The Journal of Physical Chemistry C最新文献

{"title":"A-Site-Dependent Hydrogen Affinity in Ti3AlC2 Single Crystal and Ti3ZnC2-Oriented Platelet","authors":"Qingyu Zhang,Yanmei Chen,Yinghui Li,Yukun Xiao,Mian Li,Jianxin Zou,Ke Chen,Qing Huang","doi":"10.1021/acs.jpcc.6c06938","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06938","url":null,"abstract":"MAX phases provide compositionally tunable layered structures for investigating hydrogen interactions, but the role of A-site chemistry remains insufficiently understood. Here, Ti3ZnC2-oriented platelets were prepared from Ti3AlC2 single-crystal precursors through Al-to-Zn substitution in a Lewis-acidic molten salt. Under the tested conditions, the temperature required for near-complete Al removal increased with the lateral size of the precursor platelets. Surface and cross-sectional EDS analyses were consistent with near-complete Al-to-Zn substitution in the examined regions. Density functional theory calculations of selected ideal-bulk configurations identified Ti–A layer interstitial sites as energetically favorable for H insertion in both phases. Replacing Al with Zn lowered the most favorable single-H formation energy from −0.22 to −0.61 eV and stabilized selected multi-H configurations. At 77 K and 72.2 bar, Ti3ZnC2 showed an H2 uptake of 0.303 wt %, compared with 0.145 wt % for Ti3AlC2. The Ti3ZnC2-oriented platelets reached 0.505 wt % at 100 bar, despite having slightly lower N2-accessible BET surface area and pore volume than the Ti3AlC2 precursors. These results reveal an A-site-dependent difference in ideal-bulk H-insertion energetics and total low-temperature H2 uptake. These findings identify A-site chemistry as an effective compositional variable for tuning hydrogen interactions in Ti-based MAX phases.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"9 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368353","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":"Systematic Investigation of Superconducting Trends in Lanthanide-Substituted MC2H8 Ternary Hydrides","authors":"Izabela A. Wrona","doi":"10.1021/acs.jpcc.6c05103","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05103","url":null,"abstract":"The pursuit of high-temperature superconductors represents a persistent challenge in solid-state physics. Hydrogen-rich ternary materials subjected to high pressure have emerged as particularly promising candidates. Among these, the Fm3̅m-MC2H8 family exhibits remarkable stability and compositional diversity. While LaC2H8 has been investigated, other lanthanide substituted variants remain largely unexplored. This work systematically investigates the superconducting properties of lanthanide-based MC2H8 compounds over a wide range of pressures. Calculations predicted 14 unknown superconductors within this family, with critical temperatures strongly dependent on the choice of metal M. Notably, LuC2H8 achieves the highest Tc of 99.5 K (at 200 GPa), while YbC2H8 stabilizes at the lowest pressure (30 GPa). The pressure- and temperature-dependent trends governing superconductivity in these systems have been further elucidated, providing insight into the role of lanthanide substitution in enhancing superconducting properties. These findings expand the landscape of high-temperature superconductors and highlight the potential of hydrogen-rich ternary hydrides under extreme conditions.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"10 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368361","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":"Prolonged Exciton Survival with Enhanced Spatial Contraction in Layered WSSe Alloys","authors":"Le Zheng,Zhengyi Lu,Wei Dai,Yan Zeng,Huiting Zhang,Yan Li,Cidu Lin,Shibin Deng,Zhenhua Yu,Quanbing Guo,Ti Wang","doi":"10.1021/acs.jpcc.6c06705","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06705","url":null,"abstract":"The spatial extent of an optically detected excitation population is determined by both particle motion and spatially selective survival, so a more persistent signal need not imply greater spreading. Here, we combine broadband transient transmission spectroscopy, fluence-dependent kinetics, and transient absorption microscopy to follow the A-exciton bleach in monolayer, bilayer, and trilayer nominal WS0.9Se1.1 alloys. Increasing layer thickness produces a pronounced temporal–spatial contrast. The bleach becomes more persistent, whereas its spatial profile undergoes stronger transient contraction. Fluence-dependent kinetics further reveal that enhanced survival after the initial decay can coexist with faster depletion at later times. Joint analysis using a trapping–diffusion model with shared reaction parameters supports a picture in which traps fill more rapidly near the excitation center, suppressing further capture there, while continued capture at the periphery narrows the bleach-active population. Diffusion and density-dependent loss oppose this narrowing and contribute to the subsequent width recovery. These results show that temporal persistence and spatial spreading need not evolve together when relaxation is spatially selective.