The Journal of Physical Chemistry Letters最新文献

Large Magnetic Anisotropy in van der Waals Ferromagnet Fe3GaTe2 above Room Temperature 室温以上范德华铁磁体 Fe3GaTe2 中的大磁各向异性

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-21 DOI: 10.1021/acs.jpclett.4c02426

Yilian Xi, Hanqing Shi, Jingwei Zhang, Heping Li, Ningyan Cheng, Hang Xu, Jiaqi Liu, Keren Li, Huaiming Guo, Haifeng Feng, Jianfeng Wang, Weichang Hao, Yi Du

{"title":"Large Magnetic Anisotropy in van der Waals Ferromagnet Fe3GaTe2 above Room Temperature","authors":"Yilian Xi, Hanqing Shi, Jingwei Zhang, Heping Li, Ningyan Cheng, Hang Xu, Jiaqi Liu, Keren Li, Huaiming Guo, Haifeng Feng, Jianfeng Wang, Weichang Hao, Yi Du","doi":"10.1021/acs.jpclett.4c02426","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02426","url":null,"abstract":"Discoveries of above-room-temperature intrinsic ferromagnetism in two-dimensional (2D) van der Waals (vdW) materials offer a platform for studying fundamental 2D magnetism and spintronic devices, especially the recently discovered above-room-temperature 2D vdW Fe3GaTe2 (FGaT). However, the magnetic mechanism in FGaT remains elusive. Here, a detailed investigation using magnetic force microscopy on the thickness-dependent magnetic behavior of FGaT single crystals is reported. The Heisenberg exchange interaction constant (J) at room temperature is determined to be 1.32836 × 10–12 J/m. Our study combining angle-resolved photoemission spectroscopy and density functional theory suggests that the high Curie temperature in FGaT is attributed to the shift of the localized Fe d band toward the Fermi level as well as the enhanced magnetic exchange effect due to the strong itinerant ability of Fe. This work sheds light on the understanding of magnetism in FGaT and provides a promising platform to investigate the mechanisms of 2D magnetic materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452016","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

Nucleoprotein Phase-Separation Affinities Revealed via Atomistic Simulations of Short Peptide and RNA Fragments 通过对短肽和 RNA 片段的原子模拟揭示核蛋白相分离亲和力

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-21 DOI: 10.1021/acs.jpclett.4c02654

Vysakh Ramachandran, William Brown, Christopher Gayvert, Davit A. Potoyan

{"title":"Nucleoprotein Phase-Separation Affinities Revealed via Atomistic Simulations of Short Peptide and RNA Fragments","authors":"Vysakh Ramachandran, William Brown, Christopher Gayvert, Davit A. Potoyan","doi":"10.1021/acs.jpclett.4c02654","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02654","url":null,"abstract":"Liquid–liquid phase separation of proteins and nucleic acids into condensate phases is a versatile mechanism for ensuring the compartmentalization of cellular biochemistry. RNA molecules play critical roles in these condensates, particularly in transcriptional regulation and stress responses, exhibiting a wide range of thermodynamic and dynamic behaviors. However, deciphering the molecular grammar that governs the stability and dynamics of protein–RNA condensates remains challenging due to the multicomponent and heterogeneous nature of condensates. In this study, we employ atomistic simulations of 20 distinct mixtures containing minimal RNA and peptide fragments which allows us to dissect the phase-separating affinities of all 20 amino acids in the presence of RNA. Our findings elucidate chemically specific interactions, hydration profiles, and ionic effects that synergistically promote or suppress protein–RNA phase separation. We map a ternary phase diagram of interactions, identifying four distinct groups of residues that promote, maintain, suppress, and disrupt protein–RNA clusters.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452014","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

Bidirectional Allostery Mechanism in Catch-Bond Formation of CD44 Mediated Cell Adhesion CD44 介导的细胞粘附捕捉键形成过程中的双向异位机制

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-21 DOI: 10.1021/acs.jpclett.4c02598

