The Journal of Physical Chemistry Letters最新文献_第2页

Generalized Valence Bond-Based Block-Correlated Coupled Cluster Theory with up to Five-Pair Correlation for Accurate Static Correlation of Strongly Correlated Systems 基于广义价键的块相关耦合聚类理论，最多可达五对相关，用于强相关系统的精确静态相关

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-29 DOI: 10.1021/acs.jpclett.5c00990

FanHong Han, Pengfei Ma, Xiaochuan Ren, Wei Li, Shuhua Li

引用次数: 0

High Damage Threshold Plasmonic Nanocavity Realized by Single Semiconductor Nanowires for Strong Coupling 利用单半导体纳米线实现高损伤阈值等离子体纳米腔的强耦合

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-28 DOI: 10.1021/acs.jpclett.5c00593

Si Kan, Xiaobo Han, Lin Luo, Zijian He, Wenjuan Huang, Xiaohong Li, Huatian Hu, Kai Wang

{"title":"High Damage Threshold Plasmonic Nanocavity Realized by Single Semiconductor Nanowires for Strong Coupling","authors":"Si Kan, Xiaobo Han, Lin Luo, Zijian He, Wenjuan Huang, Xiaohong Li, Huatian Hu, Kai Wang","doi":"10.1021/acs.jpclett.5c00593","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00593","url":null,"abstract":"Strong coupling, as a unique paradigm of cavity quantum electrodynamics, provides an important foundation for exploring novel quantum phenomena. Under ambient conditions, exciton–plasmon strong coupling systems have developed rapidly with various exquisite nanocavity structures proposed and refined. Nanocavities based on metal nanoparticles, such as single-particle and nanoparticle-on-mirror (NPoM), offer excellent compatibility with exciton materials, making them significant platforms for studying plasmon-exciton strong coupling. However, the intrinsic losses of metallic materials severely limit the exploration of novel quantum phenomena such as low-threshold lasing and nonlinear properties. In this work, we propose and realize a plasmonic nanocavity based on high-refractive-index GaAs nanowires positioned on a Au substrate, forming a nanowire-on-mirror (NWoM) architecture. The NWoM nanocavities exhibit strong local field confinement and a significantly enhanced damage threshold, reaching 5.6×106 W/cm2. Furthermore, by integrating the nanocavity with monolayer WSe2, we successfully realized the strong coupling at room temperature. By tuning the diameters of the dielectric nanowires, we observe the characteristic anticrossing behavior and achieve a Rabi splitting of 140 meV. This study lays the foundation for future investigations into more efficient quantum behaviors and provides a new approach to designing low-loss strong coupling systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"57 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144165722","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

Alloying Engineering toward Tunable White Light-Emitting Perovskites 可调谐白光钙钛矿的合金化工程

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-28 DOI: 10.1021/acs.jpclett.5c01073

Deyu Li, Mingming Zhang, Yutong Zhang, Yi Han, Lei Wang, Xinfeng Liu, Jun Xing

引用次数: 0

Kinetic Mechanism for Fidelity of CRISPR-Cas9 Variants CRISPR-Cas9变体保真度的动力学机制

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-28 DOI: 10.1021/acs.jpclett.5c01154

Andrew D. Hecht, Oleg A. Igoshin

引用次数: 0

Two-Dimensional Electronic Spectroscopy in the Condensed Phase Using Equivariant Transformer Accelerated Molecular Dynamics Simulations 用等变变压器加速分子动力学模拟凝聚态的二维电子能谱

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-28 DOI: 10.1021/acs.jpclett.5c00911

Joseph Kelly, Frank Hu, Arianna Damiani, Michael S. Chen, Andrew Snider, Minjung Son, Angela Lee, Prachi Gupta, Andrés Montoya-Castillo, Tim J. Zuehlsdorff, Gabriela S. Schlau-Cohen, Christine M. Isborn, Thomas E. Markland

