The Journal of Physical Chemistry C最新文献

{"title":"Interfacial Charge\u0000Transfer and Optoelectronic Properties\u0000of the SnS2/HfS2 van der Waals Heterostructure:\u0000Insights from Ground-State Properties and Nonadiabatic Excited-State\u0000Dynamics","authors":"Xin Ran,Yue Tang,Xinlu Cheng,Hong Zhang","doi":"10.1021/acs.jpcc.6c04624","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04624","url":null,"abstract":"Abstract Based on density functional theory (DFT) and nonadiabatic molecular dynamics (NAMD) methods, the interface charge transfer dynamics and strain-controlled optoelectronic properties of SnS2/HfS2 van der Waals heterojunctions were systematically investigated. The results indicate that SnS2 and HfS2 can form a stable van der Waals stacking structure and form a type-I band alignment, where photogenerated electrons and holes are localized within the HfS2 layer. Optical property analysis shows that the absorption coefficient of the heterojunction is significantly improved in the ultraviolet band, and it also exhibits a remarkably enhanced light absorption capacity in the visible region. NAMD simulations further reveal that the system possesses a long electron–hole recombination lifetime of approximately 283.98 ns and an ultrafast interfacial hole transfer process of around 633.82 fs. Under weak electron–phonon coupling dominated by low-frequency vibrations, the nonadiabatic coupling strength of the system is markedly reduced, which effectively suppresses carrier recombination loss. This synergistic combination of ultrafast interfacial hole transfer and long-lived carrier retention is of great significance for boosting the performance of photodetectors. In addition, biaxial strain can significantly modulate the band gap, band alignment, and optical absorption characteristics of the system. Compressive strain can further induce band structure evolution and a redshift of the absorption spectrum, offering a feasible strategy for the tunable optimization of its optoelectronic properties.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"10 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209267","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}

{"title":"Ag-CuO\u0000 x\u0000 -MnO\u0000 x\u0000 -CeO2 Interfacial Interactions\u0000in Low-Temperature Oxidation Catalysts: Effect of Cu Loading","authors":"Natalia V. Dorofeeva,Anna S. Savel’eva,Aleksandra V. Selivanova,Tatiana A. Bugrova,Mikhail A. Salaev","doi":"10.1021/acs.jpcc.6c04982","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04982","url":null,"abstract":"Abstract In environmental multielement catalysts, the catalytic function usually emerges when the elements in desired oxidation states are involved in interfacial interactions on the catalyst surface. The approaches to tune the distribution and interplay of states of elements are in demand. Here, two series of bimetallic Ag/X%CuCeOx and Ag/X%CuCeMnOx catalysts with varied Cu loading (X = 3–4%wt.) are prepared combining solvothermal approach with incipient wetness impregnation and tested in low-temperature CO oxidation and soot combustion. In both series, the bimetallic samples exhibit higher activity compared to the Ag-free reference systems. The bimetallic particles are formed, and the synergistic action of the metal species in cooperation with the active oxidative sites of the mixed oxide support is observed. The copresence of Mn and Cu species enhances the reoxidation properties of catalysts due to the distribution of oxides within the intergranular space of CeO2. Larger CuOx species formed at higher Cu loading do not improve the catalytic performance. The results obtained have implications for the rational development of next-generation oxidation catalysts for energy and environmental applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"14 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209266","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}

{"title":"Strain- and Electric\u0000Field-Induced Band Alignment\u0000Transitions in a GaSe/ZrSe2 van der Waals Heterostructure","authors":"Weiyin Li,Shixun Li,Vei Wang","doi":"10.1021/acs.jpcc.6c03985","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c03985","url":null,"abstract":"Abstract Two-dimensional (2D) van der Waals heterostructures (vdWHs) have emerged as a highly versatile platform for designing next-generation optoelectronic devices. In this study, we perform systematic first-principles calculations to investigate the structural, electronic, and optical properties of the GaSe/ZrSe2 vdWH, as well as its responses under biaxial strain and perpendicular external electric fields. Our results predict that the equilibrium vdWH exhibits an indirect bandgap of 1.18 eV with a prominent Type-I band alignment, which effectively confines both photoexcited electrons and holes within the ZrSe2 layer. Furthermore, we demonstrate that a transition from Type-I to Type-II band alignment can be dynamically induced either by applying a tensile strain of +2% or higher, or a positive external electric field exceeding +0.2 V/Å, thereby facilitating the spatial separation of photogenerated carriers. Concurrently, the optical spectral profiles can be strategically manipulated because biaxial strain prominently boosts visible-light absorption while modulating the omnidirectional reflectance and transmittance, whereas external electric fields enable precise regulation over the infrared and ultraviolet responses. These fundamental insights into the underlying microscopic mechanisms position the GaSe/ZrSe2 vdWH as a promising dynamically controllable building block for multifunctional nanodevices such as strain gauges, ultraviolet photodetectors, transparent optoelectronics, and highly efficient photocatalytic systems.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"3 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209265","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}