Xingyue Guan, Yunqiang Bian, Zilong Guo, Jian Zhang, Yi Cao, Wenfei Li, Wei Wang

{"title":"Bidirectional Allostery Mechanism in Catch-Bond Formation of CD44 Mediated Cell Adhesion","authors":"Xingyue Guan, Yunqiang Bian, Zilong Guo, Jian Zhang, Yi Cao, Wenfei Li, Wei Wang","doi":"10.1021/acs.jpclett.4c02598","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02598","url":null,"abstract":"Catch-bonds, whereby noncovalent ligand–receptor interactions are counterintuitively reinforced by tensile forces, play a major role in cell adhesion under mechanical stress. A basic prerequisite for catch-bond formation, as implicated in classic catch-bond models, is that force-induced remodeling of the ligand binding interface occurs prior to bond rupture. However, what strategy receptor proteins utilize to meet such specific kinetic control remains elusive. Here we report a bidirectional allostery mechanism of catch-bond formation based on theoretical and molecular dynamics simulation studies. Binding of ligand allosterically reduces the threshold force for unlocking of otherwise stably folded force-sensing element (i.e., forward allostery), so that a much smaller tensile force can trigger the conformational switching of receptor protein to high binding-strength state via backward allosteric coupling before bond rupture. Such bidirectional allostery fulfills the specific kinetic control required by catch-bond formation and is likely to be commonly utilized in cell adhesion. The essential thermodynamic and kinetic features of receptor proteins essential for catch-bond formation were identified.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452029","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

Conductance Channels in a Single-Entity Enzyme 单实体酶中的传导通道

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-21 DOI: 10.1021/acs.jpclett.4c01796

Rafael Neri Prystaj Colombo, Steffane Q. Nascimento, Frank Nelson Crespilho

{"title":"Conductance Channels in a Single-Entity Enzyme","authors":"Rafael Neri Prystaj Colombo, Steffane Q. Nascimento, Frank Nelson Crespilho","doi":"10.1021/acs.jpclett.4c01796","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c01796","url":null,"abstract":"For a long time, the prevailing view in the scientific community was that proteins, being complex macromolecules composed of amino acid chains linked by peptide bonds, adopt folded structure with insulating or semiconducting properties, with high bandgaps. However, recent discoveries of unexpectedly high conductance levels, reaching values in the range of dozens of nanosiemens (nS) in proteins, have challenged this conventional understanding. In this study, we used scanning tunneling microscopy (STM) to explore the single-entity conductance properties of enzymatic channels, focusing on bilirubin oxidase (BOD) as a model metalloprotein. By immobilizing BOD on a conductive carbon surface, we discern its preferred orientation, facilitating the formation of electronic and ionic channels. These channels show efficient electron transport (ETp), with apparent conductance up to the 15 nS range. Notably, these conductance pathways are localized, minimizing electron transport barriers due to solvents and ions, underscoring BOD’s redox versatility. Furthermore, electron transfer (ET) within the BOD occurs via preferential pathways. The alignment of the conductance channels with hydrophilicity maps, molecular vacancies, and regions accessible to electrolytes explains the observed conductance values. Additionally, BOD exhibits redox activity, with its active center playing a critical role in the ETp process. These findings significantly advance our understanding of the intricate mechanisms that govern ETp processes in proteins, offering new insights into the conductance of metalloproteins.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452090","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

Electron Transfer Capability in Atomic Hydrogen Reactions for Imidazole Groups Bound to the Insulating Alkanethiolate Layer on Au(111). 与 Au(111) 上绝缘烷硫酸盐层结合的咪唑基团在原子氢反应中的电子转移能力。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02306

Hiroyuki S Kato,Mizuho Muroyama,Nano Kobayakawa,Riku Muneyasu,Yasutaka Tsuda,Natsumi Murase,Seiya Watanabe,Takashi Yamada,Yusuke Kanematsu,Masanori Tachikawa,Megumi Akai-Kasaya,Michio Okada,Akitaka Yoshigoe

