The Journal of Physical Chemistry Letters最新文献_第7页

Plasmon-Induced Degradation of Short-Chain PFAS by Noble Metal Nanoclusters. 等离子体诱导的贵金属纳米团簇降解短链PFAS。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-31 DOI: 10.1021/acs.jpclett.5c01683

Samir Kumar Nayak, Khushboo Bhardwaj, P K Verma, Sharma S R K C Yamijala

{"title":"Plasmon-Induced Degradation of Short-Chain PFAS by Noble Metal Nanoclusters.","authors":"Samir Kumar Nayak, Khushboo Bhardwaj, P K Verma, Sharma S R K C Yamijala","doi":"10.1021/acs.jpclett.5c01683","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01683","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) are widely used in industry and consumer products due to their unique physical and chemical properties. However, due to their toxicity and environmental persistence, the production of long-chain PFAS such as perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) has been systematically phased out. Instead, short-chain PFAS have been widely used as replacements for long-chain PFAS. However, recent studies indicate that even short-chain PFAS can be toxic to the environment. Despite numerous attempts, complete degradation of these short-chain PFAS has not yet been achieved, leaving room for further exploration. In this work, we explored the potential of plasmonic silver (Ag) and gold (Au) nanoclusters (NCs) in the complete degradation of short-chain PFAS. By considering icosahedral Ag55 and Au55 NCs, as well as different types of PFAS, we present a thorough study of plasmon-induced processes for NC-PFAS complexes. Among different decay channels, our study focuses on plasmon decay through the direct hot electron transfer (DHET) and direct hot hole transfer (DHHT) pathways from NC to PFAS. Our calculations reveal that DHET is more probable in Ag-PFAS complexes and DHHT is more probable in Au-PFAS complexes. Furthermore, among all complexes, the Ag-PFBS complex exhibits the highest DHET with a total probability of 10%. Our Ehrenfest molecular dynamics simulations show that the PFAS in Ag-PFAS complexes undergo efficient degradation in the presence of these hot carriers, albeit at different rates.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"8046-8055"},"PeriodicalIF":4.6,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144751890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Multifunctional Pentafluorobenzoic Acid Boosts the Efficiency and Stability for Tin Halide Perovskite Solar Cells. 多功能五氟苯甲酸提高卤化锡钙钛矿太阳能电池的效率和稳定性。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-30 DOI: 10.1021/acs.jpclett.5c01921

Yong Guo,Miao Zhang,Junke Liu,Cheng Wu,Pengyu Yan,Jialin Du,Liming Ding,Feng Hao

{"title":"Multifunctional Pentafluorobenzoic Acid Boosts the Efficiency and Stability for Tin Halide Perovskite Solar Cells.","authors":"Yong Guo,Miao Zhang,Junke Liu,Cheng Wu,Pengyu Yan,Jialin Du,Liming Ding,Feng Hao","doi":"10.1021/acs.jpclett.5c01921","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01921","url":null,"abstract":"Tin halide perovskite solar cells (TPSCs) have made remarkable breakthroughs in photovoltaic performance recently. However, the Sn2+/Sn4+ oxidation has limited the stability of TPSCs, which is related to many factors, including film crystallinity, hydrophobicity, etc. In this work, we report a multifunctional molecule of pentafluorobenzoic acid (PFBA) as an additive into tin halide perovskite to enhance the stability. The carboxyl and hydroxyl groups in PFBA effectively acted with SnI2 through Lewis acid-base addition and hydrogen bonding, respectively, which effectively regulated the crystallization process of tin halide perovskite and reduced the lattice stress, thus avoiding defect-induced recombination centers in TPSCs. In addition, the hydrophobicity of the -F functional group in PFBA was conducive to improving the hydrophobicity of the tin halide perovskite film, thus alleviating the invasion of water and oxygen. Finally, the target device with PFBA obtained a power conversion efficiency (PCE) of 11.59% and maintained 88.00% of the initial PCE after aging 1500 h in a N2 glovebox.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"96 1","pages":"8007-8013"},"PeriodicalIF":6.475,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144748032","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Stability Diagram of Layer-Polarized Quantum Hall States in Twisted Trilayer Graphene. 扭曲三层石墨烯中层极化量子霍尔态的稳定性图。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-30 DOI: 10.1021/acs.jpclett.5c01221

Konstantin Davydov, Daochen Long, Jack A Tavakley, Kenji Watanabe, Takashi Taniguchi, Ke Wang