{"title":"Two-Dimensional Electronic Spectroscopy in the Condensed Phase Using Equivariant Transformer Accelerated Molecular Dynamics Simulations","authors":"Joseph Kelly, Frank Hu, Arianna Damiani, Michael S. Chen, Andrew Snider, Minjung Son, Angela Lee, Prachi Gupta, Andrés Montoya-Castillo, Tim J. Zuehlsdorff, Gabriela S. Schlau-Cohen, Christine M. Isborn, Thomas E. Markland","doi":"10.1021/acs.jpclett.5c00911","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00911","url":null,"abstract":"Two-dimensional electronic spectroscopy (2DES) provides rich information about how the electronic states of molecules, proteins, and solid-state materials interact with each other and their surrounding environment. Atomistic molecular dynamics simulations offer an appealing route to uncover how nuclear motions mediate electronic energy relaxation and their manifestation in electronic spectroscopies but are computationally expensive. Here we show that by using an equivariant transformer-based machine learning architecture trained with only 2500 ground state and 100 excited state electronic structure calculations, one can construct accurate machine-learned potential energy surfaces for both the ground-state electronic surface and excited-state energy gap. We demonstrate the utility of this approach for simulating the dynamics of Nile blue in ethanol, where we experimentally validate and decompose the simulated 2DES to establish the nuclear motions of the chromophore and the solvent that couple to the excited state, connecting the spectroscopic signals to their molecular origin.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"176 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153500","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

Modulating the Structural Dynamics and Catalytic Properties of a Cu Cluster via CO-Mediated Spatial Confinement. 通过co介导的空间约束调节Cu簇的结构动力学和催化性能。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-28 DOI: 10.1021/acs.jpclett.5c00949

Yurui Han, Feiyang Ren, Qiang Fu, Jinlong Yang

{"title":"Modulating the Structural Dynamics and Catalytic Properties of a Cu Cluster via CO-Mediated Spatial Confinement.","authors":"Yurui Han, Feiyang Ren, Qiang Fu, Jinlong Yang","doi":"10.1021/acs.jpclett.5c00949","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00949","url":null,"abstract":"Spatial confinement provides a powerful approach to tune the catalytic properties of metal clusters by creating unique nanoscale environments around them. However, the dynamic structural evolution of the confined clusters covered by high-coverage adsorbates and the consequent impact on the catalytic properties remain poorly understood. In this work, using density functional theory calculations and ab initio molecular dynamics simulations, we demonstrate that the CO molecules adsorbed on an encapsulated Cu18 cluster can mediate interactions between the (17, 0) zigzag carbon nanotube (CNT) inner wall and Cu18, which significantly regulates the structural dynamics and reactivity of the confined cluster. It is found that the Cu cluster in the CNT exhibits reduced Cu-Cu coordination numbers and recurrent multiadsorption structures of CO, both of which are absent in the corresponding cluster on the open space of graphene. The unique structural features of the encapsulated Cu cluster in the CNT can further promote a C-C coupling reaction. Our work provides a new adsorbate-assisted approach to tune the structural dynamics of confined clusters and may open up new opportunities to improve the performance of confined catalysts.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5553-5560"},"PeriodicalIF":4.8,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144155281","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

Electrocatalytic Nitrogen Reduction to Ammonia Using TiO2-Supported Cu4Cl4(PPh3)4 and Ag4Cl4(PPh3)4 Nanoclusters 二氧化钛负载Cu4Cl4(PPh3)4和Ag4Cl4(PPh3)4纳米团簇电催化氮还原制氨研究

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-27 DOI: 10.1021/acs.jpclett.5c00866

