The Journal of Physical Chemistry Letters最新文献_第3页

Sulfur Passivation Engineering of Carbon Defects in N-Surface GaN: Suppressing Nonadiabatic Carrier Recombination Via Self-Compensated S_N-C_N Complexes. 氮表面氮化镓中碳缺陷的硫钝化工程：通过自补偿的SN-CN配合物抑制非绝热载流子重组。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-05 DOI: 10.1021/acs.jpclett.5c01144

Fang-Jing Kang, Shuai-Shuai Liu, Jian-Jie Kang, Ze Peng, Shao-Qiang Guo, Juan Lyu, Hai-Shan Zhang, Jian Gong

{"title":"Sulfur Passivation Engineering of Carbon Defects in N-Surface GaN: Suppressing Nonadiabatic Carrier Recombination Via Self-Compensated SN-CN Complexes.","authors":"Fang-Jing Kang, Shuai-Shuai Liu, Jian-Jie Kang, Ze Peng, Shao-Qiang Guo, Juan Lyu, Hai-Shan Zhang, Jian Gong","doi":"10.1021/acs.jpclett.5c01144","DOIUrl":"10.1021/acs.jpclett.5c01144","url":null,"abstract":"In gallium nitride (GaN), the carbon-on-nitrogen substitutional defect (CN) has been extensively investigated as a prototypical deep acceptor center, particularly for its well-characterized yellow luminescence associated with the (-/0) transition. However, the carrier dynamics involving its secondary (0/+) transition remains poorly understood. Combining first-principles calculations and nonadiabatic molecular dynamics simulations, we systematically investigate the nonradiative carrier capture processes mediated by the CN defects on nitrogen-terminated GaN surfaces, along with their sulfur-based passivation mechanisms. Our results demonstrate that the neutral CN defect serves as a critical nonradiative recombination center, exhibiting an ultrafast hole capture rate (τ ≈ 10-12 s). Notably, sulfur atoms can migrate with a low energy barrier (0.64 eV) to occupy adjacent nitrogen vacancies on the N surface, forming SN-CN complex defects through a self-compensation mechanism. This structural modification induces a significant charge redistribution, shifting the defect level from deep within the bandgap to near the valence band maximum. Such electronic structure modulation effectively suppresses nonadiabatic transitions between defect states and the valence band. This work provides the first atomistic visualization of sulfur passivation mechanisms for CN defects in GaN, establishing a quantitative relationship between defect configuration engineering and carrier recombination dynamics.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5938-5945"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232640","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

Warp-Driven Dual-Side Adsorption for Superior Surface-Enhanced Raman Scattering Performance of Transition Metal Dichalcogenides Nanosheets. 翘曲驱动的双面吸附对过渡金属二硫族化合物纳米片表面增强拉曼散射性能的影响。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-12 DOI: 10.1021/acs.jpclett.5c01197

Tong Xiang, Qiao Wang, Biwen He, Jibo Zhang, Xixi Huang, Wei Chen, Siwei Luo, Xiang Qi

{"title":"Warp-Driven Dual-Side Adsorption for Superior Surface-Enhanced Raman Scattering Performance of Transition Metal Dichalcogenides Nanosheets.","authors":"Tong Xiang, Qiao Wang, Biwen He, Jibo Zhang, Xixi Huang, Wei Chen, Siwei Luo, Xiang Qi","doi":"10.1021/acs.jpclett.5c01197","DOIUrl":"10.1021/acs.jpclett.5c01197","url":null,"abstract":"Surface-enhanced Raman scattering (SERS) technology is highly sensitive but limited by the high cost of noble-metal substrates and the low enhancement of two-dimensional (2D) materials. This work proposes a dual-sided adsorption strategy utilizing warped structures at the cracks and edges of WSe2 and MoSe2 nanosheets grown by Chemical Vapor Deposition (CVD). Driven by capillary forces, probe molecules infiltrate the nanosheet-substrate interface, enabling dual-sided adsorption on both the upper and lower surfaces. This approach enhances SERS signals by up to 20-fold, with a detection limit of 10-10 M, surpassing most reported traditional single-sided adsorption modes. Additionally, it improves stability by isolating the probe molecules from oxygen. This study further enhanced the formation efficiency and coverage area of the dual-sided adsorption mode by leveraging wide warped structures. It offers new perspectives on the application of crack defects and the potential for the development of high-performance and highly stable SERS substrates.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6212-6218"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144273729","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

