Physical Chemistry Chemical Physics最新文献_第8页

Hybrid moiré excitons in strained heterobilayer of transition metal dichalcogenides

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-15 DOI: 10.1039/d4cp04759a

Houssem Eddine Hannachi, Sihem Jaziri

{"title":"Hybrid moiré excitons in strained heterobilayer of transition metal dichalcogenides","authors":"Houssem Eddine Hannachi, Sihem Jaziri","doi":"10.1039/d4cp04759a","DOIUrl":"https://doi.org/10.1039/d4cp04759a","url":null,"abstract":"In this paper, we theoretically study the effects of twist and heterostrain on moiré excitons in the $MoSe_2/WSe_2$ heterobilayer. Using a continuum model, we analyze the band structures and wavefunction distributions of moiré excitons, photoluminescence spectra, and the hybridization between interlayer and intralayer moiré excitons. Our key findings reveal that, under the influence of twisting effect, moiré excitons flat bands emerge. Additionally, we observe that the bright states exhibit a linear and quadratic dependence on the twist angle. We predict the existence of a critical twist angle, $theta_c simeq 2^circ$, which distinguishes between localized and delocalized regimes. In contrast, the three-fold rotational symmetry breaking induced by heterostrain leads to significant tunability of the exciton band structure and the distribution of bright states. Moreover, exploring the strain magnitude and direction may enhance the brightness of moiré exciton bright states, emphasizing the importance of strain orientation in excitonic optical modulator applications. Furthermore, the combined effects of twist and strain result in a high degree of tunability in the hybridization between interlayer and intralayer excitons. Interestingly, under specific strain magnitudes and directions, such as normal compressive strain, we observe the emergence of a topological moiré exciton Chern insulator, featuring the protected edge modes. Our predictions may pave the way for exploring novel topological exciton phenomena and moiré exciton-correlated physics. They are particularly intriguing for potential device applications in the excitonic quantum anomalous Hall effect (EQAHE) enabled by the combined effects of strain and twist.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"108 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837450","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

Research on the Influence of Ultraviolet Radiation on OLED and the Luminance Attenuation Model of Light Aging

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-15 DOI: 10.1039/d5cp00664c

Lulu Zhou, Zhanhan Hu, Wei Shi, Yixiao Zhang, Yangyang Zhu, Yi Liao, Yachen Xu, Jialu Gu, Weixia Lan, Bin Wei

引用次数: 0

Correlations between free volume structure and ionic conductivity of poly (ethylene oxide) and dendritic fibrous nanosilica composite based electrolyte: An investigation using positron annihilation and broadband dielectric spectroscopy

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-15 DOI: 10.1039/d4cp04826a

Jaideep Mor, Kanaklata Pandey, Sandeep Kumar Sharma

{"title":"Correlations between free volume structure and ionic conductivity of poly (ethylene oxide) and dendritic fibrous nanosilica composite based electrolyte: An investigation using positron annihilation and broadband dielectric spectroscopy","authors":"Jaideep Mor, Kanaklata Pandey, Sandeep Kumar Sharma","doi":"10.1039/d4cp04826a","DOIUrl":"https://doi.org/10.1039/d4cp04826a","url":null,"abstract":"Passive and active fillers loaded poly(ethylene oxide), PEO, based solid state polymer electrolytes (SPEs) are considered promising alternatives for currently used flammable liquid electrolytes in lithium metal batteries. The enhancement in ionic conductivity of PEO based composite electrolytes is attributed to the additional ion-conduction pathways available at the interphase region. Considering this aspect, in the present study, we have prepared dendritic fibrous nanosilica (DFNS) loaded PEO based polymer composite (PEO-DNFS) and electrolytes (PEO-Li, PEO-Li-DFNS) having (EO:Li = 20:1). DFNS has been chosen as filler due to its unique dendritic fibrous structure which is expected to create large interphase region in the composites. These composites and electrolytes were characterized using various techniques viz. powder X-ray diffraction (PXRD), attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR), differential scanning calorimetry (DSC) for determining the modifications in chemical bonding and thermal properties. Positron annihilation lifetime spectroscopy (PALS) and broadband dielectric spectroscopy (BDS) were employed to determine the modifications in the free volume structure/chain packing of PEO and ion conduction mechanism, respectively. The relative free volume was observed to increase with DFNS loading due to modifications in the chain packing. The higher number of free volume holes provide additional pathways for ionic diffusion leading to an enhancement in ionic conductivity. The role of relative free volume in ionic conductivity enhancement is further established through the strong coupling observed between ionic conduction and segmental relaxations of PEO electrolytes investigated using BDS.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"119 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143832139","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

Is the DBU-CO2 Adduct Stable in Ionic Liquid Media?

