The Journal of Physical Chemistry C最新文献_第9页

High-Throughput Screening of MN4 Coordinated Macrocyclic Frameworks for CO Reduction by Combining First-Principles Calculations and Machine Learning 结合第一性原理计算和机器学习的MN4协调大环框架的高通量筛选

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-28 DOI: 10.1021/acs.jpcc.6c05023

Ziyue Zhang, Mengmeng Xu, Juan Xie, Yujin Ji, Huilong Dong, Youyong Li

{"title":"High-Throughput Screening of MN4 Coordinated Macrocyclic Frameworks for CO Reduction by Combining First-Principles Calculations and Machine Learning","authors":"Ziyue Zhang, Mengmeng Xu, Juan Xie, Yujin Ji, Huilong Dong, Youyong Li","doi":"10.1021/acs.jpcc.6c05023","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05023","url":null,"abstract":"The electrochemical CO reduction reaction (CORR) by single-atomcatalysts (SACs) provides a promising route for converting CO intovalue-added C1 products, but the rational discovery ofefficient SACs remains challenging because of the large configurationalspace and complex reaction network. Herein, we chose two-dimensionalperiodic macrocyclic frameworks with MN4 coordination centersas the SACs and established a multilevel screening strategy by combiningfirst-principles calculations and machine learning (ML). After evaluatingthermodynamic stability, dissolution resistance, *CO adsorption, andhydrogen evolution reaction suppression, 90 candidates were screenedout from 156 SACs for further analysis. The hydrogenation of *CO to*CHO was identified as a key step for deep CO reduction, and ΔG(*CHO-*CO) was selected as the main descriptor. An ExtraTreesregression model trained on the screened SACs achieved high predictiveaccuracy, with R2 values of 0.947 and 0.925 for the trainingand test sets, respectively. By scanning the full reaction pathwayof CORR (CH4 as the final product) on the SACs with relativelylow ΔG(*CHO-*CO) value, the FeC8N8 was found to exhibit the highest catalytic activityamong the examined candidates, with a low limiting potential (UL) of −0.30 V. To accelerate catalyst evaluation, ΔG(*CHO-*CO), which describes the first hydrogenationof adsorbed *CO, was selected as the key descriptor and predictedby ML algorithm. Full-pathway calculations were subsequently carriedout for catalysts with relatively low ΔG(*CHO-*CO) values to validate the descriptor-guided screening results.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13669–13678"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124995","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

Investigating theRole of Intermediate Carbon Specieson Methane Activation over Molten In–Sn and In–Ni 中间碳在熔融In-Sn和In-Ni上甲烷活化作用的研究

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 DOI: 10.1021/acs.jpcc.6c05394

Nikil Surya Rajaprabu,Abdul Kaish,D. Chester Upham,Vishal Agarwal

{"title":"Investigating the\u0000Role of Intermediate Carbon Species\u0000on Methane Activation over Molten In–Sn and In–Ni","authors":"Nikil Surya Rajaprabu,Abdul Kaish,D. Chester Upham,Vishal Agarwal","doi":"10.1021/acs.jpcc.6c05394","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05394","url":null,"abstract":"Abstract Methane pyrolysis over molten metal catalysts has gained attention as a promising route for CO2-free hydrogen production owing to the intrinsic resistance of liquid catalysts to carbon-induced deactivation. In this work, we investigate the role of intermediate carbon species on the surface composition and methane activation over molten In–Sn and In–Ni alloys using ab initio molecular dynamics (AIMD) simulations and density functional theory (DFT) calculations. Free-energy calculations indicate that methane dissociation proceeds through the formation of carbon monomer and dimer intermediates, which are likely to serve as the initial building blocks for carbon nucleation and subsequent growth of larger poly-aromatic carbon structures. Carbon exhibits distinct segregation behavior in the two molten alloys, preferentially occupying the surface and subsurface regions in In–Sn, while migrating toward the subsurface and bulk in In–Ni. These contrasting distributions are largely independent of the carbon concentration and arise from the preferential interaction of carbon with Sn in In–Sn and Ni in In–Ni. Although carbon segregation modifies the local surface environment, methane activation barriers remain qualitatively unchanged, while the dissociated intermediates are preferentially stabilized on surface carbon species rather than on the molten alloy surface, highlighting the sustained catalytic activity of the molten catalysts.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"297 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149150845","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