{"title":"Stability Diagram of Layer-Polarized Quantum Hall States in Twisted Trilayer Graphene.","authors":"Konstantin Davydov, Daochen Long, Jack A Tavakley, Kenji Watanabe, Takashi Taniguchi, Ke Wang","doi":"10.1021/acs.jpclett.5c01221","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01221","url":null,"abstract":"In the twisted trilayer graphene (tTLG) platform, the rich beating patterns between the three graphene layers give rise to a plethora of new length scales and reconstructed electronic bands arising from the emergent moiré and moiré-of-moiré superlattices. The coexisting lattices and superlattices interact and compete with each other to determine the overall transport properties of tTLG, the hierarchy of which can be electrostatically controlled by tuning the out-of-plane charge distribution or layer polarization. In this work, we measure the stability diagram of layer-polarized quantum Hall states in tTLG by systematically mapping out layer-specific Chern numbers in each layer and intra- and interlayer Chern transitions as a function of displacement field D and total carrier density n. In contrast to twisted bilayer systems, the rich interplay between the three atomic layers gives rise to a complex layer-polarized stability diagram with unconventional transport features that evolve rapidly with electric and magnetic fields. The stability diagram quantitatively characterizes the interlayer screening and charge distribution in tTLG with implication of strong interatomic-layer Coulomb coupling. Our work provides comprehensive guidance and insights into predicting and controlling layer-polarization and interlayer transitions in tTLG, and for tuning the individual role and interactions of each participating constituent toward novel material properties.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"7990-7997"},"PeriodicalIF":4.6,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144740609","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Higher Order Polaronic-Exciton Recombination in Two-Dimensional Dion-Jacobson-Type Perovskites. 二维dion - jacobson型钙钛矿中的高阶极化子-激子复合。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-30 DOI: 10.1021/acs.jpclett.5c01620

Somnath Biswas,Ruyan Zhao,Dwight S Seferos,Gregory D Scholes

{"title":"Higher Order Polaronic-Exciton Recombination in Two-Dimensional Dion-Jacobson-Type Perovskites.","authors":"Somnath Biswas,Ruyan Zhao,Dwight S Seferos,Gregory D Scholes","doi":"10.1021/acs.jpclett.5c01620","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01620","url":null,"abstract":"Understanding electronic and structural factors governing non-radiative recombination is key to developing hybrid low-dimensional materials for light-emitting applications. Here, we demonstrate that the ultrafast (0.6-5 ps) biexcitonic Auger process is the dominant exciton recombination pathway that occurs within the sub-picosecond to few picoseconds in two-dimensional Dion-Jacobson (2D DJ) hybrid perovskites. Studying two DJ perovskites with polaronic character and different exciton-phonon coupling, we reveal that ultrafast non-radiative recombination rates are primarily governed by strong exciton-phonon coupling and dielectric confinement in these materials. The third-order recombination rate reflects the interplay among exciton-phonon coupling, lattice distortion, band gap, and exciton binding energy. We show that Auger recombination occurs well below the Mott density in these 2D materials. We therefore establish a lower bound of 1.3 × 1019 cm-3 for the Mott density, much higher than that of three-dimensional (3D) perovskites. This work highlights the intrinsically ultrafast higher order recombination of polaronic-excitons in 2D DJ perovskites, emphasizing their unique excitonic properties and fundamental differences from conventional 3D systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"1 1","pages":"7998-8006"},"PeriodicalIF":6.475,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Symmetric Ligand Binding Pathways and Dual-State Bottleneck in [NiFe] Hydrogenases from Unbiased Molecular Dynamics. [NiFe]氢化酶的对称配体结合途径和双态瓶颈。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c01673

Farzin Sohraby, Ariane Nunes-Alves

引用次数: 0

Valence Bond Wave-Function-Based Automatic Diabatization Approach. 基于价键波函数的自动非对称化方法。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c01643

Yang Zhang,Jiao Li,Guoxia Gou,Ruru Wei,Dongping Chen,Peifeng Su,Wei Wu

{"title":"Valence Bond Wave-Function-Based Automatic Diabatization Approach.","authors":"Yang Zhang,Jiao Li,Guoxia Gou,Ruru Wei,Dongping Chen,Peifeng Su,Wei Wu","doi":"10.1021/acs.jpclett.5c01643","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01643","url":null,"abstract":"In this work, an automatic diabatization approach based on valence-bond (VB) wave functions, called VBADA, is proposed. Compared with the original VB based diabatization implementation [Zhang, Y.; et al. J. Phys. Chem. Lett. 2020, 11, 5295-5301; Zhang, Y.; et al. J. Phys. Chem. Lett. 2021, 12, 1885-1892], VBADA introduces two critical advancements: (1) the improved framework enables rigorous treatment of three-state diabatization, and (2) it relies on VB adiabatic wave functions rather than explicit Hamiltonian matrix operations. These are achieved by a novel criterion, which maximizes both the diversity of adiabatic VB wave functions and the trace of the adiabatic-to-diabatic (ATD) transformation matrix. The diabatic representations of two prototype hydrogen atom transfer (HAT) reactions, including Na + H2 → NaH + H and H + HCl → Cl + H2, is studied by employing VBADA. The computational results demonstrate that VBADA enables rigorous construction of three-state diabatic state, with benchmark validation showing exact numerical equivalence to conventional VB based diabatization implementation in two-state systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"31 1","pages":"7921-7928"},"PeriodicalIF":6.475,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720315","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Onset and Morphological Evolution of Cooperativity in Glass-Forming Liquids Composed of Anisotropically Shaped Molecules. 各向异性分子组成的玻璃形成液体中协同性的发生和形态演化。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c01863

