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

Alternative Photoreduction Pathway Involving Electron Tunneling and Proton Transfer in a Bifunctional Cryptochrome. 双功能隐花色素中涉及电子隧穿和质子转移的替代光还原途径。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-20 DOI: 10.1021/acs.jpclett.5c01003

Shuhua Zou,Xiu-Wen Kang,Yao Lu,Zijing Chen,Zhongneng Zhou,Siwei Tang,Dongping Zhong,Bei Ding

引用次数: 0

A Machine-Learning-Based Investigation on the Formation and Evolution of Silicic Acid Oligomers Structurally Analogous to Zeolite Building Units. 基于机器学习的结构类似沸石构建单元的硅酸低聚物的形成和演化研究。

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.5c01376

Xin Liu, Yongbo Zhao, Huimin Guo, Changgong Meng

引用次数: 0

Nonradiative Recombination of Excitons in Periodic Solids: A Case Study of Dion-Jacobson Lead-Halide Perovskite. 周期性固体中激子的非辐射复合：以Dion-Jacobson铅卤化钙钛矿为例。

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.5c01174

Aaron Forde, Carlos MoraPerez, Nikhil Singh, Dibyajyoti Ghosh, Amanda J Neukirch, Sergei Tretiak

{"title":"Nonradiative Recombination of Excitons in Periodic Solids: A Case Study of Dion-Jacobson Lead-Halide Perovskite.","authors":"Aaron Forde, Carlos MoraPerez, Nikhil Singh, Dibyajyoti Ghosh, Amanda J Neukirch, Sergei Tretiak","doi":"10.1021/acs.jpclett.5c01174","DOIUrl":"10.1021/acs.jpclett.5c01174","url":null,"abstract":"Nonadiabatic dynamics describe the nonradiative relaxation of excited states in semiconducting materials which determine the efficiency of optoelectronic devices. Due to the computational complexity of modeling the coupled electronic-nuclear dynamics approximations are required. In the solid state a common approximation is the independent orbital approximation (IOA) as the electronic basis for surface-hopping trajectories describing nuclear dynamics. We examine the impact of the IOA on the computed nonradiative lifetimes in nanostructured Dion-Jacobson lead-halide perovskite. Specifically, we compute the nonadiabatic couplings between the excited states and the ground state using either IOA or many-body states to propagate the surface-hopping trajectories. Many-body corrections renormalize the nonadiabatic couplings compared to the IOA resulting in a 50% increase in the time-averaged coupling strength. However, when including decoherence corrections the differences in the computed recombination lifetimes reduce significantly. This result suggests that the IOA serves as an efficient approximation for prediction of nonradiative lifetimes in strongly confined nanomaterials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"5929-5937"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144232637","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

Decoding Chiral Interactions: Molecular Insights into the Selective Binding of Nanoparticles at Biological Interfaces. 解码手性相互作用：纳米颗粒在生物界面上选择性结合的分子见解。

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.5c01194

Jing Liu, Chaofan Deng, Lin Yang, Hongxia Ma, Changcheng Gao, Shixin Li, Jian Zhao, Tongtao Yue

{"title":"Decoding Chiral Interactions: Molecular Insights into the Selective Binding of Nanoparticles at Biological Interfaces.","authors":"Jing Liu, Chaofan Deng, Lin Yang, Hongxia Ma, Changcheng Gao, Shixin Li, Jian Zhao, Tongtao Yue","doi":"10.1021/acs.jpclett.5c01194","DOIUrl":"10.1021/acs.jpclett.5c01194","url":null,"abstract":"Chirality is a pivotal attribute of nanoparticles, crucial for biomedical applications. Despite evidence of chiral preferences in biological responses, the molecular origin of chiral selectivity remains unclear. Here, we designed gold nanoparticles (GNPs) with opposite chirality (l/d-GNPs) to unravel chiral selectivity in cell membrane attachment and protein adsorption. All-atom molecular dynamics simulations revealed that l-GNPs preferentially attach to lipid bilayers. This selectivity arises from stereomatching between chiral molecules on GNPs and lipid headgroups, leading to distinct lipid conformations and binding affinity. Anionic lipids show higher chiral preference than zwitterionic lipids due to enhanced electrostatic interactions. Chiral selectivity is diminished for lipids with primary charged groups exposed at the outermost position, as the lowest interaction energy is insensitive to stereomatching. For proteins with diverse residues, stereomatching and other interactions collectively determine chiral preference based on binding modes. Our findings provide molecular insights into chiral selectivity at nano-bio interfaces, advancing chiral nanomedicine.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"6040-6051"},"PeriodicalIF":4.8,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256810","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

Extracting Coupling-Mode Spectral Densities with Two-Dimensional Electronic Spectroscopy 二维电子能谱法提取耦合模谱密度

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 DOI: 10.1021/acs.jpclett.5c00928

Roosmarijn de Wit, Jonathan Keeling, Brendon W. Lovett, Alex W. Chin

引用次数: 0

Relatively Bright Intraband 5 μm Photoluminescence from HgSe/CdS Quantum Dot Films after Lead Halide Treatment. 卤化铅处理后的HgSe/CdS量子点薄膜带内相对明亮的5 μm光致发光。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-06-19 Epub Date: 2025-06-06 DOI: 10.1021/acs.jpclett.5c01021

Rounak Naphade, Augustin Caillas, Philippe Guyot Sionnest

引用次数: 0

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