Bridging Bulk and Surface Thermodynamics: A Hybrid Pourbaix Framework for Electrocatalyst Stability 桥接体积和表面热力学：电催化剂稳定性的hybriddpourbaix框架

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-23 DOI: 10.1021/acs.jpcc.6c04369

Hyeonjung Jung, Evan Z. Carlson, Md Delowar Hossain, Michal Bajdich

{"title":"Bridging Bulk and Surface Thermodynamics: A Hybrid Pourbaix Framework for Electrocatalyst Stability","authors":"Hyeonjung Jung, Evan Z. Carlson, Md Delowar Hossain, Michal Bajdich","doi":"10.1021/acs.jpcc.6c04369","DOIUrl":"10.1021/acs.jpcc.6c04369","url":null,"abstract":"A long-term durability of electrocatalysts remains acentral challenge,particularly for nonprecious metal catalysts that often exhibit highactivity but suffer from rapid degradation under practical operatingconditions. A major degradation pathway is the dissolution of activemetal sites as ionic or oxidized species at the surface–electrolyteinterface, which remains difficult to capture using conventional computationalapproaches. Here, we introduce the hybrid Pourbaix diagram as a unifiedframework that integrates bulk and surface thermodynamics to assessthe stability of surface metal atoms against dissolution, the redoxbehavior of adsorbates under electrochemical conditions, and the ion(de)intercalation from and into the crystal lattice. By combiningdensity functional theory (DFT) calculations of such surface phenomenawith experimentally reported bulk thermodynamic data, the hybrid Pourbaixdiagram describes pH- and potential-dependent stability across surface-boundand dissolved states. The framework is flexible to incorporate grand-canonical(GC) DFT to account for potential-dependent electronic effects andapplicable to different types of systems and reactions. We demonstratethe versatility of this approach through representative case studiesincluding Ti–N–C for nitrate reduction, Fe–N–Cfor oxygen reduction with potential-induced spin-state transitions,and α-K0.125MnO2 surfaces involving Mndissolution and K+ deinsertion. The hybrid Pourbaix diagramprovides a practical platform for analyzing catalyst stability andactivation, guiding the design of durable and active electrocatalysts.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13746–13755"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049368","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

Key Morphological and Chemical Features of Anodized Nb Relevant for Sn Nucleation in Nb3Sn Growth 与Nb3Sn生长中Sn成核相关的阳极氧化Nb的关键形态和化学特征

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-29 DOI: 10.1021/acs.jpcc.6c04768

Van Do, Jasper T. Brown, Liana Shpani, Cristóbal Méndez, Helena Lew-Kiedrowska, Tomás A. Arias, Matthias U. Liepe, Steven J. Sibener

{"title":"Key Morphological and Chemical Features of Anodized Nb Relevant for Sn Nucleation in Nb3Sn Growth","authors":"Van Do, Jasper T. Brown, Liana Shpani, Cristóbal Méndez, Helena Lew-Kiedrowska, Tomás A. Arias, Matthias U. Liepe, Steven J. Sibener","doi":"10.1021/acs.jpcc.6c04768","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04768","url":null,"abstract":"The performance of superconducting radiofrequency (SRF)cavitiesis governed by material properties within the RF penetration depth.Nb3Sn is a promising next-generation SRF material, capableof Q-factors of 1010 at 4.2 K, yet its performance remainsbelow theoretical predictions due in part to surface inhomogeneitieswithin the ∼100 nm RF penetration depth. Preanodization ofNb enhances Sn nucleation and improves Nb3Sn stoichiometry,but the factors responsible for this improvement remain poorly understood.Using in situ X-ray photoelectron spectroscopy and atomic force microscopy,we investigate the chemical and morphological evolution of anodizedpolycrystalline Nb while annealing to 500 °C, representativeof Nb3Sn growth conditions. The anodized surface is ∼10times rougher than the control and exhibits isotropic bumps and poresthat persist after annealing. Kinetic modeling of the thermal evolutionpredicts that the anodic Nb2O5 surface is morethermally stable than native Nb2O5 during theNb3Sn growth process. Na contamination is also observedon the anodized surface and persists after annealing. ComplementaryDFT calculations predict favorable oxidation reactions and greaterSn stability relative to SnO and SnO2 on Nb2O5 compared with NbO. Together, these results suggestthat the persistent Nb2O5 layer and rough, porousmorphology may promote Sn nucleation and stabilization on anodizedNb, providing insight for optimizing anodization and vapor-diffusiongrowth of Nb3Sn coatings for advanced SRF cavities.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"14050–14059"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124960","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

