The Journal of Physical Chemistry Letters最新文献_第6页

Wave Function Localization Reduces the Bandgap of Disordered Double Perovskite Cs₂AgBiBr₆. 波函数局部化降低了无序双包晶石 Cs2AgBiBr6 的带隙。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-04 DOI: 10.1021/acs.jpclett.4c02946

Dongyu Liu, Bayan Amer Abzakh, Elena A Kazakova, Dmitrii A Abrameshin, Pavel A Troshin, Run Long, Andrey S Vasenko

{"title":"Wave Function Localization Reduces the Bandgap of Disordered Double Perovskite Cs2AgBiBr6.","authors":"Dongyu Liu, Bayan Amer Abzakh, Elena A Kazakova, Dmitrii A Abrameshin, Pavel A Troshin, Run Long, Andrey S Vasenko","doi":"10.1021/acs.jpclett.4c02946","DOIUrl":"10.1021/acs.jpclett.4c02946","url":null,"abstract":"Double perovskite Cs2AgBiBr6 is a promising alternative to lead-based perovskites with excellent stability and attractive optoelectronic properties. However, a relatively large bandgap severely limits its performance in many applications such as solar cells and photodetectors. It has been reported that a random distribution of Ag and Bi atoms in Cs2AgBiBr6 effectively reduces its bandgap without introducing dopants or impurities, while the mechanism remains unclear. Here, using density functional theory calculations, we demonstrate that the Ag-Bi disorder in Cs2AgBiBr6 generates localized electronic states as band edges to regulate the bandgap. The disordered structures segregate Ag and Bi atoms in the lattice, and the formed homoatomic clusters lead to wave function localization. Moreover, the bandgap decrease exhibits a non-monotonic dependence on the degree of disorder. Our results are comparable with experimental observations and provide crucial insights into understanding the order-disorder transition in double perovskites.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11268-11274"},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566370","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

Luminescence and Transport Behavior in Incommensurately Modulated CaGd₂(MoO₄)₄:Yb/Er. 不可比调制 CaGd2(MoO4)4:Yb/Er.中的发光和传输行为

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-06 DOI: 10.1021/acs.jpclett.4c02554

Yinghan Wang, Zeyue Zhang, Guohong Cai, Jingxie Xiong, Zhengren Tao, Chunhai Wang, Junliang Sun, Shi Ye

{"title":"Luminescence and Transport Behavior in Incommensurately Modulated CaGd2(MoO4)4:Yb/Er.","authors":"Yinghan Wang, Zeyue Zhang, Guohong Cai, Jingxie Xiong, Zhengren Tao, Chunhai Wang, Junliang Sun, Shi Ye","doi":"10.1021/acs.jpclett.4c02554","DOIUrl":"10.1021/acs.jpclett.4c02554","url":null,"abstract":"The phenomenon of thermal quenching of luminescence can significantly compromise the efficiency of luminescent materials, a process accompanied by the generation of substantial phonon populations. While plenty of models for elucidating this behavior have been proposed, the crucial role of phonon transport has largely been neglected, particularly in the enigmatic incommensurate scheelite structure with good luminescence performance. In this study, we delve into the thermal quenching dynamics of the near-infrared emission in the incommensurately modulated CaGd2(MoO4)4:Yb/Er system. Our comprehensive investigation reveals distinct evolutionary patterns in electrical conductivity, luminescence intensity, thermal conductivity, and Raman scattering at varying temperature regimes. Notably, we have determined that thermally induced ion migration, occurring above ∼300 °C, serves as a pivotal trigger for the activation of all phonons and the enhancement of phonon-defect scattering within this incommensurate framework. This phenomenon not only diminishes the thermal conductivity but also accelerates the multiphonon relaxation of the Er3+ emission levels, culminating in a marked thermal quenching of luminescence. This work illuminates the thermal quenching mechanism of luminescence by focusing on phonon scattering dynamics, providing critical insights for the design of thermally robust near-infrared luminescent materials, which are essential for the advancement of optical amplification systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":" ","pages":"11374-11382"},"PeriodicalIF":4.8,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581022","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