Aamir Shehzad, Lijun Geng, Zhixun Luo

{"title":"Electrocatalytic Nitrogen Reduction to Ammonia Using TiO2-Supported Cu4Cl4(PPh3)4 and Ag4Cl4(PPh3)4 Nanoclusters","authors":"Aamir Shehzad, Lijun Geng, Zhixun Luo","doi":"10.1021/acs.jpclett.5c00866","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00866","url":null,"abstract":"The electrocatalytic nitrogen reduction reaction (ENRR) offers a sustainable and promising approach for synthesizing ammonia under ambient conditions, providing an alternative to conventional industrial processes. However, challenges such as the inherent inertness of N2 and the competing hydrogen evolution reaction (HER) in aqueous electrolytes hinder ammonia yield and Faradaic efficiencies. This research use TiO2-supported Cu4Cl4(PPh3)4 and Ag4Cl4(PPh3)4 nanoclusters (NCs) with quasi-cubic M4Cl4 cores (M = Ag or Cu) for ENRR investigations. The results reveal that TiO2-supported Cu4Cl4(PPh3)4 NCs achieved an ammonia yield of 4.25 μg·h–1·cm–2 with a Faradaic efficiency (FE) of 53.0% at −0.9 V vs RHE. In contrast, TiO2-supported Ag4Cl4(PPh3)4 NCs produced a yield of 3.60 μg·h–1·cm–2 and an FE of 51.39% at −0.8 V vs RHE. Both NCs on the TiO2 support demonstrated superior performance compared to their unsupported counterparts, underscoring the critical role of TiO2 in improving electron transfer and fostering synergistic effects, thereby boosting catalytic activity. This research offers important insights into the design of supported NCs as high-performance catalysts, advancing the development of environmentally sustainable and energy-efficient approaches for ammonia production.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"1 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153504","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

Thermal Tuning of Brønsted Acidic Phosphorated Carbon Catalyst Coupled with Deep Eutectic Solvent Fractionation Boosts Heterogeneous Catalysis of Biomass toward Levoglucosenone Brønsted酸性磷酸碳催化剂的热调谐耦合深度共晶溶剂分馏促进生物质对左旋葡萄糖酮的非均相催化

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-27 DOI: 10.1021/acs.jpclett.5c00874

Mian Xu, Xianqing Zhu, Chaoran Duan, Xintong Xiao, Zhongyue Zhou, Qingang Xiong, Ao Xia, Yun Huang, Xun Zhu, Qiang Liao

{"title":"Thermal Tuning of Brønsted Acidic Phosphorated Carbon Catalyst Coupled with Deep Eutectic Solvent Fractionation Boosts Heterogeneous Catalysis of Biomass toward Levoglucosenone","authors":"Mian Xu, Xianqing Zhu, Chaoran Duan, Xintong Xiao, Zhongyue Zhou, Qingang Xiong, Ao Xia, Yun Huang, Xun Zhu, Qiang Liao","doi":"10.1021/acs.jpclett.5c00874","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00874","url":null,"abstract":"This work proposed a controllable thermal tuning strategy for Brønsted acid sites in phosphorated carbon catalysts combined with deep eutectic solvent fractionation to stimulate levoglucosenone generation from biomacromolecules. The phosphorus immobilization into the carbonaceous substrate was enhanced via motivating the bonding between phosphorus and oxygen at elevated temperatures, yielding a high concentration of P–O groups (41.93%). Therefore, the catalysts’ proton-donating ability was promoted for intensified Brønsted acidity, and the generation of intermediates in sequential reactions was accelerated as confirmed by online experiments, which finally converted into levoglucosenone with a high yield of 10.31 wt %. Monte Carlo simulations proved that the immobilized C–P(O)(OH)2 exhibited the best adsorption ability for levoglucosenone precursor, whose hydroxyls were reactive sites for strong chemical adsorption with a high ΔEad of −160.45 kJ mol–1 as calculated by DFT. These findings provided an effective approach to selectively producing valuable anhydrosugars and disclosed the atomic-level catalytic mechanism.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"19 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144153505","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

Photoelectron Spectroscopy and Ion Chemistry of Benzoxazolide 苯并恶唑烷的光电子能谱与离子化学

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-27 DOI: 10.1021/acs.jpclett.5c01067

Sydney Cordova, Beverly Feng, Connor Fang, Andrei Sanov

引用次数: 0

Interaction of Metal Ion Stabilized Oligomeric Dipeptide with Lipid Membrane: Concurrent Observations of Supported Lipid Membrane, Wetting, and Uptake 金属离子稳定低聚二肽与脂膜的相互作用：支持脂膜、润湿和摄取的同步观察

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-05-27 DOI: 10.1021/acs.jpclett.5c01228

Priyanka Nath, Debanjan Bagchi, Avijit Maity, Huma Tabassum, Suman Choudhury, Naveen Kumar, Anjan Chakraborty

引用次数: 0