Co-Assembled Piezoelectric Nanofibers as Self-Powered Sensors for Human Physiological Signals 协同组装压电纳米纤维作为人体生理信号的自供电传感器

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-26 DOI: 10.1021/acs.jpcc.6c03185

Niladri Hazra, Kousik Gayen, Anupam Ghosh, Buddhadev Mukherjee, Soumyajit Hazra, Jayanta Dolai, Supratim Bose, Ayan Datta, Nikhil R. Jana, Arindam Banerjee

{"title":"Co-Assembled Piezoelectric Nanofibers as Self-Powered Sensors for Human Physiological Signals","authors":"Niladri Hazra, Kousik Gayen, Anupam Ghosh, Buddhadev Mukherjee, Soumyajit Hazra, Jayanta Dolai, Supratim Bose, Ayan Datta, Nikhil R. Jana, Arindam Banerjee","doi":"10.1021/acs.jpcc.6c03185","DOIUrl":"10.1021/acs.jpcc.6c03185","url":null,"abstract":"Soft supramolecular materials have emerged as promisingalternativesto conventional inorganic systems for next-generation bioelectronicand self-powered sensing applications due to their intrinsic flexibility,biocompatibility, and mechanical compliance. Herein, we report a coassembledpiezoelectric nanofibrous organogel system constructed from a functionalizedpeptide–appended pyrene (Py–P) donor and a core-substitutednaphthalene diimide (c-NDI) acceptor. While the individual organogelsexhibit relatively lower piezoelectric response, their coassembledstate at an equimolar ratio displays a remarkable enhancement in piezoelectricperformance. The engineered donor–acceptor coassembly producesa highly ordered supramolecular architecture with a piezoelectriccoefficient of 55 pm/V, approaching the upper limit of reported supramolecularorganic piezoelectric materials and convincingly demonstrating theeffectiveness of donor–acceptor engineering for high-performancepiezoelectric energy harvesting. Combined experimental investigationsand theoretical analyses consistently demonstrate the origin of theamplified piezoelectricity in the coassembled system. Leveraging thishigh piezoelectric response, self-powered devices were fabricatedand successfully employed for the detection of human physiologicalsignals, including finger movements and highly sensitive arterialpulse signals. The results demonstrate that this coassembled nanofiber-basedsupramolecular system represents a potent soft piezoelectric materialplatform for self-powered physiological sensing and wearable bioelectronicapplications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13786–13799"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049360","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

Molecular Modeling of the Raman and SERS Response of 6-Mercaptopurine: Tautomerism, Surface Coverage, and Charge Transfer 6-巯基嘌呤拉曼和SERS反应的分子模型：互变异构、表面覆盖和电荷转移

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-27 DOI: 10.1021/acs.jpcc.6c03520

Paola Cimino, Pellegrino Musto, Marianna Pannico, Federico Coppola, Nadia Rega

{"title":"Molecular Modeling of the Raman and SERS Response of 6-Mercaptopurine: Tautomerism, Surface Coverage, and Charge Transfer","authors":"Paola Cimino, Pellegrino Musto, Marianna Pannico, Federico Coppola, Nadia Rega","doi":"10.1021/acs.jpcc.6c03520","DOIUrl":"10.1021/acs.jpcc.6c03520","url":null,"abstract":"Surface-enhancedRaman spectroscopy (SERS) of 6-mercaptopurine(6-MP) was investigated by combining the experimental Raman measurementswith Density Functional Theory calculations to clarify the effectsof tautomerism, aggregation, adsorption geometry, and short-rangecharge transfer. In aqueous solution the thione forms, Thione(N1,N7) and Thione(N1,N9), arethe only thermally accessible species, whereas the thiol forms aresignificantly less stable. X-ray derived dimeric models provide closeragreement with spontaneous Raman spectrum, showing that intermolecularinteractions are essential for describing the solid-state spectrum;for the best Thione(N1,N9) dimer, the mean deviationis 1.1 ± 0.6%. For the adsorbed species, calculations on a tetrahedralAu20 cluster reveal that the thermodynamically preferredflat configurations do not provide the best match to the experimentalSERS spectrum, which is instead more accurately reproduced by sulfur-boundvertex and center motifs. Increasing surface coverage and mixed-tautomeradsorption are further required to recover the experimental relativeintensities, with a 3:1 Thione(N1,N9)/Thione(N1,N7) model giving the best agreement. Distance-dependentanalysis further indicates a short-range chemical-enhancement regimebelow about 4 Å, marked by charge separation, HOMO stabilization,and selective amplification of vibrational modes localized at themolecule–gold adsorption interface. This work introduces amultitautomer modeling strategy that explicitly goes beyond the conventionalsingle-molecule 1:1 adsorption paradigm, demonstrating that only theconcurrent treatment of surface coverage, tautomeric coexistence,and short-range charge transfer yields a physically consistent andquantitatively accurate description of the SERS response.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13824–13841"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049340","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