Explicit Configurational Entropy of Mixing in Molecular Dynamics Simulations. 分子动力学模拟中混合的显式构型熵。

IF 4.8 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-14 Epub Date: 2024-11-05 DOI: 10.1021/acs.jpclett.4c02819

T Hanke, A L Upterworth, D Sebastiani

引用次数: 0

Multiband Spectrum Method for Quantifying the Ionic Contribution of Volume Strategy and Filler Strategy: Enhancing the Ionic Transport Channels for Polymeric Solid-State Batteries 量化体积策略和填充策略的离子贡献的多频谱方法：增强聚合物固态电池的离子传输通道

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-13 DOI: 10.1021/acs.jpclett.4c02525

Shanyan Huang, Kai-Lun Zhang, Na Li, Wei-Li Song, Yan-li Zhu, Shuqiang Jiao

{"title":"Multiband Spectrum Method for Quantifying the Ionic Contribution of Volume Strategy and Filler Strategy: Enhancing the Ionic Transport Channels for Polymeric Solid-State Batteries","authors":"Shanyan Huang, Kai-Lun Zhang, Na Li, Wei-Li Song, Yan-li Zhu, Shuqiang Jiao","doi":"10.1021/acs.jpclett.4c02525","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02525","url":null,"abstract":"As a promising solution for solid-state batteries with high energy density and safety, understanding the mechanism of fast ion conduction in polymer-ceramic composite solid-state electrolytes (CSEs) is still a challenging task. Herein, we understand the enhanced ion conduction in CSEs using a series of ionic spectra. Ionic insight is extended to ion conduction in CSEs, resolving the mechanism of fast ion migration. With the cooperation of enhanced interface and filler ion conduction, the CSE with a conductive filler exhibits ionic conductivity higher than that of CSEs with insulating fillers. Volume and filler strategies of CSE design are proposed based on volcanic maps of conductivity. An equivalent circuit is established to describe the conduction mechanism of CSEs. Specifically, Rinterface and Rfiller are in parallel to describe the cooperation of interface and filler conduction. They are in series with Rbulk, which represents a competition between the fundamental matrix and enhanced interface conduction. The proposed conduction model is verified though the energy storage performance of solid-state batteries; a fast dynamic process promises a better rate performance and cycling stability of solid-state batteries. These results provide deep insights into fast ion conduction in ceramic-polymer CSEs, which are indispensable to develop high-performance solid-state batteries.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"119 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601479","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

Intrinsic Rashba Effect in Stable Configurations of Two-Dimensional (PEA)2PbI4 二维 (PEA)2PbI4 稳定构型的内在拉什巴效应

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-13 DOI: 10.1021/acs.jpclett.4c02222

Shahar Zuri, Leeor Kronik, Efrat Lifshitz

{"title":"Intrinsic Rashba Effect in Stable Configurations of Two-Dimensional (PEA)2PbI4","authors":"Shahar Zuri, Leeor Kronik, Efrat Lifshitz","doi":"10.1021/acs.jpclett.4c02222","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02222","url":null,"abstract":"Halide perovskites (HPs) are crystalline solids that feature a unique softness, absent in conventional semiconducting materials. In recent years, this softness has been pivotal to many properties in these materials, in both static and dynamic regimes. Here, we focus on the two-dimensional (2D) (PEA)2PbI4 crystal. We employ extensive density functional theory calculations and structural analysis to uncover a rich mosaic of ground-state configurations, identifying several stable configurations with distinct electronic properties. Our study uncovers an intrinsic Rashba effect within a structure traditionally considered as globally centrosymmetric, presenting a challenge to conventional understanding in the field. The observed effect emerges from a local symmetry-breaking induced by specific spatial orientations of the organic PEA molecules. This intrinsic Rashba effect, observed in select configurations, underscores the nuanced symmetrical complexities of 2D HPs and highlights their potential for spin-related applications. Additionally, our investigation demonstrates the exceptional flexibility of 2D HPs, as evidenced by an observed significant tolerance toward single-molecule rotations. This flexibility suggests potential pathways for smoother transitions between different molecular domains within these materials. Overall, our findings emphasize the intricate interplay between the organic/inorganic counterparts and the electronic properties in 2D HPs, paving the way for further exploration and exploitation of their unique characteristics in various optoelectronic and spintronic applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"28 12 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609805","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

