Physical Chemistry Chemical Physics最新文献_第9页

Fluoranthene Imide Dimers with Strong Isomeric Effects on the Charge Transport Properties 对电荷传输特性具有强烈异构效应的荧蒽酰亚胺二聚体

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp03245d

Ting-Yu Wang, Huangcheng Liu, Miao Liu, Yen-Han Shih, Xinyu Yu, Zhong'an Li, Chu-Chen Chueh

引用次数: 0

Fluorescence and absorption of Rhodamine 6G solutions as pressure standards for a diamond-anvil cell 罗丹明 6G 溶液的荧光和吸收作为金刚石振荡池的压力标准

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp03351e

Ida Moszczyńska, Anna Golczak, Marek Sikorski, Andrzej Katrusiak

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Cryptate Binding Energies Towards High Throughput Chelator Design: Metadynamics Ensembles with Cluster-Continuum Solvation 实现高通量螯合剂设计的隐子结合能：具有簇连续求解的元动力学集合

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp03129f

Sean Nations, Lauren Burrows, Scott Crawford, Wissam Saidi

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The role of density functional theory in decoding the complexities of hydrogen embrittlement in steels 密度泛函理论在破解钢中氢脆复杂性方面的作用

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp02233e

Assa Aravindh Sasikala Devi, Vahid Javaheri, Sakari Pallaspuro, Jukka Kömi

{"title":"The role of density functional theory in decoding the complexities of hydrogen embrittlement in steels","authors":"Assa Aravindh Sasikala Devi, Vahid Javaheri, Sakari Pallaspuro, Jukka Kömi","doi":"10.1039/d4cp02233e","DOIUrl":"https://doi.org/10.1039/d4cp02233e","url":null,"abstract":"Hydrogen (H) is considered as the key element in aiding the initiated green energy transition. To facilitate this, efficient and durable technologies need to be developed for the generation, storage, transportation, and use of H. All these value chain stages require materials that can withstand continuous exposure to H, as once absorbed it can eventually concentrate to critical levels in a stressed microstructure, inducing specific damage mechanisms and consecutive loss of mechanical properties. This is known as hydrogen embrittlement (HE). Being one of the most significant structural material types, steels are widely used throughout the H value chain. They can suffer from HE, and attempts are made towards understanding and mitigating this complex phenomenon. While originating at a size scale of atoms, HE acts on multiple spatio-temporal scales, and comined efforts of experimental and modelling techniques are needed to deal with it. This perspective is devoted to assimilating the knowledge that can be generated by density functional theory (DFT) methods to understand interactions between H and iron-based materials, and to promote finding solutions to HE in metallic materials in general. We aim to provide a comprehensive understanding of the properties calculated using DFT that can help advance finding novel H resistant high-strength materials that facilitate the green shift at sufficient performance levels to meet the future needs.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142385042","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

Observation of metastable structures of the dimer of ethylene glycol with water in helium nanodroplets 观察氦纳米液滴中乙二醇与水的二聚体的瞬变结构

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp02899f

Daniel William Polak, Lewis J. P. Turnbull, Owen D. Bass, Shengfu Yang, Andrew M Ellis

引用次数: 0

Theoretical Elucidation of the Effect of Linkage and Orientation of Carbazole on the Naphthalenediimide and the TADF and RTP Propensity 从理论上阐明咔唑的连接和取向对萘二亚胺以及 TADF 和 RTP 倾向的影响

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp02636e

CHETAN SAINI, Siddan Gouthaman, K. R. Justin Thomas

{"title":"Theoretical Elucidation of the Effect of Linkage and Orientation of Carbazole on the Naphthalenediimide and the TADF and RTP Propensity","authors":"CHETAN SAINI, Siddan Gouthaman, K. R. Justin Thomas","doi":"10.1039/d4cp02636e","DOIUrl":"https://doi.org/10.1039/d4cp02636e","url":null,"abstract":"Thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) are most promising technologies for harvesting triplet excitons in organic emitters. In this work, the effect of connection modes between carbazole (Cz) donor (D) and naphthalene diimide (NDI) acceptor (A) on the TADF and RTP propensities are elucidated using the density functional theoretical computations using D-A, D-A-D, D-π-A, and D-π-A-π-D structural designs. The relationship of the dihedral angle between donor and acceptor units, with the spin orbit coupling (SOC) values, the energy difference between the singlet-triplet excited states (ΔEST), radiative (kr), inter-system crossing (kISC) and reverse inters system crossing (kRISC) rates are obtained. The molecules possessing direct linkage between Cz and NDI exhibit large energy difference between the lowest singlet and triplet excited states (ΔEST) due to substantial overlap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). However, the incorporation of phenyl spacer between the Cz and NDI units led to the separation of HOMO and LUMO and consequently resulted in small ΔEST. Furthermore, the presence of two donors with and without a phenyl spacer on NDI results in high-lying triplet states that are energetically lower than the lowest singlet excited state, hence providing additional channels to the TADF and RTP process. Additionally, the orientation of Cz and NDI in ortho positions of the phenyl unit resulted in a T1 state with dominant LE character which led to large spin-orbit coupling constants and kr than the analogous meta and para-linked derivatives. Overall, the compounds containing phenyl linkage are expected to have high TADF propensity than the directly linked derivatives.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142384379","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