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"17 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149368357","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":"T-pentagraphene: A New Carbon Network with Enriched Properties","authors":"Nirmal Barman,Utpal Sarkar","doi":"10.1021/acs.jpcc.6c04681","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04681","url":null,"abstract":"The discovery of novel two-dimensional (2D) semiconducting carbon networks is crucial for advancing next-generation all-carbon electronics. We are proposing a novel two-dimensional semiconducting carbon allotrope, termed as T-pentagraphene, which may be consider as a blend of pentagraphene and T-graphene. This structure is energetically more favorable than other graphyne family members, including experimentally synthesized graphyne and graphdiyne monolayers. Density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations confirm that this new carbon allotrope is dynamically, thermally, and mechanically stable; capable of withstanding temperatures up to 2000 K. T-pentagraphene exhibits an intrinsic semiconducting nature, band gap as large as 3.07 eV, close to TTH-carbon (3.23 eV), penta-graphene (3.25 eV), tetrahexcarbon (3.70 eV), TO-C10 (3.97 eV). Additionally, it demonstrates an ultrahigh hole carrier mobility of 1.619 × 105 cm2·V–1·s–1 (HSE06) and outstanding optical properties, covering entire the UV region. Due its ultrahigh hole carrier mobility alongside superior optical performance, makes T-pentagraphene a promising candidate for next-generation electronics and optoelectronic devices. We also investigate the mechanical properties of T-pentagraphene, including its Young’s modulus, in-plane stiffness, Poisson’s ratio, bulk modulus, and shear stiffness under applied mechanical strain. Owing to its exceptional multifunctional properties including electronic, optical and mechanical, T-pentagraphene suggest its strong potential for influencing various scientific and nanotechnology applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"23 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360351","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":"Temperature Driven Evolution of Alumina Nanowhiskers in Aluminum Intercalated Layered Graphene Oxide","authors":"Shankee Verma,Sonali Patajoshi,Atanu Samanta,Suman Chowdhury,Rahul Singhal,Aloke Kanjilal","doi":"10.1021/acs.jpcc.6c04946","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c04946","url":null,"abstract":"Layered graphene oxide (GO) has attracted considerable attention for a wide range of applications, from optoelectronic devices to solar cells, where performance can be significantly enhanced through elemental intercalation. In this work, we demonstrate the temperature-dependent hydrothermal growth of Al-intercalated GO (Al@GO), achieved through the chemical reaction of GO and aluminum acetylacetonate, resulting the formation of Al–O–C bonds, as confirmed by X-ray photoelectron spectroscopy. X-ray diffraction measurements reveal the transformation of GO to reduced GO (rGO) at 180 °C, while scanning electron microscopy indicates the formation of layered GO with tortuous porous morphology. High-resolution transmission electron microscopy, along with energy-dispersive X-ray spectroscopy, further confirms the discrete evolution of alumina nanowhiskers, predominantly in the γ-phase, as evidenced by selected area electron diffraction. Density functional theory calculations support the formation of Al–O–C bonds in Al@GO, while Al intercalation induces an indirect-to-direct bandgap transition in GO.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"12 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360501","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":"Interplay of Janus Polarization and Interfacial Electric Fields Governing Carrier Dynamics in MoS2/MoSSe Heterostructures","authors":"Hao Dong,Yuna Li,Chenxu Zhang,Rui Yang,Huan Yang,Yujun Zheng","doi":"10.1021/acs.jpcc.6c05449","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05449","url":null,"abstract":"It is crucial to understand the role of polarization and the built-in electric field in heterostructures of two-dimensional materials, as these factors significantly affect carrier dynamics, interfacial properties, and device performance. Here, we combine first-principles calculations with nonadiabatic molecular dynamics simulations to investigate the electronic structure and excited-state carrier dynamics of MoS2/MoSSe heterostructures. We show