Separating Orders of Response in Transient Absorption and Coherent Multidimensional Spectroscopy by Intensity Variation. 利用强度变化分离瞬态吸收和相干多维光谱的响应阶数。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-05 DOI: 10.1021/acs.jpclett.5c01177

Jacob J Krich, Luisa Brenneis, Peter A Rose, Katja Mayershofer, Simon Büttner, Julian Lüttig, Pavel Malý, Tobias Brixner

引用次数: 0

Cation Effects on CO₂ Delivery to Cu Electrode in Reactive Capture of CO₂. 活性捕集CO2中阳离子对Cu电极上CO2传递的影响。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-09 DOI: 10.1021/acs.jpclett.5c01022

Shawn Chiu, Anastassia N Alexandrova

{"title":"Cation Effects on CO2 Delivery to Cu Electrode in Reactive Capture of CO2.","authors":"Shawn Chiu, Anastassia N Alexandrova","doi":"10.1021/acs.jpclett.5c01022","DOIUrl":"10.1021/acs.jpclett.5c01022","url":null,"abstract":"The direct electrochemical conversion of captured CO2, known as reactive capture of CO2 (RCC), remains a formidable challenge in heterogeneous catalysis. Given that amines are one of the most widely used capture agents for CO2, it would be desirable to electrochemically reduce the resultant adducts, such as carbamate, directly in RCC. However, current understanding suggests that the primary species undergoing reduction in RCC with amines is the CO2 dissociated from the sorbent. Herein, we employ ab initio molecular dynamics (AIMD) with DFT to analyze how the nature of alkali metal cations in the electrolyte affects carbamate at the Cu surface, thereby assessing the possibility of promoting RCC by cation effects. The simulations show that the carbamate's orientation with respect to the electrode is governed by the optimal distance between the carbamate and the cation, specifically how this distance aligns with the cation's hydration spheres. Moreover, the slow-growth AIMD results indicate that the CO2 dissociation barrier correlates with the orientation of carbamate at the interface. When the carbamate resides beyond the cation's first hydration sphere, it adopts a flat orientation with respect to the surface that promotes the release of CO2 from the capture agent. In contrast, when the carbamate disrupts the first hydration sphere and exhibits a strong cation-π interaction, it adopts an upright orientation that is less conducive to CO2 release. These findings reveal a nontrivial cation effect in RCC, suggesting that it should be possible to optimize RCC via the choice of the electrolyte.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6032-6039"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256808","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

Direct Observation of Orbital Hybridization Evolution in BAs. BAs轨道杂化演化的直接观察。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-09 DOI: 10.1021/acs.jpclett.5c01040

Jingwei Dong, Yingxin Zhang, Yunbo Wu, Zhe Sun, Zhongwei Chen

引用次数: 0

Synergistic Structural-Compositional Modification of V2O5/C Films for Enhanced Multicolor Electrochromic Devices. 增强型多色电致变色器件用V2O5/C薄膜的结构-成分协同改性。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 DOI: 10.1021/acs.jpclett.5c01233

Xiaodan Guo,Qing Sui,Ying Lv,Hang Zhou,Sensen Jia,Chunjing Li,Jinhui Wang,Guofa Cai