Hydrogen-designed spin-states of 2D silicon carbide and graphene nanostructures 二维碳化硅和石墨烯纳米结构的氢设计自旋态

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp02762k

L. Fiorini Filho, Wallace P. Morais, Nathanael Nardoto Batista, Fábio A. L. de Souza, Antonio J. C. Varandas, W. S. Paz, Fernando Nespoli Nassar Pansini

{"title":"Hydrogen-designed spin-states of 2D silicon carbide and graphene nanostructures","authors":"L. Fiorini Filho, Wallace P. Morais, Nathanael Nardoto Batista, Fábio A. L. de Souza, Antonio J. C. Varandas, W. S. Paz, Fernando Nespoli Nassar Pansini","doi":"10.1039/d4cp02762k","DOIUrl":"https://doi.org/10.1039/d4cp02762k","url":null,"abstract":"Identifying and manipulating spin in two-dimensional materials is of great interest in advancing quantum information and sensing technologies, as well as in the development of spintronic devices. Here, we investigate the influence of hydrogen adsorption on the electronic and magnetic properties of graphene-like triangulenes. We have constructed triangulenes from SiC monolayers, which have been successfully synthesized very recently, extending our investigation to include graphene triangulenes. This advancement in the synthesis of SiC monolayers allows us to investigate deeper into the unique properties of SiC-based triangulenes and compare them with their graphene counterparts. The addition of hydrogen has been found to induce a magnetic moment in the SiC monolayer, with a more localized spin density when H is adsorbed in the C sites while spreading through the lattice when adsorbed on the Si sites. In triangular flakes, the ground spin state changes with the adsorption site: decreasing multiplicity on edge-defined sublattices and increasing it on the opposite sublattice. These findings suggest hydrogen adsorption as a tool for tuning spin-state properties in SiC and graphene nanostructures, with potential applications in spintronics and spin quantum dot devices.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142384325","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

Ultrasensitive detection of a responsive fluorescent thymidine analogue in DNA via pulse-shaped two-photon excitation 通过脉冲型双光子激发技术超灵敏检测 DNA 中的反应性荧光胸苷类似物

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp03391d

Steven Magennis, Alexandra E Bailie, Henry G Sansom, Rachel S S Fisher, Ryo Watabe, Yitzhak Tor, Anita C Jones

{"title":"Ultrasensitive detection of a responsive fluorescent thymidine analogue in DNA via pulse-shaped two-photon excitation","authors":"Steven Magennis, Alexandra E Bailie, Henry G Sansom, Rachel S S Fisher, Ryo Watabe, Yitzhak Tor, Anita C Jones","doi":"10.1039/d4cp03391d","DOIUrl":"https://doi.org/10.1039/d4cp03391d","url":null,"abstract":"Fluorescent base analogues (FBAs) are versatile nucleic acid labels that can replace a native nucleobase, while maintaining base pairing and secondary structure. Following the recent demonstration that free FBAs can be detected at the single-molecule level, the next goal is to achieve this level of detection sensitivity in oligonucleotides. Due to the short-wavelength absorption of most FBAs, multiphoton microscopy has emerged as a promising approach to single-molecule detection. We report the multiphoton-induced fluorescence of 5-(5-(4-methoxyphenyl)thiophen-2-yl)-6-aza-uridine (MeOthaU), a polarity-sensitive fluorescent thymidine analogue, as a nucleoside, and in two single-stranded deoxyribo-oligonucleotides, with and without their complement strands. Ensemble steady-state and time-resolved measurements in dioxane, following one-photon and two-photon excitation, reveals both strongly and weakly emissive species, assigned as rotamers, while in Tris buffer there are additional non-emissive states, which are attributed to tautomeric forms populated in aqueous environments. The two-photon (2P) brightness for MeOthaU is highest as the free nucleoside in dioxane (10 GM) and lowest as the free nucleoside in Tris buffer (0.05 GM). The species-averaged 2P brightness values in DNA are higher for the single strands (0.66 and 0.82 GM for sequence context AXA and AXT, respectively, where X is MeOthaU) than in the duplex (0.31 and 0.25 GM for AXA and AXT, respectively). Using 2P microscopy with pulse-shaped broadband excitation, we were able to detect single- and double-stranded oligos with a molecular brightness of 0.8-0.9 kHz per molecule. This allowed the detection of as few as 7 DNA molecules in the focus, making it the brightest responsive FBA in an oligonucleotide reported to date.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142384323","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