that the interplay between the intrinsic polarization of Janus MoSSe and the interface-induced electric field strongly modulates interlayer charge transfer. This dual-field coupling drives a transition between type-I and type-II band alignments and switches the dominant carrier relaxation pathways from intralayer recombination to interlayer charge separation. Carrier relaxation is further governed by the interplay between nonadiabatic coupling and phonon-assisted transitions. These results identify polarity reversal as an effective strategy for tuning charge-transfer pathways and excited-state dynamics in van der Waals heterostructures, and provide guidance for designing two-dimensional optoelectronic and photocatalytic materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"37 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360356","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":"Electron-Induced Formation of C2 on Si(100) from Acetylene and Ethylene","authors":"Oliver MacLean,Marc Savoie,Damian G. Allis,Rafik Addou,Ryan Groome,Si Yue Guo,Aru Joy Hill,Alex Inayeh,Hadiya Ma,Cameron J. Mackie,Sheena Ou,Marco Taucer,Denis A. B. Therien,Finley Van Barr,Ryan Yamachika","doi":"10.1021/acs.jpcc.6c06086","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c06086","url":null,"abstract":"Hydrogen Desorption Lithography on Si(100) demonstrates the ability of the Scanning Tunneling Microscope (STM) to create functional atomic-scale structures and devices. The dehydrogenation of adsorbed molecules represents a potential complementary technique that has received little attention. For example, formation of C2 could introduce local strain or act as a center for subsequent reactions and would inform positionally controlled mechanosynthesis, an approach with vast potential in surface patterning and functionalization. Here, we studied the electron-induced dehydrogenation of acetylene and ethylene on Si(100) at 4 K using STM. Excitation of acetylene at ≥+3.2 V induces configurational switching, including to a new sublayer-bonded geometry previously predicted to be an adsorption precursor, as well as migration and desorption. Excitation also induces dehydrogenation to C2. Switching between three observed C2 configurations can be induced by excitation at ≥+4.2 V. Simulations using density functional theory reproduced the experimental images based on the choice of functional, dimer-buckling averaging, and the inclusion of diffuse basis functions. In addition, dehydrogenation could be induced using field-emitted electrons on a scale ranging from a single molecule to a radius of >10 nm. These observations highlight the potential of carbon dehydrogenation as an additional tool in Atomically Precise Fabrication (APF).","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"10 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360348","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":"Direct Observation of Crystal Structures and Raman Spectra during Photochemical Changes of Organic Charge-Transfer Complexes: Thermodynamic Aspect of Heavy Atom Effects","authors":"Hiromu Nagao,Harune Nishida,Minaho Nakaie,Hiromichi Toyota,Toshio Naito","doi":"10.1021/acs.jpcc.6c03626","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c03626","url":null,"abstract":"For insight into photochemical processes, it is required to observe structures and spectra with the corresponding thermodynamic functions and electronic states. We have compared the photochemical processes between MV[NiL2]2 (L = 1,3-dithole-2-selone-4,5-dithiolate, the selone derivative, or L = 1,3-dithiole-2-thione-4,5-dithiolate, the thione derivative), which exhibited sufficiently slow photochemical changes to observe them by various methods, to study heavy-atom effects on photoluminescence. X-ray single-crystal structural analyses, first-principles calculations, and Raman spectra indicated that, in both derivatives after cessation of photoirradiation, their molecular orbitals, charge distributions, and thermodynamic quantities remained changing for weeks to months. Triggered by a 532 nm laser, the selone derivative more efficiently emitted infrared light than did the thione derivative. Comparison between the two derivatives revealed structural and thermodynamic aspects of heavy-atom effects. The findings bridge macroscopic and microscopic viewpoints of photoinduced phenomena in materials, providing experimental grounds for theories.