The Journal of Physical Chemistry Letters最新文献_第4页

Distinct Magnetic Response to Isoelectronic Substitution in (Fe1-δ)3GeTe2: A Mössbauer Spectroscopy Study. （Fe1-δ）3GeTe2中等电子取代的独特磁响应：Mössbauer光谱研究。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-29 DOI: 10.1021/acs.jpclett.5c02407

Shixin Hu,Jijun Xue,Xu Bai,Hua Pang,Junli Zhang

{"title":"Distinct Magnetic Response to Isoelectronic Substitution in (Fe1-δ)3GeTe2: A Mössbauer Spectroscopy Study.","authors":"Shixin Hu,Jijun Xue,Xu Bai,Hua Pang,Junli Zhang","doi":"10.1021/acs.jpclett.5c02407","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02407","url":null,"abstract":"Isoelectronic substitution is a powerful tool for disentangling charge-carrier and lattice-driven effects in van der Waals (vdW) magnets, yet its microscopic impact is still poorly explored. Here, we systematically investigate the effect of isoelectronic Ni and Co substitution on the magnetic properties of (Fe1-δ)3GeTe2 single crystals using a combination of macroscopic magnetometry and microscopic 57Fe Mössbauer spectroscopy. Although substituting Fe with specific concentrations of Ni and Co was designed to introduce the same total number of excess 3d electrons, these substituents induce markedly different magnetic responses, with Co leading to a more pronounced suppression of the Curie temperature and saturation magnetization. Mössbauer analysis reveals that these differences originate from dopant-specific site occupancy and the resulting local modification of Fe magnetic exchange pathways. In particular, Co preferentially substitutes at the (Fe1)A and Fe2 sites, whereas Ni exhibits partial interstitial incorporation, introducing additional structural disorder. These local effects alter hyperfine interactions, suppress Fe-Fe exchange, and promote magnetic moment localization. Our findings highlight the critical role of dopant identity beyond electron count, emphasizing that local atomic environments govern the tuning of magnetic order in vdW ferromagnets. This work provides microscopic insight into substitution-driven magnetism and guides future strategies for tailoring spintronic functionalities in two-dimensional materials.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"17 1","pages":"10336-10344"},"PeriodicalIF":6.475,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188922","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

From Salt-in-Water to Water-in-Salt: How Ion Identity Governs Surfactant Self-Assembly in Salt-Water-Nonionic Surfactant Mixtures. 从水中盐到盐中水：离子同一性如何控制盐-水-非离子表面活性剂混合物中表面活性剂的自组装。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-29 DOI: 10.1021/acs.jpclett.5c02158

Cemal Albayrak,Yizhen Li,Ömer Dag,Gregory G Warr

{"title":"From Salt-in-Water to Water-in-Salt: How Ion Identity Governs Surfactant Self-Assembly in Salt-Water-Nonionic Surfactant Mixtures.","authors":"Cemal Albayrak,Yizhen Li,Ömer Dag,Gregory G Warr","doi":"10.1021/acs.jpclett.5c02158","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02158","url":null,"abstract":"Self-assembled mesostructures derived from nonionic surfactants can be tuned by adjusting parameters, such as the hydrophilic-lipophilic balance or electrolyte content. Such tuning permits control of key functional properties including conductivity, mass transport, and rheology. Although salts have frequently been used to influence the phase behavior of nonionic surfactant mixtures, they are almost always treated as minor additives. In contrast, here we extended the salt concentration range to hydrous melt and even nearly anhydrous conditions in which the salt no longer acts as an additive but replaces water as the solvent component. To elucidate the effect of ion identity on phase behavior, partial pseudoternary phase diagrams of salt-water-C12E10 mixtures were constructed using NaNO3, Zn(NO3)2, Ca(NO3)2 and CaCl2. Each salt represents a distinct set of intermolecular interactions and gives rise to markedly different phase diagrams, demonstrating that salt selection, or using a mixture of salts, can be strategically employed to finely tune self-assembly across the full hydration window.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"66 1","pages":"10299-10305"},"PeriodicalIF":6.475,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182569","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

The First Experimental Charge Density Studies and Comparative Periodic DFT Calculations for Crystalline Hydrogen Peroxide Adducts: Peculiarities of the HO-OH Covalent Bond. 第一次实验电荷密度研究和比较周期DFT计算的结晶过氧化氢加合物：hooh - oh共价键的特性。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-29 DOI: 10.1021/acs.jpclett.5c01752

Mikhail V Vener,Alexander G Medvedev,Adam I Stash,Alexey A Mikhaylov,Petr V Prikhodchenko,Dmitry E Baravikov,Igor L Dalinger,Andrei V Churakov,Fedor M Dolgushin