Coordinated Water Molecules Regulate Exciton Localization and Bright Luminescence in Sb3+-Doped Indium Bromide Hybrid 配位水分子调节Sb3+掺杂的溴化铟杂化物的激子定位和明亮发光

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-25 DOI: 10.1021/acs.jpcc.6c05722

Ashwath Kudlu, Palak Chugh, Thomas Jose Maliakal, Arup Mahata, Janardan Kundu

{"title":"Coordinated Water Molecules Regulate Exciton Localization and Bright Luminescence in Sb3+-Doped Indium Bromide Hybrid","authors":"Ashwath Kudlu, Palak Chugh, Thomas Jose Maliakal, Arup Mahata, Janardan Kundu","doi":"10.1021/acs.jpcc.6c05722","DOIUrl":"10.1021/acs.jpcc.6c05722","url":null,"abstract":"Inner-sphere coordination in metal halide hybrids (MHHs)representsa powerful yet largely unexplored handle for regulating excitonicemission. Here, we demonstrate that inner-sphere coordinated watermolecules govern the photophysics of Sb3+-doped indiumbromide hybrid (Sb:DAMPInBr), synthesized using 1-(2-dimethylaminoethyl)-4-methylpiperazine(DAMP). The zero-dimensional hybrid comprises two inequivalent halometallateunits, (In/Sb)Br6 and water-coordinated (In/Sb)Br4(H2O)2, enabling direct interrogation of coordination-inducedstructural and electronic effects on excitonic emission. The hydratedphase exhibits intense yellow emission (∼570 nm, PLQY 47%),whereas dehydration produces a red-shifted, weak orange emission (∼600nm, PLQY ∼4%). Density functional theory reveals that coordinatedwater actively participates in the excited-state electronic structure,enhancing exciton localization, thereby stabilizing self-trapped excitons(STE) within the [(Sb/In)Br4(H2O)2] unit and promoting radiative recombination. In contrast, dehydrationweakens exciton localization, leading to increased nonradiative decay.The reversible restoration of emission upon rehydration establishesa hydration-driven luminescence switching mechanism and identifiescoordinated water as an active structural motif rather than a passivesource of lattice distortion. More broadly, this work extends thecurrent understanding of luminescence in MHHs by demonstrating thatstructural distortion-induced STE formation alone does not fully accountfor the observed emission efficiency. Instead, our findings establishexciton localization, directly regulated by inner-sphere coordinatedwater molecules, as a key factor governing radiative recombinationand luminescence efficiency in hydrated MHHs, providing a new designprinciple for engineering stimuli-responsive luminescent materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13871–13881"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049362","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

From Waste Polyethylene to Photophysical Probes: Mechanistic Investigation of Hg2+-Induced Fluorescence Quenching in Carbon Dots 从废聚乙烯到光物理探针：Hg2+诱导碳点荧光猝灭的机理研究

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-23 DOI: 10.1021/acs.jpcc.6c03760

Sasikumar Priya, Easwaramoorthi Karthikeyan, Sudhin Rathnakumaran, Sreedharan Sreena, Chalappurath Pattelath Reshmi, Analiparambil Ravindran Ramesh