M Rams-Baron,A Błażytko,M Matussek,P Lodowski,A Radoń,M Paluch

{"title":"Onset and Morphological Evolution of Cooperativity in Glass-Forming Liquids Composed of Anisotropically Shaped Molecules.","authors":"M Rams-Baron,A Błażytko,M Matussek,P Lodowski,A Radoń,M Paluch","doi":"10.1021/acs.jpclett.5c01863","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01863","url":null,"abstract":"Many theories attribute the dramatic slowdown in glass-forming liquid dynamics to a transition from independent to cooperative molecular motion. Although the concept of cooperative rearranging regions (CRRs) is well established, the microscopic nature of these regions and their evolution upon cooling remain subjects of active investigation. Molecules with anisotropic shapes offer a new perspective, as molecular reorientations along their long and short axes act as distinct and complementary probes of emerging cooperativity. Here, we introduce model molecules with tailored dipole orientations and demonstrate that the temperature-dependent evolution of a bimodal dielectric response captures the transition from independent to cooperative dynamics. This clear spectroscopic signature marks a significant advance in our understanding of how cooperativity emerges and evolves in glass-forming systems. Upon cooling, CRRs adopt increasingly compact morphologies, leading to a reduction in effective shape anisotropy. This transition from anisotropic to isotropic CRR geometries reveals previously unrecognized mechanisms by which anisotropy becomes suppressed during vitrification.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"1 1","pages":"7953-7959"},"PeriodicalIF":6.475,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Adsorption of Fluorinated Ether Electrolyte Solvent Molecules on Boron Nitride Nanosheets Studied by Solid-State NMR and Computational Methods. 用固体核磁共振和计算方法研究氟醚电解质溶剂分子在氮化硼纳米片上的吸附。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c01962

Hridip Sarma,Jhonatan S Puelles,Shebin K Joby,Anthony Somers,Maria Forsyth,Steve Rowlands,Baozhi Yu,Paul M Bayley,Fangfang Chen,Luke A O'Dell

引用次数: 0

One-Step Exsolution Strategy for the Reconstruction of the RuO2/La0.9Fe0.92Ru0.08O3 Composite for the Enhanced Oxygen Evolution Reaction. 一步溶出策略重建RuO2/ la0.9 fe0.92 ru0.080 o3复合材料增强析氧反应

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c01769

Xin Hu,Wei Cheng,Xin Zhang,Tianyi Wang,Shaoheng Cheng,Nan Gao,Hongdong Li

{"title":"One-Step Exsolution Strategy for the Reconstruction of the RuO2/La0.9Fe0.92Ru0.08O3 Composite for the Enhanced Oxygen Evolution Reaction.","authors":"Xin Hu,Wei Cheng,Xin Zhang,Tianyi Wang,Shaoheng Cheng,Nan Gao,Hongdong Li","doi":"10.1021/acs.jpclett.5c01769","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01769","url":null,"abstract":"The noble metal oxide RuO2 is an efficient catalyst for the oxygen evolution reaction (OER), and its catalytic activity can be significantly improved by Ru exsolution and subsequent oxidation to RuO2 nanoparticles on the perovskite surface. Conventional methods typically require sequential H2/Ar reduction for Ru exsolution followed by oxidation, which complicates the process and introduces potential safety hazards. Herein, we propose introducing nanodiamond (ND) into La0.9Fe0.92Ru0.08O3 (LFR) gels for ambient calcination. ND facilitates Ru exsolution and oxidation to RuO2, significantly simplifying RuO2/LFR preparation. The ND-modified RuO2/LFR exhibits high OER activity, achieving an overpotential of 275 mV at 10 mA cm-2 and a Tafel slope of 48.16 mV decade-1. This Tafel slope represents a 50% reduction compared to that of pure RuO2. Furthermore, the catalyst retains 84% of its initial current density after 24 h. Our work provides insight into enhancing electrocatalytic activity by a one-step in situ exsolution of metal oxides.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"59 1","pages":"7944-7952"},"PeriodicalIF":6.475,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Benign Hydrogen Vacancy in Bromide-Based Organic-Inorganic Hybrid Perovskites. 溴基有机-无机杂化钙钛矿中的良性氢空位。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-07-29 DOI: 10.1021/acs.jpclett.5c02036

Shi-Yao Liu,Xingxing Jiang,Bing-Bin Li,Zhen-Kun Tang,Chuan-Jia Tong

引用次数: 0