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-15 DOI: 10.1039/d5cp00899a

Giovanni Rodrigues Morselli, Frederik Philippi, Pedro Henrique Sabanay, R Bazito, Margarida Costa Gomes, Rômulo Augusto Ando

引用次数: 0

Understanding the Excited State Decay Mechanism of Complex Systems: A General First-Order Kinetic Model

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-15 DOI: 10.1039/d5cp00606f

Aline De Souza Bozzi, Rita de Cássia Oliveira Sebastião, Willian R. Rocha

{"title":"Understanding the Excited State Decay Mechanism of Complex Systems: A General First-Order Kinetic Model","authors":"Aline De Souza Bozzi, Rita de Cássia Oliveira Sebastião, Willian R. Rocha","doi":"10.1039/d5cp00606f","DOIUrl":"https://doi.org/10.1039/d5cp00606f","url":null,"abstract":"In this work, we have proposed and evaluated a first-order kinetic model to describe the excitedstates dynamics of molecules as a computationally cheaper alternative to describe and understand the photophysical profile of large systems. The method is based on calculating the radiative and nonradiative rate constants of all photophysical processes of a collection of crucial low-lying excited states and modeling the decay over time using a first-order kinetic model. We have successfully applied the method to the [Ru(bpz)3]2+ (bpz = 2,2’-bipyrazyl) complex as a case study, obtaining good results. By employing this first-order kinetic model, it is possible to simulate the time-dependent decay process and the evolution of the excited-state population, revealing not only the primary deactivation pathway but also secondary states that contribute to the overall decay mechanism, highlighting alternative channels that may lead to photochemical side products. This approach provides a computationally efficient yet accurate method for studying more intricate systems relevant to photoinduced processes. It enhances the understanding of these compounds and offers guidance for fine-tuning their chemical and structural properties for targeted applications.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"50 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837396","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

Theoretical Study on Catalytic Ammonia Synthesis by Trimetallic Clusters with or without Sumanene Support

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-14 DOI: 10.1039/d5cp00926j

Xiao-Meng Huang, Zhi-Wen Ji, Xun-Lei Ding, Yan Chen, Wei Li, Jiao-Jiao Chen, Shao-Peng Xu, Lin-Lin Li

{"title":"Theoretical Study on Catalytic Ammonia Synthesis by Trimetallic Clusters with or without Sumanene Support","authors":"Xiao-Meng Huang, Zhi-Wen Ji, Xun-Lei Ding, Yan Chen, Wei Li, Jiao-Jiao Chen, Shao-Peng Xu, Lin-Lin Li","doi":"10.1039/d5cp00926j","DOIUrl":"https://doi.org/10.1039/d5cp00926j","url":null,"abstract":"DFT calculations were utilized to explore the electrocatalytic nitrogen reduction reaction (NRR) mechanisms catalyzed by trimetallic clusters M3 (M = Ti, Zr, V, and Nb), both unsupported and supported by bowl-shaped sumanene. The substrate enhanced N2 adsorption and activation but hindered hydrogenation due to more negative adsorption energies. The substrate promoted hydrogenation on nitrogen, reducing the interference of the hydrogen evolution reaction (HER) and enhancing the NRR selectivity. Three fundamental and three mixed pathways were investigated, and the rate-determining step (RDS) was identified for each pathway. Both through a consecutive pathway, V3 exhibits the best catalytic performance with the free energy change of the RDS (ΔGRDS) as 0.82 eV, while the optimal supported catalyst, Nb3 supported on sumanene, has a ΔGRDS of 1.43 eV. The introduction of the substrate generally increased ΔGRDS by 0.3-0.8 eV. The substrate can effectively regulate the distance between metal atoms and reduce the change in geometric structures of M3 clusters during the reaction process, thereby enhancing the structural stability of the active sites in the NRR process. The substrate can reduce the reactivity differences among catalysts with different metal types. This so-called blurring effect allows cheap metals to partially replace noble metals while maintaining catalyst performance. A linear correlation between charge changes on M3 or M3 together with the substrate and ΔG was observed, providing a potential method for optimizing the catalyst performance and designing new catalysts.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"108 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827480","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

Reactive Uptake via Inelastic Scattering of CN Radicals at a Liquid Hydrocarbon Surface

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-14 DOI: 10.1039/d5cp00406c

Paul David Lane, Katya E Moncrieff, Stuart Greaves, Kenneth G McKendrick, Matthew L Costen

