The Journal of Physical Chemistry C最新文献

{"title":"Crystallization Behavior of Ambient-Air-Processed CsPbBr3 Thin Films on Various Electron Transport Layers and Its Impact on Solar Cell Performance","authors":"Annisa Nandhita Kurniawati, Xorell Ivanov Monov, Bening Tirta Muhammad, Prima Fitri Rusliani, Phutri Milana, Roni Adi Wijaya, Ahmad Ibrahim, Shobih, Natalita Maulani Nursam, Gunawan, Nandang Mufti, Veinardi Suendo, Lydia Helena Wong, Kartika Sari, Brian Yuliarto, Wilman Septina","doi":"10.1021/acs.jpcc.5c03182","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c03182","url":null,"abstract":"CsPbBr₃ perovskite is a promising wide-bandgap semiconductor for photovoltaic applications, but its crystallization dynamics and charge transport properties are highly dependent on interfacial interactions with electron transport layers (ETLs). This study systematically investigates the influence of ETLs: SnO₂, TiO₂, and In₂S₃, on the crystallization, morphology, and photovoltaic performance of CsPbBr₃ thin films processed under ambient-air conditions. The choice of ETL is found to significantly affect the structural evolution of the PbBr₂ precursor and the final CsPbBr₃ film, impacting the device efficiency. Among the studied ETLs, SnO₂ promotes the formation of compact and uniform CsPbBr₃ films, leading to the highest power conversion efficiency (PCE) of 5.05%. In comparison, TiO₂-based devices exhibit a moderate efficiency of 3.44% due to suboptimal film flatness, whereas In₂S₃ results in small-grained films with high defect densities, limiting the efficiency to 0.70%. Photoluminescence and impedance spectroscopy analyses further confirm that SnO₂ effectively suppresses defect-mediated recombination, enhancing charge transport and extraction. These findings underscore the crucial role of ETL selection in optimizing CsPbBr₃ crystallization and provide valuable insights for developing efficient wide-bandgap perovskite solar cells under ambient conditions.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"19 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145314831","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":"Boosting Hot Electron Generation of Plasmonic Nanoparticles in TiO2/TiN Nanocavities for Solar Energy Conversion","authors":"Zahra Ashrafi-Peyman, Amir Jafargholi, Alireza Z. Moshfegh","doi":"10.1021/acs.jpcc.5c03594","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c03594","url":null,"abstract":"The efficient generation and harvesting of hot electrons (HEs) remains a key challenge in advanced nanophotonic applications. Here, we propose a novel strategy to boost HE generation by incorporating plasmonic nanoparticles (NPs)─including Au, Ag, Pt, and TiN─into TiO₂/TiN nanocavities. While our previous study on TiO₂/TiN nanotube arrays achieved excellent optical absorption across 200–1300 nm, it showed weak absorption in the 350–600 nm visible range. To overcome this limitation, we decorate the nanostructure with plasmonic NPs. Comprehensive analytical, finite-difference time-domain (FDTD), and finite element method (FEM) simulations reveal strong coupling between nanocavity modes and plasmonic Mie resonances, leading to significantly enhanced absorption in the visible range. Among the examined materials, the optimized 70 nm TiN NPs placed at the bottom of the nanocavity demonstrate the best performance, outperforming noble metals in both optical and cost efficiency. Quantum mechanical analysis of HE generation shows that the TiN NPs within TiO₂/TiN nanocavities achieve a hot carrier generation rate of ∼10¹⁴ s^–1 at a wavelength of 600 nm, with a red-shifted spectral response compared to noble metals. The observed HE enhancement is attributed to localized electric fields (hot spots) induced by Mie resonances. These findings pave the way for advanced hot electron device engineering with potential applications in photodetectors, photocatalysis, and solar energy conversion in the visible spectrum.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"5 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306270","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":"Functionalization-Driven Formation of TiO2/Ti2CTx Interfaces","authors":"Néstor García-Romeral, Giovanni Di Liberto, Ángel Morales-García, Francesc Viñes, Francesc Illas, Gianfranco Pacchioni","doi":"10.1021/acs.jpcc.5c04505","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c04505","url":null,"abstract":"In this study, the nature of the interface between TiO₂ and MXenes was systematically explored by using density functional theory and taking Ti₂C as a case study. TiO₂/MXene interfaces are emerging as potential photoactive systems, but a deep understanding of their nature is often elusive. Our findings reveal that MXene