化学•材料最新文献

{"title":"","authors":"Siyu Hou, Qin Yu, Xiya Peng, Shufang Gao and Jian Luo*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 26","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpcb.5c03440","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"","authors":"Zhiyin Huang, Yue Chen, Jiefen Yu, Haiyi Wang, Ning Wang, Lei Du*, Lixin Xing* and Siyu Ye*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"129 26","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":3.3,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpcc.5c02561","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535298","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}

{"title":"","authors":"Marcus T. Cicerone*, Jessica Z. Dixon, John P. Stoppelman, Kelly Badilla-Nunez and Jesse G. McDaniel*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 26","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":2.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpcb.5c01033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535310","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"","authors":"Valentina V. Sobornova, Valeriya V. Mulloyarova, Konstantin V. Belov, Alexey A. Dyshin, Peter M. Tolstoy, Michael G. Kiselev and Ilya A. Khodov*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 26","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01303","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"","authors":"Sheraz Ahmed, Jiwon An, Muhammad Zubair, Ho-Jung Sun, Joongpyo Shim* and Gyungse Park*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 26","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":4.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c01560","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535347","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of Chemistry-Inspired Dynamic Ansatz Utilizing Generative Machine Learning.","authors":"Sonaldeep Halder, Kartikey Anand, Rahul Maitra","doi":"10.1021/acs.jpca.5c02346","DOIUrl":"10.1021/acs.jpca.5c02346","url":null,"abstract":"<p><p>Generative machine learning models like the Restricted Boltzmann Machine (RBM) provide a practical approach for ansatz construction within the quantum computing framework. This work introduces a method that efficiently leverages RBM and many-body perturbative measures to build a compact chemistry-inspired ansatz for determining accurate molecular energetics. By training on low-rank determinants derived from an approximate wave function, RBM predicts the key high-rank determinants that dominate the ground-state wave function. A shallow depth ansatz is constructed to explicitly incorporate these dominant determinants after dynamically decomposing them into low-rank components and applying many-body perturbative measures for further screening. The method requires no additional measurements beyond the initial training phase. Moreover, it incorporates Bayesian hyperparameter optimization for the RBM, ensuring efficient performance with minimal training data during its limited usage. This approach facilitates the efficient computation of molecular properties, paving the way for exploring new chemical phenomena with near-term quantum computers.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":"5889-5900"},"PeriodicalIF":2.7,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144315490","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}

{"title":"Diboron-Doped Perylene-Based Polycyclic Aromatic Hydrocarbons for Enhancing Charge Transport: A Theoretical Perspective.","authors":"Rui Wang, Gui-Ya Qin, Xiao-Qi Sun, Hui-Yuan Li, Jing-Fu Guo, Lu-Yi Zou, Ai-Min Ren","doi":"10.1021/acs.jpca.5c00547","DOIUrl":"10.1021/acs.jpca.5c00547","url":null,"abstract":"<p><p>The enhancement of the optoelectronic properties of organic conjugation materials through boron doping may reshape current understanding, with boron-doped polycyclic aromatic hydrocarbons (PAHs) poised to be high-performance organic optoelectronic materials. However, the impact of boron doping on charge transport remains underexplored. In this study, the effects of diboron doping, including both dense and dispersed doping, along with further π-extension on the electronic structure, stacking pattern, and charge transport of perylene-based PAHs were systematically investigated using density-functional theory. The results indicate that diboron doping can switch the molecular packing from herringbone to π-stacking, which increases the transfer integrals and significantly improves the mobility. Furthermore, it is revealed that intermolecular B···B and B···C interactions promote the formation of π-π stacking by symmetry-adapted perturbation theory and Hirshfeld surface analysis. In addition, densely doped B₂-TBPA exhibits a one-dimensional intrinsic hole mobility of up to 40.86 cm² V^-1 s^-1, while B₂-HBP with π-extension and dispersed diboron doping exhibits pitched-π stacking, allowing it to display potential for bipolar transport. Monte Carlo and molecular dynamics simulations further demonstrate that diboron-doped PAHs offer more stable charge transport with reduced thermal disorder. This research provides new insights for the experimental design and synthesis of high-performance organic semiconductor devices.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":"5722-5736"},"PeriodicalIF":2.7,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144315491","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}