{"title":"Synergistic Structural-Compositional Modification of V2O5/C Films for Enhanced Multicolor Electrochromic Devices.","authors":"Xiaodan Guo,Qing Sui,Ying Lv,Hang Zhou,Sensen Jia,Chunjing Li,Jinhui Wang,Guofa Cai","doi":"10.1021/acs.jpclett.5c01233","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01233","url":null,"abstract":"The color variations of electrochromic materials originate from the redox reaction triggered by the coinjection of electrons and ions under an applied electric field. Hence, the performance of electrochromic materials is highly dependent on the ion-electron transport process. However, the simultaneous realization of efficient ion and electron transport remains challenging. Herein, a porous V2O5/C electrochromic film with improved ion/electron transport rates was constructed through a dual structure-composition synergistic strategy. The porous structure of the film was optimized by a facile and economic plasma treatment technology due to the easily etched organic components introduced in the precursor. An optimized small-size pore structure results in outstanding electrolyte affinity and shorter ion transport paths. Furthermore, the residual carbon during the annealing process enhances the conductivity of the material, promoting electron transport. Benefiting from the optimized structure and composition, the plasma-treated V2O5/C film realizes superior ion and electron transport during electrochromic redox reactions. Therefore, the electrochromic performance of the film is significantly improved (18.4% faster switching and 51.9% greater optical modulation than unplasma-treated films), showing promising applications in smart windows and information displays. Such a simple and economical strategy for simultaneously enhancing ion/electron transport kinetics would offer a distinctive pathway for other metal oxide-based electrochemical materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"36 1","pages":"6585-6593"},"PeriodicalIF":6.475,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144328783","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

Chiral Orbital Modifying Dipolar Polarization and Recombination in Chiral Perovskites. 手性钙钛矿的手性轨道修饰偶极极化和复合。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-05 DOI: 10.1021/acs.jpclett.5c01227

Yuan Yu, Xiangping Zhao, Chenghao Liu, Zhiyong Pang, Wei Qin

{"title":"Chiral Orbital Modifying Dipolar Polarization and Recombination in Chiral Perovskites.","authors":"Yuan Yu, Xiangping Zhao, Chenghao Liu, Zhiyong Pang, Wei Qin","doi":"10.1021/acs.jpclett.5c01227","DOIUrl":"10.1021/acs.jpclett.5c01227","url":null,"abstract":"The chiral spatial structure of chiral perovskite materials enriches the physical and optical properties of perovskite materials, making them an excellent platform to deeply understand charge-spin-photon interactions. In this work, we fabricated chiral perovskite crystals and their nonchiral isomeric counterparts. The significant differences in the crystal structures of these two types of materials lead to notable variations in their fluorescence lifetimes and electron-phonon coupling strength, which present an externally presentable change in physical properties, such as the dielectric constant. Moreover, inside chiral structures, the chiral orbit should be taken into account. Under the effect of a magnetic field versus a chiral orbit, dipolar polarization and charge recombination will be rebalanced after disruption, where the dielectric constants and photoluminescence intensities of the S- and R-type chiral perovskites display opposite trends. It is also noted that chiral orbit-induced spin relaxation determined the spin dependence of recombination, which presents a potential materials platform to fabricate devices resisting external signal interference well.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5912-5917"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232635","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

Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities. 非线性光学晶体双折射及不同双折射活性多晶的机器学习预测。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-09 DOI: 10.1021/acs.jpclett.5c00980

Ding Peng, Zhaoxi Yu, Sangen Zhao, Junhua Luo, Lin Shen, Wei-Hai Fang

{"title":"Machine Learning Prediction on Birefringence of Nonlinear Optical Crystals and Polymorphs with Different Birefringence Activities.","authors":"Ding Peng, Zhaoxi Yu, Sangen Zhao, Junhua Luo, Lin Shen, Wei-Hai Fang","doi":"10.1021/acs.jpclett.5c00980","DOIUrl":"10.1021/acs.jpclett.5c00980","url":null,"abstract":"Nonlinear optical (NLO) crystal materials have been widely used in the scientific and industrial fields. Birefringence is an important property of the NLO crystals. Tuning appropriate birefringence through element substitution or polymorphic transformation may promote phase-matching performance facing various demands of laser wavelength. A growing number of studies based on machine learning (ML), such as the multilevel descriptors developed in our group (Zhang et al. J. Phys. Chem. C 2021, 125, 25175-25188), can successfully predict birefringence of NLO materials. However, how to identify polymorphs with different birefringence activities is still a nascent research topic. In this work, we proposed hp-wACSFs, a new descriptor based on the widely used atom-centered symmetric function, to predict the birefringence of inorganic crystals. A series of ML classifiers were built using hp-wACSFs. Two learning tasks, which aim at birefringence-active NLO crystals or polymorphs with different birefringence activities, were implemented. The performance on the former task was as good as our previously reported work, while the best accuracy on the latter task, which cannot be processed in the absence of three-dimensional descriptors, achieved 0.8 in this work. We finally implemented virtual screening using constructed ML models to search polymorphs with different birefringence activities.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6087-6097"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256774","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