{"title":"From Waste Polyethylene to Photophysical Probes: Mechanistic Investigation of Hg2+-Induced Fluorescence Quenching in Carbon Dots","authors":"Sasikumar Priya, Easwaramoorthi Karthikeyan, Sudhin Rathnakumaran, Sreedharan Sreena, Chalappurath Pattelath Reshmi, Analiparambil Ravindran Ramesh","doi":"10.1021/acs.jpcc.6c03760","DOIUrl":"10.1021/acs.jpcc.6c03760","url":null,"abstract":"Understanding the photophysical origin of metal-ion-inducedfluorescencequenching in carbon dots remains challenging because of their structuralheterogeneity and complex surface chemistry. Herein, waste polyethylene-derivedcarbon dots (PECDs) were synthesized and employed as a model systemto investigate Hg2+-induced fluorescence quenching throughcombined experimental and computational analyses. The fluorescentcarbon dots were synthesized via a hydrothermal method and characterizedby HR-TEM, XRD, FTIR, Raman, and XPS. This valorized material candetect mercury ions in the nanomolar range, by fluorescence quenching,with a limit of detection (LOD) of 31.1 nM (6.24 ppb). The fluorescencequenching is substantiated as a static quenching mechanism by fluorescencelifetime studies and ζ-potential analysis. Density functionaltheory (DFT) calculations were performed to model the PECD structureand evaluate the binding of Hg2+ and selected metal ionsto different surface functional groups. Time-dependent DFT (TDDFT)analysis of the absorption and emission properties reproduces theexperimental fluorescence trends and provides insights into the observedquenching behavior of the PECD–metal ion complexes.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13959–13969"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049372","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 Origin of Intermolecular Photoexcited-State Dynamics in Flavonoids 黄酮类化合物分子间光激发态动力学的结构起源

IF 3.4 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 Epub Date: 2026-09-28 DOI: 10.1021/acs.jpcc.6c05022

Jiali Liu, Zhuoyi Cai, Yanjiao Fu, Wenjin Huang, Yingchen Peng, Ziyi Fan, Fengyong Yang, Xiaolin Zhu, Lei Shan, Weiwei Tang, Jiajing Guo, Yaxin Zhai

{"title":"Structural Origin of Intermolecular Photoexcited-State Dynamics in Flavonoids","authors":"Jiali Liu, Zhuoyi Cai, Yanjiao Fu, Wenjin Huang, Yingchen Peng, Ziyi Fan, Fengyong Yang, Xiaolin Zhu, Lei Shan, Weiwei Tang, Jiajing Guo, Yaxin Zhai","doi":"10.1021/acs.jpcc.6c05022","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05022","url":null,"abstract":"Flavonoidsare a widespread class of natural polyphenols with diversephotophysical and photochemical properties. Understanding how molecularstructure governs their photoexcited-state dynamics is essential forelucidating photoinduced energy dissipation. Here, we employ femtosecondtransient absorption (TA) spectroscopy to investigate the concentration-dependentphotoexcited-state dynamics of flavonoids spanning flavanone glycosides(FGs), flavanones, flavones, and polymethoxyflavones (PMFs). Althoughthe steady-state UV–vis absorption spectra changed little withconcentration, TA measurements revealed pronounced differences inthe concentration-dependent photoexcited-state dynamics among theflavonoid families. With increasing concentration, FGs progressivelydeveloped a new long-lived photoinduced absorption (PIA) band centeredat approximately 433 nm. Concurrently, the contribution of the long-livedphotoexcited population increased from approximately 17% to 86%, whereasthe fast and long-lived decay lifetimes remained nearly unchangedat approximately 0.3 and 60 ps, respectively. In contrast, PMFs displayeda characteristic delayed buildup followed by decay that remained essentiallyunchanged over the investigated concentration range. Systematic comparisonreveals that the degree of π-conjugation associated with theC2–C3 linkage, rather than glycosylation, governs the concentration-dependentphotoexcited-state dynamics. These findings establish a clear structure-dynamicsrelationship in flavonoids and provide a molecular framework for understandingand engineering their intermolecular photoexcited-state behavior.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 40","pages":"13863–13870"},"PeriodicalIF":3.4,"publicationDate":"2026-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149124909","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

Electric-Field-InducedSecond-Harmonic Generationat Charged Interfaces: From Inception to the Eisenthal χ(3) Method and toward Interfacial Electrostatics: A Mini Review 电场感应二次谐波产生的带电界面：从初始到艾森塔尔χ(3)方法和界面静电：一个小回顾

IF 4.126 3区化学

The Journal of Physical Chemistry C Pub Date : 2026-10-08 DOI: 10.1021/acs.jpcc.6c05063

Raiden Speelman,Franz M. Geiger

引用次数: 0