer friction in two-dimensional ferromagnetic CrBr3","authors":"Xinyue Bi, Yushu Xu, Xinqi Zhang, Junqin Shi, Tengfei Cao, Feng Zhou, W. M. Liu, Xiaoli Fan","doi":"10.1039/d4cp01520g","DOIUrl":"https://doi.org/10.1039/d4cp01520g","url":null,"abstract":"Two-dimensional (2D) magnetic materials may offer new opportunities in the field of lubrication at nanoscale. It is essential to investigate the interfacial property, particularly magnetic coupling, at the interfaces of 2D magnetic materials from the point view of friction. In the present study, we investigated the tribological and interfacial properties at the interface of bilayer CrBr3 by performing the first-principles calculations. The effects of normal load, biaxial strain and carrier doping on the interlayer magnetic coupling were also studied. Our calculations identify the ferromagnetic (FM) - antiferromagnetic (AFM) conversion of the interlayer magnetic couplings, which leads to the reduction of the sliding energy barriers. Importantly, our calculations demonstrate the lower sliding energy barrier at the interface of 2D FM CrBr3, implying lower friction and better lubricating property. Additionally, we found that the normal load of 0.5 ~ 1.0 eV/Å, biaxial compressive strain of 0% ~ -5%, and carrier doping of -0.2 ~ 0.2 e f.u.-1 are effective on reducing the sliding energy barrier and the friction. It is also found that the biaxial strain tunes the interlayer electron redistribution, and thus alters the interlayer interaction and friction. The differences between the lubricating properties of 2D magnetic CrX3 (X = Cl, Br and I) have also been studied. The present findings are inspiring for the application of 2D magnetic materials as solid lubricant in the fields of lubrication at nanoscale.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443880","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 efficient triplet states formation of Se-modified PDI dimers and tetramers in solvents 在溶剂中高效形成 Se 修饰的 PDI 二聚体和四聚体的三重态

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp00954a

Feijun Huang, Wenli Su, Yubo Yang, Hang Wang, Pengfei Jing, Zhishan Bo, Wenkai Zhang

{"title":"The efficient triplet states formation of Se-modified PDI dimers and tetramers in solvents","authors":"Feijun Huang, Wenli Su, Yubo Yang, Hang Wang, Pengfei Jing, Zhishan Bo, Wenkai Zhang","doi":"10.1039/d4cp00954a","DOIUrl":"https://doi.org/10.1039/d4cp00954a","url":null,"abstract":"The triplet excited states of molecules play an important role in photophysical processes, which has attracted great research interest. Perylene diimide (PDI) is a widely studied material closely associated with the generation of triplet states, and it is highly anticipated to become an electron acceptor material for improving photovoltaic conversion efficiency. In this work, we prepared dimers and tetramers composed of selenium-modified PDI-C5 (N,N’-bis(6-undecyl) perylene-3,4,9,10-bis(dicarboximide)) units. We investigated the photophysical processes of these dimers and tetramers in chloroform and toluene using UV-visible absorption spectroscopy, fluorescence spectroscopy, and femtosecond transient absorption spectroscopy. Both the dimers and tetramers undergo efficient triplet state formation processes in the solvents. Solvents with higher polarity facilitate charge transfer thereby promote the triplet states formation. The differences in the configurations of the dimer and tetramer molecules lead to variations in triplet states generation. The twisted angles in the tetramer restricted the intramolecular electronic coupling, posing certain hindrances to exciton coupling and lowering the intramolecular CT characteristics. The emission of excimer in tetramers also competes with the triplet states formation. The research demonstrates the influence of various factors on the generation of triplet states of PDI oligomers.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443898","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Structural and Sorption Characterization of Aerogel Composite Material with Flufenamic acid: Insights from MAS NMR and High-Pressure NOESY Studies 氟灭酸气凝胶复合材料的结构和吸附特性：MAS NMR 和高压 NOESY 研究的启示

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp03217a

Valentina V. Sobornova, Valeriya V. Mulloyarova, Konstantin V. Belov, Alex Dyshin, Peter Tolstoy, Michael Grigorievich Kiselev, Ilya Khodov