Probing Electrocatalytic Gas Evolution Reaction at Pt by Force Noise Measurements. Part 1. Hydrogen. 用力噪声测量法探测铂电催化释气反应。第1部分。氢。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-09 DOI: 10.1021/acs.jpclett.5c00053

Nataraju Bodappa, Zixiao Zhang, Ramin Yazdaanpanah, Wyatt Behn, Kirk H Bevan, Gregory Jerkiewicz, Peter Grutter

{"title":"Probing Electrocatalytic Gas Evolution Reaction at Pt by Force Noise Measurements. Part 1. Hydrogen.","authors":"Nataraju Bodappa, Zixiao Zhang, Ramin Yazdaanpanah, Wyatt Behn, Kirk H Bevan, Gregory Jerkiewicz, Peter Grutter","doi":"10.1021/acs.jpclett.5c00053","DOIUrl":"10.1021/acs.jpclett.5c00053","url":null,"abstract":"Electrocatalytic processes occurring at a heterogeneous interface are complex, and their understanding at the molecular level remains challenging. Atomic force microscopy (AFM) can detect force interactions down to the atomic level, but so far it has been mainly used to obtain in situ images of electrocatalysts. Here, for the first time, we employ AFM to investigate gas evolution at a platinum ultramicroelectrode (Pt UME) under electrochemical conditions using force noise measurements. We detect excess force noise when individual H2 gas bubble nucleation, growth, and detachment events occur at the Pt UME. Based on our in situ AFM, electrochemical, and optical microscopy analyses, we conclude that larger size H2 gas bubbles remain pinned to the UME surface while smaller H2 gas bubbles are released until an overpotential of -0.8 V vs RHE. This study demonstrates the viability of in situ AFM in studying gas evolution under electrocatalytic conditions and contributes to a mechanistic understanding of the H2 gas bubble detachments during the hydrogen evolution reaction (HER).","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6015-6022"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256776","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

Solution-Based Laser-Induced Silver Nanowire Growth on Substrates through Photothermal and Chemical Comodulation. 通过光热和化学调节在衬底上基于溶液的激光诱导银纳米线生长。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-09 DOI: 10.1021/acs.jpclett.5c01309

Wenhui Li, Yongsen He, Shuang Yang, Wenyuan Yu, Siyu Liu

{"title":"Solution-Based Laser-Induced Silver Nanowire Growth on Substrates through Photothermal and Chemical Comodulation.","authors":"Wenhui Li, Yongsen He, Shuang Yang, Wenyuan Yu, Siyu Liu","doi":"10.1021/acs.jpclett.5c01309","DOIUrl":"10.1021/acs.jpclett.5c01309","url":null,"abstract":"Solution-based laser-induced synthesis (LIS) is a promising nanomanufacturing technique for the localized fabrication of nanomaterials. However, achieving controlled growth of silver nanowires (Ag NWs) remains challenging due to the complex mechanisms of photothermal and chemical dynamics. This study demonstrates direct synthesis of crystalline Ag NWs on various substrates, including flexible ones, through the comodulation of laser parameters and chemical factors. Heat and mass transfer analysis revealed that repetition rate and fluence of the pulsed laser play key roles in modulating temperature distribution and fluid convection, influencing nucleation and crystal growth. Under appropriate power density and chemical conditions, high fluence, inducing high peak temperature, favors the formation of smaller particles with higher number densities, while higher repetition rates generally enhance mass transport, promoting anisotropic growth of Ag nanocrystals. These findings deepen the understanding of photothermal mechanisms governing LIS and highlight its potential for electrode integration in flexible and next-generation electronic devices.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6098-6105"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256778","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