surface functionalization predominantly governs the interaction between TiO₂ and MXenes. Specifically, when the Ti₂C MXene is terminated with −H or −OH or when it is not functionalized, the formation of the interface leads to a strong interaction due to the formation of new chemical bonds. Weak van der Waals interactions are present when the Ti₂C MXene surface termination involves −F, −Cl, or −O groups. The analysis of the interface polarization shows a systematic charge transfer from MXene surfaces toward TiO₂, which is localized at the interface and influenced by MXene functionalization. The results of this study provide new atomistic insights on the interaction between these two materials, helping the understanding of the nature of this emerging class of photoactive materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"100 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306272","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":"Predictive Quantum Mechanics-Based Force Field for Iron Oxide Systems: Mechanical, Dielectric, and Piezoelectric Response in Hematite, Magnetite, Maghemite, and Wüstite","authors":"Vigila N. Vijayakumar, Tridip Das, Andres Jaramillo-Botero, William A. Goddard, III, Fahmi Bedoui","doi":"10.1021/acs.jpcc.5c03757","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c03757","url":null,"abstract":"Iron oxide systems are well-known for their diverse magnetic and electronic properties, making them pivotal in materials science, catalysis, and biomedical applications. Among these, Fe₃O₄ (magnetite) stands out as a ferrimagnetic half-metallic material with exceptional versatility. Through controlled oxidation or reduction, Fe₃O₄ can transform into other iron oxide phases, such as wüstite (Fe_1–<i>x</i>O), an antiferromagnetic phase, or γ-Fe₂O₃ and α-Fe₂O₃, which exhibit ferrimagnetic and antiferromagnetic insulating behaviors, respectively. These phase transitions provide a unique platform for tuning the magnetic and electrical properties of iron oxides. In this work, we present the development of a novel force field (FF′) specifically designed to model the structural, mechanical, dielectric, and piezoelectric properties of iron oxide systems. By capturing the intrinsic relationships between Fe₃O₄ and its oxidized and reduced counterparts, this force field provides a unified framework for simulating phase transitions and property tuning in iron oxides. The force field is parametrized based on the quantum-mechanical structure of Fe₃O₄ and extended to accurately describe the properties of γ-Fe₂O₃, α-Fe₂O₃, and Fe_1–<i>x</i>O. Our FF′ successfully reproduced quantum mechanical calculations for the elastic constants, dielectric responses, and piezoelectric coefficients across these phases. This study highlights the potential of FF′ as a robust tool for molecular dynamics simulations of iron oxide systems across diverse compositions and applications. The ability to accurately model phase-dependent magnetic and electric properties makes this force field particularly valuable for advancing the design of magnetoelectric devices, catalysts, sensors, and biomedical materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"12 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306285","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":"Structural Stability and Kinetics of Hydrogenation of β-Tantalum at Low Temperatures","authors":"Ziqing Yuan, Herman Schreuders, Ewout Voorrips, Robert Dankelman, Roger M. Groves, Bernard Dam, Lars J. Bannenberg","doi":"10.1021/acs.jpcc.5c05265","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05265","url":null,"abstract":"The development of reliable hydrogen sensing materials for subzero environments is crucial for aviation, cryogenic storage, and hydrogen infrastructure applications. In this study, we investigate tetragonal β-tantalum (β-Ta) thin films at −60 °C to assess their potential for optical hydrogen sensing. <i>In situ</i> X-ray diffraction (XRD) measurements reveal a reversible lattice expansion upon hydrogen exposure, with β-Ta exhibiting a smaller volumetric expansion compared to α-Ta, indicating lower hydrogen solubility. Optical transmission measurements demonstrate a monotonic and fully reversible optical response across a range of hydrogen pressures, free of any hysteresis. However, β-Ta exhibits prolonged response times at low temperatures due to diffusion-limited kinetics, as confirmed by power-law response rate analysis and direct diffusion front measurements. Although β-Ta offers a temperature-independent resolution and structural robustness, its slower response time suggests the need for further microstructural optimizations to enhance hydrogen diffusion.