{"title":"Modeling Reactions on the Solid–Liquid Interface with Next Generation Extended Lagrangian Quantum-Based Molecular Dynamics","authors":"Rae A. Corrigan Grove,&nbsp;Kevin G. Kleiner,&nbsp;Joshua Finkelstein,&nbsp;Ivana Matanovic,&nbsp;Michael E. Wall,&nbsp;Travis E. Jones,&nbsp;Anders M. N. Niklasson,&nbsp;Christian F. A. Negre","doi":"10.1021/acs.jpcc.6c06025","DOIUrl":"10.1021/acs.jpcc.6c06025","url":null,"abstract":"<p>We present a series of simulations of the oxygen reductionreaction(ORR) using a novel framework for atomistic simulations of surfacecatalysis under electrochemical bias. The framework makes use of quantum-mechanicalextended Lagrangian Born–Oppenheimer molecular dynamics (XL-BOMD)simulations, which provide the speed and accuracy required for explicitatomistic treatment of both electrode and electrolyte. Simulationsof solvated O₂ near nitrogen-doped graphene (NG) were performedto gain insight into the ORR, and different mechanisms were observed,depending on the applied bias. Under higher bias the ORR occurredby an outer-sphere mechanism, without adsorption of O₂ toNG. In this mechanism, electron transfer between the catalyst andthe O₂ was mediated by the solvent. Under lower bias theORR occurred by an inner-sphere mechanism involving adsorption ofO₂ to NG, leading to direct electron transfer. Our extensive,all-atom quantum-mechanical molecular dynamics simulations also showclear differences between the kinetics of the ORR on this ideallypolarizable electrode and commonly used kinetic theories, leadingto new insights regarding mechanistic changes with varied overpotentials.Combining quantum accuracy with explicit solvation and electrostaticpotential bias, XL-BOMD opens a route to predictive, atomistic insightinto electrocatalytic processes, as demonstrated with the ORR.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14193–14208"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090624","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}

{"title":"Scaling of Island Densities in Multilayer Growth and an Application to α-Sexithiophene Films","authors":"Edwin E. Mozo Luis,&nbsp;Ismael S. S. Carrasco,&nbsp;Fábio D. A. Aarão Reis","doi":"10.1021/acs.jpcc.6c04795","DOIUrl":"10.1021/acs.jpcc.6c04795","url":null,"abstract":"<p>Kinetic Monte Carlo simulations of thin-film depositionare performedwith film–substrate interactions slightly stronger than film–filminteractions and with layer-dependent Ehrlich–Schwoebel (ES)barriers for molecules to cross step edges. Simulations with rapidchanges from weak to strong ES barriers in the first few layers representthe crossover from layer-by-layer (LBL) growth to rapid rougheningobserved in ultrathin films of aligned organic molecules such as α-sexithiophene(6T) and diindenoperylene (DIP) deposited on SiO_<em>x</em>; moreover, the shapes of wide islands formed in the firstand second layers resemble those of the 6T films. However, weak ESbarriers recently predicted by a mean-field approach for that materialare ruled out by the simulations. When densities of 10^–3 islands per lattice site or less are obtained, these densities followrelations with the model parameters as predicted by submonolayer growththeories, despite the strong interlayer fluxes which those theoriesdo not account for. This feature allows extrapolations to the muchsmaller island densities of 6T films, in which the relations 2<em>E</em>_<em>S</em> + <em>E</em>_<em>B</em> = 2.1 ± 0.4 eV and 2<em>E</em>_<em>F</em> + <em>E</em>_<em>B</em> = 1.8 ± 0.3 eV are estimated for the activation energiesof molecule hopping on the substrate (<em>E</em>_<em>S</em>), on upper film layers (<em>E</em>_<em>F</em>), and of molecule bonding with lateral neighbors(<em>E</em>_<em>B</em>). From the same extrapolations,we obtain characteristic frequencies of hopping to neighboring sitesν ∼ 10²¹–10²⁸ s^–1 in the first layer and ∼10²¹–10²⁶ s^–1 in the second layer. These results suggestthat individual energy parameters are on the order of a few tenthsof eV. We propose to interpret these values by relating activationenergies and contact areas between neighboring molecules with a rod-likeshape: first, large <em>E</em>_<em>B</em> is a consequence of large contact areas of neighboring standing-upmolecules on islands; second, standing-up molecules on terraces havelarge diffusion lengths between two orientational changes, so <em>E</em>_<em>S</em> and <em>E</em>_<em>F</em> account for breaking bonds of the laying-downorientation during these changes, while the anomalously large νincorporates those diffusion lengths. These possible interpretationsmay motivate additional experimental and theoretical studies of thinfilms of rod-like molecules.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14339–14350"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090999","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}