{"title":"The First Experimental Charge Density Studies and Comparative Periodic DFT Calculations for Crystalline Hydrogen Peroxide Adducts: Peculiarities of the HO-OH Covalent Bond.","authors":"Mikhail V Vener,Alexander G Medvedev,Adam I Stash,Alexey A Mikhaylov,Petr V Prikhodchenko,Dmitry E Baravikov,Igor L Dalinger,Andrei V Churakov,Fedor M Dolgushin","doi":"10.1021/acs.jpclett.5c01752","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01752","url":null,"abstract":"Charge density distributions in crystalline peroxosolvates of parabanic acid C3H2N2O3·0.5H2O2 and ammonium salt of 3,4,5-trinitropyrazole NH4+·C3N5O6-·0.5H2O2 derived from the high-resolution single-crystal X-ray experiments are reported with comparative periodic DFT calculations. Both multipole refinement and theoretical studies showed that the O-O bonds exhibit a (3, -1) critical point with electron density (ρb) of approximately 0.24 a.u. Experimental deformation density maps show not an accumulation but a depletion of charge density around O-O bond centers. The Laplacian values of electron density (∇2ρb) obtained from X-ray data are definitely positive and lie within 0.70-0.79 a.u. Theoretical values of ∇2ρb noticeably depend on the basis sets. They exhibit small, both positive and negative values for the modest basis sets and are around 0.3 a.u. for the pob-TZVP basis set. Thus, the O-O linkage can be considered as a specific ≪charge-shift≫ bond. The F-F bond in crystalline α-F2 exhibits similar features.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"116 1","pages":"10316-10323"},"PeriodicalIF":6.475,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188926","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 Diagrams and Thermodynamic Behaviors of CunAg143-n (n = 0 ∼ 143) Alloying Nanoparticles During Cooling: Implications from Atomic Simulations. cnag143 -n （n = 0 ~ 143）合金纳米粒子在冷却过程中的结构图和热力学行为：来自原子模拟的启示。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-26 DOI: 10.1021/acs.jpclett.5c01712

Jinhan Liu,Pengyi Zhang,Ying Yan,Lin Zhang

{"title":"Structural Diagrams and Thermodynamic Behaviors of CunAg143-n (n = 0 ∼ 143) Alloying Nanoparticles During Cooling: Implications from Atomic Simulations.","authors":"Jinhan Liu,Pengyi Zhang,Ying Yan,Lin Zhang","doi":"10.1021/acs.jpclett.5c01712","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c01712","url":null,"abstract":"Structural diagrams and thermodynamic function quantities of CunAg143-n (n = 0 ∼ 143) alloying nanoparticles are studied by molecular dynamics simulations within the framework of embedded atom method potential. The simulation results at atomic scale show that the alloy composition has a significant effect on the changes of the free energies and shapes of molten nanoparticles. The structural diagrams reveal structural transition characteristics of the binary nanoparticles at different temperatures on cooling, where the transition temperature between the liquid, α, γ, Ih, and β structures changes significantly with changing Cu atomic number in the particles. The binary nanoparticles show significantly different packing patterns from their bulk counterparts. Typical alloying particles with different compositions exhibit diversities in packing patterns. These findings contribute to the understanding of the fundamental issues involved in alloying among Cu and Ag atoms, which are important for precisely controlling the preparation of Cu-Ag nanoalloys with specific structures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"3 1","pages":"10291-10298"},"PeriodicalIF":6.475,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140473","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 Nonlinear Optical Properties of (1R,2R)-DACHGeI4 through Ce3+ Doping Ce3+掺杂调制(1R,2R)-DACHGeI4的非线性光学性质

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-26 DOI: 10.1021/acs.jpclett.5c02690

Jing Huang, , , Hualin Bi, , , Huitao Zhang, , , Jia Zhou, , , Jialin Zhang, , , Huanbo Wang, , and , Jun Wang*,

{"title":"Modulating Nonlinear Optical Properties of (1R,2R)-DACHGeI4 through Ce3+ Doping","authors":"Jing Huang, , , Hualin Bi, , , Huitao Zhang, , , Jia Zhou, , , Jialin Zhang, , , Huanbo Wang, , and , Jun Wang*, ","doi":"10.1021/acs.jpclett.5c02690","DOIUrl":"10.1021/acs.jpclett.5c02690","url":null,"abstract":"Chiral perovskites exhibit great potential in polarization optics and spintronics due to their excellent structural and electronic properties. This study uses (1R,2R)-DACH as the organic component to synthesize a novel 2D germanium-based chiral perovskite single crystal, (1R,2R)-DACHGeI4 (where (1R,2R)-DACH is (1R,2R)-(−)-1,2-cyclohexanediamine). To address the impact of lattice defects in germanium-based perovskites on optical properties, a rare-earth Ce3+ doping compensation strategy is adopted. Experiments show Ce3+ doping enhances photoluminescence quantum yield and fluorescence lifetime, regulates spintronic states, replaces partial Ge2+ to cause lattice distortion, changes the crystal space group from chiral P21212 to nonchiral Pba2, and destroys the chiral structure. DFT calculations confirm these experimental results. This work provides a new approach to improving the nonlinear optical properties of 2D germanium-based perovskites and deepens the understanding of the intrinsic relationship between chiral perovskite structures and spintronic states.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10273–10281"},"PeriodicalIF":4.6,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140509","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