{"title":"Electron Transfer Capability in Atomic Hydrogen Reactions for Imidazole Groups Bound to the Insulating Alkanethiolate Layer on Au(111).","authors":"Hiroyuki S Kato,Mizuho Muroyama,Nano Kobayakawa,Riku Muneyasu,Yasutaka Tsuda,Natsumi Murase,Seiya Watanabe,Takashi Yamada,Yusuke Kanematsu,Masanori Tachikawa,Megumi Akai-Kasaya,Michio Okada,Akitaka Yoshigoe","doi":"10.1021/acs.jpclett.4c02306","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02306","url":null,"abstract":"The charge transfer capability associated with chemical reactions at metal-organic interfaces was studied via the atomic H addition reaction for an imidazole-terminated alkanethiolate self-assembled monolayer (Im-SAM) film on Au(111) at room temperature, using near-edge X-ray absorption fine structure spectroscopy, infrared reflection absorption spectroscopy, work function measurements, and density functional theory calculations. The imidazolium cation is a stable species in liquids; therefore, it is pertinent to determine whether the hydrogenation reactions of the imidazole groups produce imidazolium cations accompanied by electron transfer to the Au substrate, even in the absence of solvate and/or counterions on the insulating alkanethiolate layer. The experiments made it clear that the imidazolium moieties were formed during the irradiation of Im-SAM with atomic H. Theoretical model calculations also revealed that the total energies and molecular orbital levels satisfied the imidazolium cation formation associated with electron transfer. In a detailed analysis of the work function change depending on H irradiation, we confirmed that some of the imidazolium radicals became cations in Im-SAM.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449242","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

Elucidating Dynamical Behaviors in Kinetically Constrained Models via Energy-Activity Double-Biased Matrix Product State Analysis 通过能量-活动双偏置矩阵乘积状态分析阐明动力学约束模型中的动力学行为

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02197

Yoong Hee Lee, Jay-Hak Lee, YounJoon Jung

{"title":"Elucidating Dynamical Behaviors in Kinetically Constrained Models via Energy-Activity Double-Biased Matrix Product State Analysis","authors":"Yoong Hee Lee, Jay-Hak Lee, YounJoon Jung","doi":"10.1021/acs.jpclett.4c02197","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02197","url":null,"abstract":"We investigate dynamical phase transitions in two representative kinetically constrained models: the 1D Fredrickson–Andersen and East Models. A recently developed energy-activity double-bias approach utilizing both s and g fields, conjugated with dynamical activity and trajectory energy, is combined with matrix product state (MPS) methods. It is demonstrated that MPS methods facilitate the numerical approximation of large-deviation statistics of dynamics by determining the eigenvalues of tilted dynamical generators under the influence of double-biasing fields. Specifically, by focusing on the g-field, a nearly “half-filled” state at moderate negative g values is identified, indicating the potential existence of an anomalous phase. Additionally, dynamical quantities under various s, g, and T conditions are obtained via tensor networks, showing good qualitative consistency with mean-field results and our previous extensive numerical simulation results obtained by the path sampling method. Our study introduces novel methodologies for examining decoupled dynamical behaviors that, although energetically active, remain dynamically inactive within the system. This approach offers a fresh perspective on the theoretical framework and computational strategies for studying dynamical phase transitions in kinetically constrained systems.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449280","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

A-Site Doping Promotes CO2 Activation and Prolongs Charge Carrier Lifetimes in SrTiO3: Insight from Quantum Dynamics. A 位掺杂促进 SrTiO3 中二氧化碳的活化并延长电荷载流子的寿命：量子动力学的启示。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02649

Xiaodan Yan,Jinlu He

引用次数: 0

Dynamics of Vortex Matter in 2D Gapless Superconducting Materials with Impurities. 含杂质的二维无间隙超导材料中涡旋物质的动力学。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02775