{"title":"Anion-Activated Supramolecular Proton Relays Enable Neutral-pH and Seawater Oxidation","authors":"Faezeh Sarafraz,&nbsp;Afshin Pashabadi,&nbsp;Avat Arman Taherpour,&nbsp;Mojtaba Shamsipur","doi":"10.1021/acs.jpcc.6c03999","DOIUrl":"10.1021/acs.jpcc.6c03999","url":null,"abstract":"<p>Neutral-pH and direct seawater oxidation are criticallyhinderedby sluggish proton-coupled electron transfer (PCET) and competitivechloride corrosion. Here, we employ surface-confined azacrown macrocyclesof varying nitrogen content as supramolecular proton-management layersrather than conventional redox catalysts. In neutral phosphate buffer,OER activity follows an unconventional one aza &gt; two aza ≫six aza macrocycle trend, with Cu/Hexaaza exhibiting purely capacitivebehavior that switches to superior catalysis at 4 °C. CombinedGerischer impedance and DFT analyses reveal an anion-assisted PCETmechanism wherein phosphate binding narrows the HOMO–LUMO gap,transforming electronically inert hosts into a highly polarizableproton–anion assembly. The computational studies show thatthe interfacial activity is governed not by maximal proton affinity,but by an optimal enthalpy–entropy balance between proton storageand Grotthuss-type hopping. While hexaaza (HAZ) overstabilizes protonsat ambient temperature, monoaza (MAZ) enables rapid, exchange-dominatedproton shuttling. Substituting Cu foam with a graphite sheet deliversa metal-free OER in intact seawater without pH adjustment or desalination.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14085–14096"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092251","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}

{"title":"Anisotropic Lattice Dynamics and Carrier–Phonon Coupling in Sb2Se3 Crystals","authors":"Huijie Liu,&nbsp;Kelvin H. L. Zhang,&nbsp;Ye Yang","doi":"10.1021/acs.jpcc.6c06320","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06320","url":null,"abstract":"<p>Antimony chalcogenides (Sb₂X₃)have emergedas promising, high-efficiency, and cost-effective photovoltaic materials.We employ femtosecond transient reflectivity (TR) spectroscopy togenerate and resolve coherent acoustic phonons (CAPs) propagatingalong the three principal crystallographic directions of the Sb₂Se₃ single crystals. Sound velocities extractedfrom Brillouin oscillation frequencies agree well with the computationalresults. We quantify the electron–hole deformation potential,which suggests that strongly bound polarons are unlikely in this material.Our measurements demonstrate that highly anisotropic interatomic bondingdictates its elastic response and phonon transport behavior, deliveringcritical experimental benchmarks to guide the relevant device designs.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14260–14265"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149188094","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}