{"title":"Structural and Sorption Characterization of Aerogel Composite Material with Flufenamic acid: Insights from MAS NMR and High-Pressure NOESY Studies","authors":"Valentina V. Sobornova, Valeriya V. Mulloyarova, Konstantin V. Belov, Alex Dyshin, Peter Tolstoy, Michael Grigorievich Kiselev, Ilya Khodov","doi":"10.1039/d4cp03217a","DOIUrl":"https://doi.org/10.1039/d4cp03217a","url":null,"abstract":"The structural and sorption characteristics of a composite material consisting of silica aerogel loaded with flufenamic acid were investigated using a variety of nuclear magnetic resonance techniques. The composite structure was analyzed using Magic angle spinning nuclear magnetic resonance NMR spectroscopy, which revealed significant interactions between the aerogel matrix and the FFA molecules. Solid-state ²⁹Si NMR provided insights into the aerogel’s stability, while ¹H and ¹³C NMR confirmed the presence of FFA in the matrix, with signals from FFA molecules observed alongside tetraethoxysilane (TEOS) groups. Ethanol-induced desorption of FFA led to narrowed spectral lines, suggesting the breaking of intermolecular hydrogen bonds. 19F MAS NMR spectra indicated changes in FFA local environments upon loading into AG pores. Evaluation of CO2 sorption characteristics using 13C NMR demonstrated a slower sorption rate for AG+FFA than pure AG, attributed to decreased pore volume. Furthermore, nnuclear Overhauser effect spectroscopy (NOESY) was employed to explore the conformational behavior of FFA within the aerogel matrix. The results indicated a shift in conformer populations, particularly those related to the rotation of one cyclic fragment relative to the other. These findings provide insights into the structural and sorption characteristics of AG+FFA composites, which are valuable for developing novel drug solid forms.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Behind the glow: unveiling the nature of NanoLuc reactants and products 光辉的背后：揭示 NanoLuc 反应物和产品的本质

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp02551b

Alessandro Bonardi, Michele Turelli, Giorgio Moro, Ugo Cosentino, Claudio Greco, Carlo Adamo

{"title":"Behind the glow: unveiling the nature of NanoLuc reactants and products","authors":"Alessandro Bonardi, Michele Turelli, Giorgio Moro, Ugo Cosentino, Claudio Greco, Carlo Adamo","doi":"10.1039/d4cp02551b","DOIUrl":"https://doi.org/10.1039/d4cp02551b","url":null,"abstract":"Due to the largely recognized utility of bioluminescence in many fields, a wide variety of luciferase-luciferin systems have been investigated in order to find the best-suited for a number of different applications. The collected knowledge has allowed the identification of a few necessary, or at least desirable, properties, such as bright luminescence, low background signal and small dimension of the enzyme that must exhibit structural stability at operating conditions. The NanoLuc-Furimazine pair seems to meet all these requirements, but the mechanism of the reaction and the characteristics of the species responsible for the emission remain unknown. The aim of this study is to identify the luminescent product among the possible forms of oxidized Furimazine and to understand how the chemical form and structure of the system, before and after the oxidation, are involved into the reaction mechanism and determine emission. To do this, we consider two possible forms of Furimazine, the keto and the enol one, and test which of them is the most plausible candidate in the bioluminescence process on the basis of enzyme-substrate geometries from docking calculations. A similar procedure is repeated for three possible forms of the Furimamide luminescent product, and their properties in the protein environment are then evaluated via QM/MM calculations. In contrast with previous indications, the simulations well support the involvement of the enol form of Furimazine as reagent and point to the zwitterionic or anionic forms of Furimamide as emissive species.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Surprising torsional barrier reduction in the coupled methyl internal rotations of 2,3-dimethylfuran observed by microwave spectroscopy 通过微波光谱观察 2,3-二甲基呋喃耦合甲基内旋过程中令人惊讶的扭转势垒降低现象

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp03338h

Mike Buttkus-Barth, Thi Ha Nguyen, Gregor Brannys, Arne Luechow, Ha Vinh Lam Nguyen

{"title":"Surprising torsional barrier reduction in the coupled methyl internal rotations of 2,3-dimethylfuran observed by microwave spectroscopy","authors":"Mike Buttkus-Barth, Thi Ha Nguyen, Gregor Brannys, Arne Luechow, Ha Vinh Lam Nguyen","doi":"10.1039/d4cp03338h","DOIUrl":"https://doi.org/10.1039/d4cp03338h","url":null,"abstract":"The microwave spectrum of 2,3-dimethylfuran was investigated using a Fourier-transform microwave spectrometer under supersonic expansion. The molecule possesses two inequivalent methyl internal rotors, causing the splitting of each rotational transition into five torsional species. A total of 337 torsional transitions were assigned and fitted in a global fit with the program XIAM, where accurate and physically meaningful geometry and internal rotation parameters could be deduced. The different torsional species were also fitted separately with the program SFLAMS to validate the assignment. Both the global fit and the separate fits achieved standard deviations close to the measurement accuracy. The barriers to internal rotation of the ortho- and meta-methyl rotors, which are in direct proximity, were determined to be 298.27 cm−1 and 237.69 cm−1, respectively. These values are radically lower than the respective barriers of 412.9 cm−1 and 380.5 cm−1 found for the steric-free methyl groups in 2-methylfuran and 3-methylfuran. This observation appears to be driven primarily by electrostatic effects rather than being adequately accounted for by steric effects. The experiments were accompanied by quantum mechanical calculations. Benchmarking the rotational constants revealed that the MP2/6-31G(d,p) level of theory might be helpful to guide the microwave spectral assignment of methylfuran derivatives.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Exploiting graph theory in MD simulations for extracting chemical and physical properties of materials 在 MD 模拟中利用图论提取材料的化学和物理特性