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"106 5 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145295541","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":"Weak *CO-Binding Dopants in Cu-Based Single-Atom Alloys Serving as Diffusion-Assisting Mediators to Facilitate C–C Coupling","authors":"Yanpu Niu, Haolan Tao, Jingkun Li, Cheng Lian, Honglai Liu","doi":"10.1021/acs.jpcc.5c04850","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c04850","url":null,"abstract":"Copper-based single-atom alloy (SAA) catalysts exhibit tunable C–C coupling behavior during CO₂ reduction, governed by dopant-dependent metal–carbon (M–C) interactions. Combining density functional theory (DFT) calculation and ab initio molecular dynamics (AIMD) simulation, this study systematically investigates dopant effects across three C–C coupling pathways: *CO+*CO, *CO+*COH, and *CO+*CHO. Compared to *COH and *CHO, *CO is identified as the primary migratory intermediate governing coupling kinetics due to its weak adsorption and low coordination number. Strong M–C interactions (e.g., Ni-doped Cu) anchor *CO at dopant sites, suppressing migration and increasing C–C coupling barriers. Conversely, weak M–C interactions (e.g., Zn-doped Cu) destabilize *CO adsorption, enabling its migration between Cu sites and reducing C–C coupling energy barriers compared to pristine Cu. We propose an assisted-diffusion mechanism in which dopants with weak M–C interactions promote *CO migration for C–C coupling by acting as diffusion mediators rather than active adsorption sites, thereby enhancing the Faraday efficiency of the overall multicarbon product. These findings provide atomic-scale insights for designing high-activity Cu-based SAAs via the targeted modulation of dopant–C interactions.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"198 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306286","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":"Spectroelectrochemical Properties of Floating Lipid Membranes in Tris Organic Buffer","authors":"Marta Majewska, Justyna Bożek, Damian Dziubak, Sławomir Sęk, Izabella Brand","doi":"10.1021/acs.jpcc.5c00996","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c00996","url":null,"abstract":"In biologically and biotechnologically relevant applications, the use of organic biological buffers, e.g. Tris or HEPES, is essential to maintain the activity and stability of biomacromolecules. Knowledge of how organic biological buffers affect the properties of free-standing floating bilayers is very limited. In this work, the properties of floating lipid bilayers were investigated in Tris buffer solution. The model lipid bilayer contains zwitterionic, neutral, and negatively charged lipids, representing the composition of the outer segment of photoreceptor cells. The electrochemical characterization of the floating bilayer (membrane resistance, membrane conductance, and capacitance) differs significantly between Tris and inorganic electrolyte solutions. To discover the differences in the supramolecular structure of the floating model membrane which are introduced by a selection of an electrolyte solution, <i>in situ</i> infrared spectroscopies: polarization modulation infrared reflection absorption spectroscopy and surface-enhanced infrared absorption spectroscopy techniques, were used. The weakly hydrated [TrisH]⁺ is conducted through the floating lipid bilayer independently of the applied potential. Accumulation of [TrisH]⁺ in the spacer layer leads to the outflux of hydrated water molecules once the pores in the membrane at negative potentials are formed. The results described in this manuscript provide crucial information on the tuning of the properties of the spacer layer allowing for incorporation of transmembrane proteins of different sizes in the extra-membranous space aiming at construction of model outer segment membranes.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"8 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289372","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":"Li1.75Zr0.75Sb0.25Cl4.75O0.625 Oxyhalide Solid Electrolyte: Enhancing Performance by Regulating Phase Transition","authors":"Pengfei Du, Peng Zhang, Zhenyang Shen, Yongmei Zhou, Qingtao Wang, Ying Liu","doi":"10.1021/acs.jpcc.5c05412","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05412","url":null,"abstract":"New types of halides have garnered significant attention from researchers in the development of high-performance all-solid-state lithium-ion batteries due to their exceptional high-potential stability, high ionic conductivity, and favorable mechanical properties. Here, a mechanochemical ball milling method is employed to synthesize the Li_{2–2<i>x</i>}Zr_{1–2<i>x</i>}Sb_2<i>x</i>Cl_{6–10<i>x</i>}O_5<i>x</i> material by incorporating an