{"title":"The Impact of Electronic\u0000Structure Modification on\u0000Lewis Acidity-Basicity and Reducibility of Doped La2O3","authors":"Shikun Li,Marcus Bäumer,Zhi-Jian Zhao,Lyudmila V. Moskaleva","doi":"10.1021/acs.jpcc.6c03339","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c03339","url":null,"abstract":"Abstract Catalyst reactivity hinges on descriptors such as surface reducibility and Lewis acidity/basicity. This study systematically explores how doping the La2O3(001) surface with s-block, d-block and f-block heteroatoms modulates these properties. Dopant-induced changes in surface reducibility are quantified using oxygen vacancy formation energies, while cation-site Lewis acidity is probed by NH3 adsorption energies, and the strength of local acid–base interactions at oxygen-containing sites is compared using CO2 adsorption energies. Spin-averaged band centers of the unoccupied La 5d states and occupied O 2p states were calculated for doped La2O3(001) surfaces and correlated with these reactivity descriptors. The results reveal several clear trends: (i) Dopants with stable oxidation states lower than that of La exhibit low oxygen vacancy formation energies, strong electron-accepting abilities, and elevated d- and p-band centers caused by the formation of electron-deficient sites, whereas high-valent dopants exhibit the opposite behavior. (ii) A clear linear relationship is observed between the La 5d- or O 2p-band centers on defective doped La2O3(001) surfaces and the oxygen vacancy formation energy. (iii) In contrast, correlations between the La 5d- or O 2p-band centers and molecular adsorption-based Lewis acid–base descriptors are weaker. We find that the unoccupied dopant dz2 -band center exhibits an improved correlation with NH3 adsorption energy compared with the full dopant d-band center, providing an orbital-specific descriptor for understanding Lewis acidity trends.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"42 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209285","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}

{"title":"Synergistic Dual-Site Coordination of a Multifunctional Phosphonate Additive for Efficient Perovskite Solar Cells","authors":"Jiafu Li,&nbsp;Xu Wang,&nbsp;Jinbiao Jia,&nbsp;Yongzheng Zhang,&nbsp;Jia Dong","doi":"10.1021/acs.jpcc.6c05683","DOIUrl":"10.1021/acs.jpcc.6c05683","url":null,"abstract":"<p>The accelerated evolutionary trajectory of perovskitesolar cellshas propelled them to the forefront as a preeminent candidate foraffordable and efficient renewable energy technologies. However, crystaldefects and bulk imperfections within the perovskite films criticallyundermine their photovoltaic performance, thereby hindering the commercialization.In this work, a multifunctional additive, diethyl (4-cyanobenzyl)phosphonate(D4CP), is incorporated into the perovskite precursor solution. Theoreticalevidence reveals that D4CP forms robust coordination with Pb²⁺ ions via dual electron-donating pathways (P═O and C≡Nbonds). Moreover, experimental outcomes reveal that the strategicincorporation of D4CP improves the crystallization quality and systematicallypassivates defects within the perovskite films, thereby mitigatingdefect-assisted recombination. Ultimately, the champion device incorporatingD4CP achieves a peak PCE of 24.40%, outperforming the reference device(22.30%). The work positions D4CP as a transformative additive forperovskite solar cells that synergistically elevates PCE.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14130–14138"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092252","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}

{"title":"Spin State Switching in the [FeII(HL-F)2](AsF6)2 Compound","authors":"S. I. Klokishner,&nbsp;O. S. Reu","doi":"10.1021/acs.jpcc.6c04004","DOIUrl":"10.1021/acs.jpcc.6c04004","url":null,"abstract":"<p>The course of spin transformation induced by the protontransferin the iron(II) hydrazone crystalline compound [Fe(HL-F)₂](AsF₆)₂ has been explained through single-pointDFT calculations applying the observed structural data on the titledcompound in the temperature range 25–220 K. It has been revealedthat the four crystallographically identical complexes present inthe crystal structure at temperatures 25 K and 123 K containiron(II) ions only in the low-spin ¹A₁-state.From eight iron(II) complexes present in the crystal unit at 153 K,only a half of complexes passed to the high-spin state. From the performedcalculations, it also follows that at 220 K all iron(II) ions in thefour types of complexes experimentally detected in the crystal structurehave reached the high-spin state. The undertaken study has also revealedthe difference in the magnitudes and type of alignment of the dipolemoments of the complexes present in the crystal structure at temperatures25, 123, 153, and 220 K. On the basis of the obtained results, a qualitativeinterpretation of the observed magnetic susceptibility data of the[Fe(HL-F)₂](AsF₆)₂ compound has beengiven.</p>","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"130 41","pages":"14312–14320"},"PeriodicalIF":3.4,"publicationDate":"2026-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090585","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}