Water adsorption at the (010) and (101) surfaces of CuWO4 水在 CuWO4 (010) 和 (101) 表面的吸附情况

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/d4cp02699c

Xuan Chu, David Santos-Carballal, Nora Henriette De Leeuw

{"title":"Water adsorption at the (010) and (101) surfaces of CuWO4","authors":"Xuan Chu, David Santos-Carballal, Nora Henriette De Leeuw","doi":"10.1039/d4cp02699c","DOIUrl":"https://doi.org/10.1039/d4cp02699c","url":null,"abstract":"Copper tungstate (CuWO4) has attracted significant attention over the past two decades due to its performance as an electro-photocatalyst for water splitting, with many studies focusing on its structural, electronic, and the redox properties. However, the adsorption of water onto CuWO4, which plays a critical role in the photocatalytic water splitting process, has not been investigated in detail. In this study, we have employed density functional theory (DFT) calculations to investigate water adsorption onto the CuWO4 pristine (010) and reduced (101) surfaces. The charge transfer for each mode of adsorption was calculated after optimization. Adsorption of multiple water molecules was simulated based on the single water adsorption system. We have calculated the electronic properties, Bader atomic charges, adsorption energies, surface free energies, work functions, and band gaps at each coverage of H2O on both surfaces. The surface phase diagrams as a function of the temperature and partial pressure of H2O were also configured to determine water coverage under particular environmental conditions. Our study provides a comprehensive understanding of the adsorption of water on the major CuWO4 surfaces, which is an important preliminary step in our investigation of photocatalytic water splitting over CuWO4.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142384330","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

Reaction pathways leading to HPALD intermediates in the OH-initiated oxidation of isoprene† 异戊二烯在羟基引发的氧化过程中产生 HPALD 中间体的反应途径

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-08 DOI: 10.1039/D4CP02106A

Péter Szabó, Zhen Liu, Jean-François Müller, Jeremy N. Harvey and Jozef Peeters

{"title":"Reaction pathways leading to HPALD intermediates in the OH-initiated oxidation of isoprene†","authors":"Péter Szabó, Zhen Liu, Jean-François Müller, Jeremy N. Harvey and Jozef Peeters","doi":"10.1039/D4CP02106A","DOIUrl":"10.1039/D4CP02106A","url":null,"abstract":"In this study, we revisited the mechanism of isoprene oxidation by OH radicals, focusing on the formation of hydroperoxyaldehydes (HPALDs) in the reactions following O2-addition at the α-position to Z,Z′-OH-allyl radical products of the 1,6-H shift of the 1st-generation Z-δ-OH-isoprenylperoxy radicals. Utilizing high-level ab initio quantum chemical calculations and a master equation approach, we provide theoretical confirmation that the formation of δ-HPALDs dominates by far and show that production of β-HPALDs by the mechanism proposed by Wennberg et al. (Chem. Rev., 2018, 118, 3337–3390) is negligible. Besides the dominance of the δ-HPALD formation channel, our investigation also reveals a novel though minor reaction channel resulting in the formation of an allylic δ-hydroperoxy acid and OH radical. Of primary importance for the assessment of the respective channels is the identification of a chemically activated mechanism driving the δ-HPALD formation process under atmospheric conditions. Different from traditional thermally activated pathways, we found that the rovibrationally hot peroxy radicals resulting from O2 addition to Z,Z′-OH-allyl radicals undergo prompt rearrangement and decomposition at a rate faster than their collisional relaxation, predominantly yielding δ-HPALDs in a chemically activated manner with high efficiency under atmospheric conditions.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":2.9,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/cp/d4cp02106a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142385011","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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