Valeriia D Pashkovskaia,Elwis C S Duarte,Rafael Zadorosny,Edson Sardella,Dmitrii A Abrameshin,Andrey S Vasenko,Tiago T Saraiva

{"title":"Dynamics of Vortex Matter in 2D Gapless Superconducting Materials with Impurities.","authors":"Valeriia D Pashkovskaia,Elwis C S Duarte,Rafael Zadorosny,Edson Sardella,Dmitrii A Abrameshin,Andrey S Vasenko,Tiago T Saraiva","doi":"10.1021/acs.jpclett.4c02775","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02775","url":null,"abstract":"The recent interest in using ultrafast single-photon detectors in research and commercial applications has garnered significant attention from the scientific community. The dynamic event in the detection process consists of a photon causing local destruction of the order parameter, and then the applied current dissipates heat, bringing the material even more out of the superconducting state and then spiking a voltage peak in a measurement device. We investigated the role of superconducting and thermal parameters of the Generalized Time-Dependent Ginzburg-Landau (GTDGL) theory within the event of the first vortex penetration and the thermal dissipation in superconductors near the critical temperature. Moreover, in the vicinity of the Bogomolny point of the static Ginzburg-Landau theory, where κ ≈ 1/√2 and T → Tc, it has been found severely different vortex profiles. We point out that within the GTDGL theory, the presence of impurities (usual or paramagnetic) influences flux penetration and enhances the dissipation of heat, causing anomalous vortex configurations.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449245","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

New Hypothesis on Enhancing β-Sheet Formation during the Tau Fragment Dimer Transition from a Flexible Monomer: Insights into Primary Nucleation Processes by Histidine Behaviors. 在 Tau 片段二聚体从柔性单体转变过程中促进 β 片形成的新假说：组氨酸行为对初级成核过程的启示。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02419

Yue Sun,Yaru Shi,Jing Li,Aniu Qian,Hu Shi

{"title":"New Hypothesis on Enhancing β-Sheet Formation during the Tau Fragment Dimer Transition from a Flexible Monomer: Insights into Primary Nucleation Processes by Histidine Behaviors.","authors":"Yue Sun,Yaru Shi,Jing Li,Aniu Qian,Hu Shi","doi":"10.1021/acs.jpclett.4c02419","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02419","url":null,"abstract":"Slight perturbations in pH can have significant effects on the primary nucleation processes of the tau protein. The behaviors of histidine due to its pivotal role in modulating H-bonding network interactions and electrostatic interactions have garnered considerable attention, as it can influence the structural characteristics and aggregation properties. However, the nucleation mechanisms and related intermediates are still unclear. In the current study, we performed nine independent replica exchange molecular dynamics simulations to investigate dimer formation involving R3(εδ) in conjunction with the R1, R2, and R4 monomers. Our findings substantiate that, in comparison to R1-R3(εδ) and R4-R3(εδ) systems, the R2-R3(εδ) systems consistently manifest the highest averaged β-sheet content, with the fundamental feature of R3(εδ) promoting R2 rearrangement. Our comprehensive analysis reveals that high-β-sheet-rich systems exhibit a conserved three/five β-strand structure. In these β-strand-rich systems, one chain [R1/R2/R4 or R3(εδ)] with robust intrachain H-bonding interactions coordinates with another chain through interchain H-bonding interactions, contributing to the overall stability. Furthermore, we discuss distinct histidine behaviors, including backbone/side chain interactions and donor/acceptor roles. This study provides a comprehensive understanding of the aggregation propensities of soluble tau oligomers and sheds light on the primary nucleation mechanism. It contributes to a new perspective for understanding protein folding and misfolding.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142449243","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

Sequence Length Controls Coil-to-Globule Transition in Elastin-like Polypeptides 序列长度控制弹性蛋白样多肽中线圈到球状的转变

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2024-10-18 DOI: 10.1021/acs.jpclett.4c02568

Tatiana I. Morozova, Nicolás A. García, Jean-Louis Barrat

引用次数: 0