{"title":"Reactive Uptake via Inelastic Scattering of CN Radicals at a Liquid Hydrocarbon Surface","authors":"Paul David Lane, Katya E Moncrieff, Stuart Greaves, Kenneth G McKendrick, Matthew L Costen","doi":"10.1039/d5cp00406c","DOIUrl":"https://doi.org/10.1039/d5cp00406c","url":null,"abstract":"Collisions of ground-electronic-state CN radicals with the surface of a prototypical saturated-hydrocarbon liquid have been studied experimentally. A molecular beam of CN(X2Σ+) with a mean laboratory-frame kinetic energy of 44 kJ mol-1 was directed at normal incidence at a continually refreshed liquid squalane (2,6,10,15,19,23-hexamethyltetracosane) surface. The incident and scattered CN radicals were detected in a range of rotational states by multi-pass frequency-modulated absorption spectroscopy on selected lines of the CN(A-X) transition. The ratio of scattered-to-incident CN populations for squalane were compared with those obtained previously for a reference liquid, perfluoropolyether (PFPE), which is assumed to be inert. The overall survival probability, summed over the significantly populated rotational levels, of CN on squalane was found to be 0.15 ± 0.04. The 85% that is lost is inferred, on energetic grounds, to produce HCN via H-atom abstraction. The surviving CN has a significantly superthermal rotational distribution and a hot, non-thermal velocity distribution in the direction perpendicular to the surface normal. These dynamical attributes are characteristic of impulsive scattering. However, we conclude that the low survival probability is not compatible with a simple, ‘single-bounce’ mechanism and hence that multiple-encounter trajectories must contribute significantly to CN reactive loss. We find no evidence of a distinct trapping-desorption component, corresponding to full thermal accommodation, in the surviving CN from either squalane or PFPE at these collision energies.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"119 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827478","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

High-Efficiency and Stable Perovskite Solar Cells via DL-Methionine-Enhanced Crystallization and Defect Passivation

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-14 DOI: 10.1039/d4cp04698f

Xiaolan Li, Yanwei Xu, Fuxing Chen, Dongxing Lu, Yajun Zhu, Cong Li

{"title":"High-Efficiency and Stable Perovskite Solar Cells via DL-Methionine-Enhanced Crystallization and Defect Passivation","authors":"Xiaolan Li, Yanwei Xu, Fuxing Chen, Dongxing Lu, Yajun Zhu, Cong Li","doi":"10.1039/d4cp04698f","DOIUrl":"https://doi.org/10.1039/d4cp04698f","url":null,"abstract":"As an emerging photovoltaic technology, perovskite solar cells (PSCs) have become a research hotspot due to their excellent photoelectric conversion efficiency (PCE) and low-cost manufacturing process. Enhancing the crystallization quality of perovskite films and mitigating defects through material engineering is crucial for improving the performance of PSCs. In this study, a naturally occurring amino acid, DL-Methionine, is incorporated as an additive to enhance the crystallization quality and passivate defects in perovskite films. The results show that the appropriate concentration of DL-Methionine additive can not only improve the crystallization kinetics of perovskite but also reduce the defects of perovskite films through its coordination with perovskite ions, thereby reducing defect-assisted recombination. Finally, the optimized PSCs based on the DL-Methionine additive obtained the highest power conversion efficiency of 24.72%, significantly higher than those without the DL-Methionine additive (21.83%). Moreover, the stability of PSCs is significantly improved with the DL-Methionine additive. This work demonstrates the potential of DL-Methionine as an effective passivation agent for high-efficiency and stable PSCs.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"21 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827350","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

Ultrafast photophysics of the cyan fluorescent protein chromophore in solution

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-14 DOI: 10.1039/d5cp00942a

Anam Fatima, Eleanor K Ashworth, Isabelle Fernandes, A. N. Cammidge, Giovanni Bressan, Steve R. Meech, James N Bull

{"title":"Ultrafast photophysics of the cyan fluorescent protein chromophore in solution","authors":"Anam Fatima, Eleanor K Ashworth, Isabelle Fernandes, A. N. Cammidge, Giovanni Bressan, Steve R. Meech, James N Bull","doi":"10.1039/d5cp00942a","DOIUrl":"https://doi.org/10.1039/d5cp00942a","url":null,"abstract":"Incorporation of fluorescent proteins (FPs) into biological systems has revolutionised bioimaging and the understanding of cellular processes. Ongoing developments of FPs are driving efforts to characterise the fundamental photoactive unit (chromophore) embedded within the protein. Cyan FP has a blue emitting chromophore and is widely used in Forster resonance energy transfer studies. Here, we probe the ultrafast photophysics of the cyan FP chromophore in solution using time resolvedfluorescence up-conversion and transient absorption spectroscopies. The ultrafast dynamics are characterised by two lifetimes, sub-picosecond τ1 (or τF) associated with loss of the fluorescent Franck-Condon state, and lifetime τ2 on the order of several picoseconds that is linked with cooling of a hot ground state. MRSF-TDDFT calculations show that the relaxed S1 state equilibrium geometry is classified as a partial twisted intramolecular charge-transfer state, and lies close in energy to a conical intersection seam associated with torsion about the central double bond leading to facile internal conversion. The excited state dynamics exhibit only a weak viscosity dependence, consistent with a barrierless and near-volume-conserving non-radiative decay mechanism. Fluorescence lifetimes for the deprotonated anion are twice those for the neutral.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"34 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827479","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

Electron impact single and double ionization and dissociation: revisiting CF4 and CHF3 with an improved experimental method

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-14 DOI: 10.1039/d5cp00746a

Mevlut Dogan, Wania Wolff, Deepthy Maria Mootheril, Thomas Pfeifer, Alexander Dorn

引用次数: 0