{"title":"Free Energies of Solvation in Benzene and Hexafluorobenzene: Is Explicit Polarization Needed?","authors":"William L Jorgensen, Julian Tirado-Rives","doi":"10.1021/acs.jpcb.5c02405","DOIUrl":"10.1021/acs.jpcb.5c02405","url":null,"abstract":"<p><p>Free energies of solvation in liquid benzene and hexafluorobenzene have been computed for 42 uncharged solutes. Monte Carlo statistical mechanics was used with the free-energy perturbation theory and the OPLS-AA force field. The results address the transferability of the potential functions developed for pure liquids to mixed systems and the potential importance of explicit polarization for neutral organic molecules in aromatic solvents. Although the free-energy results cover an 11 kcal/mol range, the average error in comparison with experimental data points is only 0.4 kcal/mol. There is no systematic pattern to the discrepancies, so the need to add explicit treatment of solute-solvent polarization effects is not supported. This contrasts the situation with cationic solutes as reflected in cation-π interactions. Results for free energies of hydration are also provided for the 42 solutes in TIP4P water and give an average error of 0.49 kcal/mol. Implications for modeling biomolecular systems with standard force fields are considered. It is also interesting to note the overall similar values for free energies of solvation in benzene and hexafluorobenzene despite the reversal of polarity for the aromatic rings; the most significant exception is the more favorable solvation of perfluoroalkanes in the perfluoro solvent. Alternative accommodations of solutes in the two solvents are illustrated.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":"6574-6583"},"PeriodicalIF":2.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144315582","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}

{"title":"Understanding PET Hydrolysis via Reactive Molecular Dynamics Simulation and Experimental Investigation.","authors":"Shuangxiu Max Ma, Patrícia Pereira, Christian W Pester, Phillip E Savage, Bhavik R Bakshi, Li-Chiang Lin","doi":"10.1021/acs.jpcb.5c03080","DOIUrl":"10.1021/acs.jpcb.5c03080","url":null,"abstract":"<p><p>Polyethylene terephthalate (PET), a widely used polymer in packaging applications, has posed significant environmental challenges due to its resistance to environmental degradation. Chemical recycling via hydrolysis offers a circular solution by breaking PET down into its monomers, terephthalic acid and ethylene glycol, which can then be repolymerized into new PET. Despite its promise, the detailed pathways of PET hydrolysis─particularly the interplay between hydrolysis and thermal degradation─remain a topic of scientific debate. We combine reactive molecular dynamics (MD) simulations with experimental studies to elucidate key reaction pathways, intermediate species, and the temperature-dependent evolution of degradation products. Molecular dynamics simulations offer detailed insights into molecular motions and interactions that are often elusive in experimental setups, thus enhancing our understanding of the complex dynamics at play during PET decomposition. By systematically examining bond dissociation, intermediate species, and product formation at various temperatures, this study elucidates how hydrolysis and thermal degradation pathways evolve and interact. Furthermore, a severity index approach is employed to directly compare TPA yields from simulations with corresponding experimental data.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":"6594-6603"},"PeriodicalIF":2.8,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144473358","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}

{"title":"Thermal Transformations of Radicals Derived from Nuclear Waste Separation Ligands Exposed to Radiation.","authors":"Ilya S Sosulin, Aliaksandra Lisouskaya","doi":"10.1021/acs.jpca.5c01863","DOIUrl":"10.1021/acs.jpca.5c01863","url":null,"abstract":"<p><p>The thermal evolution of electron-beam-induced radicals generated in neat di-<i>n</i>-butyl <i>N</i>,<i>N</i>-diethylcarbamoylphosphonate (DBDECP), <i>N</i>,<i>N</i>-bis(2-ethylhexyl)butanamide (DEHBA), dioctyl phosphate (DOP), tributyl phosphate (TBP), and <i>N</i>,<i>N</i>,<i>N</i>',<i>N</i>'-tetraoctyl diglycolamide (TODGA), and TBP/dodecane extraction system was investigated using electron paramagnetic resonance (EPR) spectroscopy over the temperature range of 108-220 K. Density functional theory (DFT) calculations were employed to support the experimental results, clarifying radical structures and energetics of their thermal transformations. The stability of radicals as temperature increased varied significantly depending on the ligand structure. The diglycol- or amide-centered radicals, such as those found in TODGA and DEHBA, exhibited higher thermal stability than the alkyl radicals. This increased stability is attributed to the greater steric hindrance in the latter species. Calculated energy barriers (∼20 kcal/mol) suggested that thermal evolution predominantly involves conformational rearrangements of the radicals, rather than transformations of the radical structure itself. Additionally, trace amounts of oxygen led to the conversion of carbon-centered radicals into peroxide radicals during thermal annealing. The peroxide radicals formed decomposed more rapidly at elevated temperatures. This study provides important mechanistic insights into the radiolytic degradation of nuclear waste extraction ligands, helping to advance the development of more radiation-resistant solvents for nuclear waste separation processes.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":" ","pages":"5761-5770"},"PeriodicalIF":2.7,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144473430","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}