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp02764g

Sana Bougueroua, Alexander A. Kolganov, Chloé Helain, Coralie Zens, Dominique Barth, Evgeny A Pidko, Marie-Pierre Gaigeot

引用次数: 0

In Silico Validation of Allosteric Inhibitors Targeting Zika Virus NS2B-NS3 Proteases 针对寨卡病毒 NS2B-NS3 蛋白酶的异构抑制剂的硅学验证

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp02867h

Yeng-Tseng Wang, Yuan-Chin Hsieh, Tin-Yu Wu

{"title":"In Silico Validation of Allosteric Inhibitors Targeting Zika Virus NS2B-NS3 Proteases","authors":"Yeng-Tseng Wang, Yuan-Chin Hsieh, Tin-Yu Wu","doi":"10.1039/d4cp02867h","DOIUrl":"https://doi.org/10.1039/d4cp02867h","url":null,"abstract":"Zika virus (ZIKV), a member of the Flaviviridae family, is a pressing concern due to the lack of effective antiviral drugs. The NS2B-NS3 protease of ZIKV is currently the major target protein for antiviral inhibitors. However, viral mutations can lead to the ineffectiveness of competitive inhibitors. Allosteric inhibitors bind to highly conserved non-protease active sites and cause conformational changes in the protease active site, preventing substrate binding. No molecular simulation methods can fully predict and analyze conformational changes in the protease catalytic domain. Therefore, we propose a combined approach that includes blind docking, Gaussian accelerated molecular dynamics (GaMD), 2D potential of mean force (PMF) profiling, density functional theory (DFT) calculations, and interaction region indicator (IRI) analysis to study the allosteric inhibitor-01 molecule and its interaction with the NS2B-NS3 protease. Our results show that the binding of inhibitor-01 to the protease leads to two major conformational states, I and II. These states cause the volume of the protease active site to change from the original 1014 Å³ to 710 Å³ and 820 Å³, respectively. Further analysis using DFT and IRI reveals that in the state I structure, Lys138 and Gln139 form hydrogen bonds with inhibitor-01, and inhibitor-01 engages in van der Waals interactions with Lys138, Leu214, Asn217, Val220, and Ile221. Advancements in computational methods and computing power are expected to facilitate further progress in overcoming challenges in designing allosteric inhibitors for viral proteases.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142443882","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Experimental and theoretical investigation of the Auger electron spectra of isothiocyanic acid, HNCS 异硫氰酸 HNCS 的奥杰电子能谱的实验和理论研究

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp03104k

Dorothee Schaffner, Marius Gerlach, Emil Karaev, John Bozek, Ingo Fischer, Reinhold F Fink

{"title":"Experimental and theoretical investigation of the Auger electron spectra of isothiocyanic acid, HNCS","authors":"Dorothee Schaffner, Marius Gerlach, Emil Karaev, John Bozek, Ingo Fischer, Reinhold F Fink","doi":"10.1039/d4cp03104k","DOIUrl":"https://doi.org/10.1039/d4cp03104k","url":null,"abstract":"We investigate isothiocyanic acid, HNCS, by resonant and nonresonant Auger electron spectroscopy at the K-edge of carbon and nitrogen, and the L2,3-edge of sulfur, employing soft X-ray synchrotron radiation. The C1s and N1s ionization energies as well as the S2s and S2p ionization energies are determined and X-ray absorption spectra reveal the transitions from the core to the virtual orbitals. Final states for all normal Auger electron spectra and the resonant ones recorded at the carbon and nitrogen edge are assigned and rationalized with theoretical spectra obtained with a wave-function based protocol. The latter is based on ab initio configuration-interaction representations of the bound part of the electronic wave functions, the one-center approximation for Auger intensities, and a moment theory for band shapes. The computed spectra are in very good agreement with the experimental data and most of the relevant signals are assigned. The double ionization energy is derived from the S2p1/2 spectrum and in good agreement with a recently determined value. The Auger electron spectra are compared with those of the congener HNCO. A similar shape of the normal Auger electron spectra was found for the low binding energy final states, while intensities differed. Similarities are less pronounced in the resonant Auger electron spectra.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Spintronic performance of bent zigzag phosphorene nanoribbons: eﬀects of mechanical deformation and gate voltage 弯曲之字形磷烯纳米带的自旋电子性能：机械变形和栅极电压的影响

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-17 DOI: 10.1039/d4cp03470h

Rouhollah Farghadan

引用次数: 0