Manipulating the H2O2 Reactivity on Pristine Anatase TiO2 with Various Surface Features and Implications in Oxidation Reactions 操纵具有各种表面特征的原始无相钛白氧化物上的 H2O2 反应活性及其在氧化反应中的影响

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-12 DOI: 10.1021/acs.jpclett.4c02742

Guohan Sun, Quan Wang, Yin-Song Liao, Yifan Cui, Linyuan Tian, Jyh-Pin Chou, Yufei Zhao, Yung-Kang Peng

{"title":"Manipulating the H2O2 Reactivity on Pristine Anatase TiO2 with Various Surface Features and Implications in Oxidation Reactions","authors":"Guohan Sun, Quan Wang, Yin-Song Liao, Yifan Cui, Linyuan Tian, Jyh-Pin Chou, Yufei Zhao, Yung-Kang Peng","doi":"10.1021/acs.jpclett.4c02742","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02742","url":null,"abstract":"Anatase TiO2 is commonly used as a catalyst/support in reactions involving H2O2, yet the understanding of interactions between common TiO2 surfaces and H2O2 remains limited. Herein, we synthesized well-defined TiO2 crystallites with (101), (001), and fluorine-modified (001) [F-(001)] surfaces to examine how surface features, including the arrangement of five-coordinated Ti (Ti5c) sites and the presence of fluorine, influence H2O2 activation. Our findings reveal that these surface features significantly affect the physiochemical properties of adsorbed H2O2. Specifically, fluorine on the F-(001) surface introduces an additional hydrogen bond to the Ti5c-peroxo species, altering the electronic structure of H2O2 compared to those with the (101) and (001) surfaces. Using cyclohexene as a probe substrate, we successfully distinguished the reactivities of the Ti5c-peroxo species. The activity of those on the F-(001) surface was significantly higher than the activity of those on the (001) surface, while the (101) surface showed negligible oxidation activity. These insights can guide the design of TiO2-based catalysts for H2O2-related reactions.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"20 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601477","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

Structural, Solvent, and Temperature Effects on Protein Junction Conductance 结构、溶剂和温度对蛋白质连接传导的影响

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-12 DOI: 10.1021/acs.jpclett.4c02230

Gowtham Nirmal Jonnalagadda, Xiaojing Wu, Lukáš Hronek, Zdenek Futera

{"title":"Structural, Solvent, and Temperature Effects on Protein Junction Conductance","authors":"Gowtham Nirmal Jonnalagadda, Xiaojing Wu, Lukáš Hronek, Zdenek Futera","doi":"10.1021/acs.jpclett.4c02230","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02230","url":null,"abstract":"Cytochrome b562 is a small redox-active heme protein that has served as an important model system for understanding biological electron transfer processes. Here, we present a comprehensive theoretical study of electron transport mechanisms in protein–metal junctions incorporating cytochrome b562 using a multi-scale computational approach. Employing molecular dynamics (MD) simulations, we generated junction geometries for both vacuum-dried and solvated conditions, with the protein covalently bound to gold contacts in various configurations. Coherent tunneling, described by the Landauer–Buttiker formalism within the density functional theory (DFT) framework, is compared to the incoherent hopping charge transport mechanism captured by the semi-classical Marcus theory. The tunneling was identified as the dominant mechanism explaining the experimental data measured on the cytochrome b562 junctions, exhibiting exponential yet very shallow distance dependence. While the structural orientations and protein contacts with the electrodes influence the junction conductance significantly, the solvation effects are relatively small, affecting the electronic properties mostly via the adsorption arrangement. On the other hand, the considerable temperature dependence of the conductance was found strong only for hopping, while the tunneling current magnitudes remain practically unaffected and are a good indicator of the coherent mechanism in this case.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"7 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599628","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