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"15 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360350","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":"Tuning Magnetic Stability in Lanthanide Single-Atom Magnets on Defective Boron Nitride: From Intrinsic Protection to Field-Induced Spin-Lifetime Engineering","authors":"Yaqing Chen,Jie Liu,Ruizhi Qiu,Hongkuan Yuan","doi":"10.1021/acs.jpcc.6c05515","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05515","url":null,"abstract":"The pursuit of atomic-scale magnetic storage has driven intense research into lanthanide-based single-atom magnets (SAMs), where magnetic bistability and long magnetic relaxation times are essential for practical applications. However, a fundamental challenge is to achieve strong uniaxial magnetic anisotropy while simultaneously suppressing quantum tunneling of magnetization (QTM), since the former stabilizes the magnetization whereas the latter enables rapid relaxation and undermines magnetic memory. Here, we systematically investigate the magnetic stability and relaxation dynamics of Ho (4f10, J = 8) and Tb (4f8, J = 6) adatoms adsorbed on defective hexagonal boron nitride (Dh-BN) with C3v symmetry, using an integrated approach combining density functional theory (DFT+U+SOC) and model Hamiltonian analysis. Our results reveal that the interplay between total angular momentum J and crystal field symmetry dictates the intrinsic magnetic stability. For Ho@Dh-BN, C3v symmetry protects the degenerate |J = 8, mJ ≈ ±8⟩ ground states from QTM, as transverse crystal field terms (ΔmJ = ±3) cannot mix the |±8⟩ states. This yields a substantial effective reversal barrier of Urev = 28.72 meV and an Arrhenius magnetic lifetime of 1150 s at 12 K, demonstrating robust zero-field stability. In stark contrast, Tb@Dh-BN exhibits strong mixing of its |J = 6, mJ ≈ ±6⟩ ground states via QTM channels, resulting in a vanishing reversal barrier and no magnetic stability at zero field. Remarkably, applying an external magnetic field (B = 8 T) along the easy axis can restore the stability in the Tb system: the magnetic field lifts the ground-state degeneracy to suppress QTM by purifying the wave functions and forces magnetization reversal to proceed via multistep spin-flip pathways. This raises an effective barrier to Urev = 42.10 meV and extends the Arrhenius magnetic lifetime to 791 s at 18 K. Our work establishes two complementary design principles for achieving long spin lifetimes in lanthanide SAMs: intrinsic protection through favorable combinations of J and crystal field symmetry that inherently forbid QTM, and active field-induced stabilization that dynamically suppresses QTM in otherwise unstable systems. The findings provide a comprehensive microscopic understanding of magnetic relaxation in surface-supported lanthanide atoms and offer a clear theoretical roadmap for engineering electrically or magnetically addressable atomic-scale memory devices.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"13 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360347","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":"Abnormal Increase in Thermal Diffusivity of Lignin-Based Carbon Fibers during Vacuum Exposure","authors":"Jianchi Huang,Pengyu Hu,Haoran Cui,Amin Karamati,Theodore Maranets,Xingyu Wang,Xiuxia Zhang,Wangda Qu,Yan Wang,Xinwei Wang","doi":"10.1021/acs.jpcc.6c05759","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c05759","url":null,"abstract":"Vacuum generally suppresses gaseous heat conduction without altering intrinsic transport of solid materials. Here we report an unexpected, time-dependent increase in thermal diffusivity (α) of lignin-based carbon fibers (CFs) during vacuum exposure. At <0.08 Pa, α increases by up to ∼95% and approaches saturation, while its electrical resistance (R) shows smaller, condition-dependent changes. After ∼16 h of air re-exposure, α partially or nearly fully recovers, while R responds less consistently, demonstrating strong dependence on exposure history. Across the vacuum systems examined, the α increase diminishes as vacuum pressure rises from <0.08 to 2.13 Pa, whereas a moderate temperature rise (∼50 K) accelerates the evolution of the α increase under ∼0.21 Pa vacuum. Laser-power-normalized Raman intensities increase during air re-exposure without significant D- or G-band shifts, providing indirect evidence of reversible near-surface-state evolution rather than restructuring of the carbon framework. Atomistic simulations show that adsorbed water shortens acoustic phonon lifetimes and suppresses in-plane thermal transport. These results support vacuum-induced desorption of near-surface adsorbates as reducing phonon scattering and increasing α, as there is negligible change in volumetric heat capacity. Removal of humidity-assisted charge-transport pathways may also contribute to the increase in R observed in some sequences. It is concluded that the exposure history is an important factor in thermal and electrical measurements of carbon fibers under vacuum.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"12 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149360290","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}