appropriate amount of Sb–O into Li₂ZrCl₆. Experimental results and Rietveld refinement confirm the successful synthesis of a zirconium-based chloride-oxide solid electrolyte material (Li_1.75Zr_0.75Sb_0.25Cl_4.75O_0.625). Due to the incorporation of Sb⁵⁺, which has a smaller ionic radius but a higher valence state, the volume of the condensed crystal lattice decreased, while the number of lithium vacancies increased. The incorporation of O^2– induced a phase transition in the crystal structure, leading to the redistribution of lithium ions. The combined effects of these factors enhanced the ionic conductivity. The lithium-ion conductivity of the electrolyte at 25 °C is 4.2 × 10^–4 S cm^–1, and it possesses a wide electrochemical stability window (1.22–4.62 V vs Li⁺/Li). Simultaneously, Sb–O dual doping enhances the electrochemical reduction stability of Li₂ZrCl₆. The all-solid-state battery utilizing Li_1.75Zr_0.75Sb_0.25Cl_4.75O_0.625 as the electrolyte and sc-NCM811 as the cathode demonstrates excellent cycling performance and a high capacity retention rate. These investigations offer a promising strategy for the rational design of zirconium-based halide solid-state electrolytes, which are essential for the development of high-performance all-solid-state batteries.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"2 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289158","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":"Nitrogen-Induced Defects in VSe2 Studied by Scanning Tunneling Microscopy","authors":"U. Chazarin, M. Lezoualc’h, W. W. Pai, R. Sankar, C. Chacon, Y. Girard, C. González, A. Smogunov, Y. J. Dappe, J. Lagoute","doi":"10.1021/acs.jpcc.5c05337","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05337","url":null,"abstract":"Atomic-scale studies of dopants in transition metal dichalcogenides (TMDs) are important for tailoring their physical and chemical properties and provide a clearer picture of structure–property correlations. Nitrogen atoms as dopants in TMD materials promise tuning of carrier type and enhanced catalytic properties, however, experimental studies have rarely addressed their atomic-scale details. Here, we present a study of nitrogen dopants in nitrogen-plasma-treated 1T-phase VSe₂ bulk crystals by scanning tunneling microscopy (STM) and spectroscopy (STS). Three main N-induced species are classified. One type (type-I) is shown to be substitutional N atoms at the bottom-layer Se sites. Type-II has a not-yet-determined structure. The final type-III N atom is an adsorbed N atom at quasi-bridge sites between Se atoms. This N atom species exhibits distinct tip-induced dynamical motion. Density functional theory (DFT) calculations corroborate experimental STM and STS features, lending support to the proposed models. These results highlight the great variety of even simple atomic dopants in TMD materials and the need to finely control their properties for future applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"1 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289156","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":"Quantitative Correlation between Ligand Shell Composition and Photoluminescence in CsPbBr3 Nanocrystals with Mixed Didodecyldimethylammonium Bromide and Oleic Acid Ligands","authors":"Diana T. Reyes-Castillo, Yoarhy A. Amador-Sánchez, Diego Solis-Ibarra, Daniel Finkelstein-Shapiro","doi":"10.1021/acs.jpcc.5c05690","DOIUrl":"https://doi.org/10.1021/acs.jpcc.5c05690","url":null,"abstract":"The optoelectronic properties of halide perovskite nanocrystals are strongly determined by their surface chemistry; therefore, their improvement hinges on a detailed understanding and control of their surface properties. Given that most recombination occurs at the surface, the ligand-induced reconstruction of the lattice can remove or add trapping sites that increase or decrease the emission quantum yield. Great strides have been made in elucidating the binding sites of different ligands along with their modification of the energy levels. However, quantitative measurement has not been fully achieved. In this work, we present a quantitative correlation between the composition of a mixed-ligand shell containing oleic acid (OA) and didodecyldimethylammonium bromide (DDAB) and the photoluminescence of CsPbBr₃. We identify three different regions corresponding to three different ligand shell compositions with their associated recombination dynamics and find that an added concentration of 0.5 mM of DDAB results in a surface with both Pb and Br defects maximally passivated by the ligand shell.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"91 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289157","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}