Vibrational Mode-Dependent Circular Dichroism of Jet-Cooled Styrene Oxide 喷气冷却氧化苯乙烯的振动模式依赖性圆二色性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-12 DOI: 10.1021/acs.jpclett.4c02855

Jiyeon Yun, Changseop Jeong, Jiyoung Heo, Nam Joon Kim

引用次数: 0

Short-Range Coulomb Interaction Is a Key to Switch the Utilization of Higher Triplet Excitons in Multiresonance Thermally Activated Delayed Fluorescence Doped Film 短程库仑相互作用是切换多共振热激活延迟荧光掺杂薄膜中较高三重激子利用率的关键

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-11 DOI: 10.1021/acs.jpclett.4c02702

Yu-Chao Zheng, Yue Ren, Ming-Yue Sui, Ming-Yang Li, Guang-Yan Sun

{"title":"Short-Range Coulomb Interaction Is a Key to Switch the Utilization of Higher Triplet Excitons in Multiresonance Thermally Activated Delayed Fluorescence Doped Film","authors":"Yu-Chao Zheng, Yue Ren, Ming-Yue Sui, Ming-Yang Li, Guang-Yan Sun","doi":"10.1021/acs.jpclett.4c02702","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02702","url":null,"abstract":"Multiresonance thermally activated delayed fluorescence (MR-TADF) materials have attracted widespread attention due to ultrahigh definition display standards. However, many MR-TADF materials lack TADF properties in both the solution and solid states. Interestingly, the TADF characteristics appear once these MR-TADF compounds are doped in a suitable host film, but the precise mechanism involved in the host–guest interaction remains uncertain. Herein, we systematically investigated the role of host–guest interactions employing doped films (DABNA-1@mCBP and DABNA-1@DPEPO) with opposite phenomena. The results indicate that mCBP with a V-shape and enhanced rigidity could facilitate the formation of an energy spacing layer by employing short-range Coulomb energy through the MR luminescent core, which could offset the sensitivity of the stacking distance, enhancing the coupling between T1 and T2, and thus switch the reverse internal conversion and the higher T2 reverse intersystem crossing process. This work is a further development of luminescence mechanisms and an update of the host–guest interaction criteria for the targeted design of doped films.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"2 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599389","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

An Efficient and Stable Polarizing Agent for In-Cell Magic-Angle Spinning Dynamic Nuclear Polarization NMR Spectroscopy 用于细胞内魔角旋转动态核极化 NMR 光谱的高效稳定极化剂

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-11-11 DOI: 10.1021/acs.jpclett.4c02709

Yu Rao, Pierrick Berruyer, Andrea Bertarello, Amrit Venkatesh, Marinella Mazzanti, Lyndon Emsley

{"title":"An Efficient and Stable Polarizing Agent for In-Cell Magic-Angle Spinning Dynamic Nuclear Polarization NMR Spectroscopy","authors":"Yu Rao, Pierrick Berruyer, Andrea Bertarello, Amrit Venkatesh, Marinella Mazzanti, Lyndon Emsley","doi":"10.1021/acs.jpclett.4c02709","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02709","url":null,"abstract":"Nuclear Magnetic Resonance (NMR) spectroscopy would be a method of choice to follow biochemical events in cells because it can analyze molecules in complex environments. However, the intrinsically low sensitivity of NMR makes in-cell measurements challenging. Dynamic Nuclear Polarization (DNP) has emerged as a method to circumvent this limitation, but most polarizing agents developed for DNP are unstable in reducing cellular environments. Here, we introduce the use of Gd(III)-based DNP polarizing agents for in-cell NMR spectroscopy. Specifically, we show their persistent stability in cellular formulations, and we investigate the DNP performance of the Gd(III)-based complex [Gd(tpatcn)] in human embryonic kidney cell lysates and intact cells. For cell lysates, DNP enhancements up to −27 are obtained on the cellular signals, reproducible even after storage at room temperature for days. Mixing the [Gd(tpatcn)] solution with intact cells enables the observation of cellular signals with DNP, and DNP enhancement factors of about −40 are achieved.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"4 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599392","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