Organic Cation Dynamics in the Layered Lead Iodide Perovskites BA2PbI4 and PEA2PbI4. 层状碘化铅钙钛矿BA2PbI4和PEA2PbI4的有机阳离子动力学。

IF 6.475 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-26 DOI: 10.1021/acs.jpclett.5c02091

Rasmus Lavén,Michael M Koza,Niina H Jalarvo,Marco Moroni,Lorenzo Malavasi,Maths Karlsson

{"title":"Organic Cation Dynamics in the Layered Lead Iodide Perovskites BA2PbI4 and PEA2PbI4.","authors":"Rasmus Lavén,Michael M Koza,Niina H Jalarvo,Marco Moroni,Lorenzo Malavasi,Maths Karlsson","doi":"10.1021/acs.jpclett.5c02091","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c02091","url":null,"abstract":"We report on a quasielastic neutron scattering (QENS) study of the rotational dynamics of organic cations in the optoelectronic layered metal halide perovskites BA2PbI4 (BA = butylammonium, CH3(CH2)3NH3) and PEA2PbI4 (PEA = phenethylammonium, C6H5(CH2)2NH3). For BA2PbI4, the measurements reveal highly temperature dependent dynamics. Between 100 and 260 K, the dynamics are ascribed to rotational dynamics of the -CH3 and -NH3 groups of the BA cation, whereas above 300 K we also observe the additional presence of full rotations of the whole BA cation around its long molecular axis. For PEA2PbI4, the measurements reveal dynamics that are more spatially restricted in nature, i.e., rotational dynamics of the -NH3 groups of the PEA cations for temperatures above 200 K, with no other dynamical processes observed at higher temperatures. A correlation of the dynamics results to literature data on the optical properties of the materials suggests that the more restricted organic cation dynamics in PEA2PbI4 are related to its longer lifetime and diffusion lengths for charge carriers, as compared to BA2PbI4.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"15 1","pages":"10282-10290"},"PeriodicalIF":6.475,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140474","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

Strain-Induced Interlayer Interactions under Hydrostatic Pressure Can Boost Circularly Polarized Luminescence in Chiral Hybrid Halide Perovskites 静水压力下应变诱导的层间相互作用可增强手性杂化卤化物钙钛矿的圆极化发光。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-25 DOI: 10.1021/acs.jpclett.5c02393

Mariagrazia Fortino, , , Alessandro Mattoni, , , Sascha Feldmann, , and , Adriana Pietropaolo*,

{"title":"Strain-Induced Interlayer Interactions under Hydrostatic Pressure Can Boost Circularly Polarized Luminescence in Chiral Hybrid Halide Perovskites","authors":"Mariagrazia Fortino, , , Alessandro Mattoni, , , Sascha Feldmann, , and , Adriana Pietropaolo*, ","doi":"10.1021/acs.jpclett.5c02393","DOIUrl":"10.1021/acs.jpclett.5c02393","url":null,"abstract":"The influence of hydrostatic pressure on the structure and circularly polarized luminescence (CPL) of the 2D chiral perovskite S-(MBA)2PbI4 (MBA = methylbenzylammonium) is investigated and compared to that of a brominated derivative, employing parallel-bias metadynamics coupled with excited-state ab initio molecular dynamics and time-dependent DFT simulations. A stepwise increase in pressure is shown to promote noncovalent interactions above the Fermi level, which in turn amplifies CPL emission and even allows for switching its sign. A comparable effect can be obtained by brominating the aromatic ring of (R)- or (S)-methylbenzylammonium. Strain, arising from both intrinsic structural constraints and applied external pressure, can deform the lattice and distort the inorganic octahedra. These strain-induced distortions promote parallel stacking of the chiral ligands, resulting in a CPL response within stable free energy minima and enabling chiral memory. We conclude that interlayer interactions can act as a powerful tool for engineering chiroptical properties through external pressure or structure-induced strain (internal pressure), enabling the design of new stimulus-responsive materials or the tuning of existing ones via strain engineering.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10234–10239"},"PeriodicalIF":4.6,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c02393","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rational Design of a Cu(II) Spin Label Improves the Sensitivity of Distance Measurements 合理设计Cu（II）自旋标签，提高距离测量的灵敏度。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-25 DOI: 10.1021/acs.jpclett.5c02221

Shramana Palit, , , Zikri Hasanbasri, , , Nicholas A. Moriglioni, , , Joshua Casto, , and , Sunil Saxena*,

{"title":"Rational Design of a Cu(II) Spin Label Improves the Sensitivity of Distance Measurements","authors":"Shramana Palit, , , Zikri Hasanbasri, , , Nicholas A. Moriglioni, , , Joshua Casto, , and , Sunil Saxena*, ","doi":"10.1021/acs.jpclett.5c02221","DOIUrl":"10.1021/acs.jpclett.5c02221","url":null,"abstract":"The measurement of distance constraints in biomolecules using Cu(II) spin labels at Q-band EPR is complicated due to the selective excitation of only some orientations of the label. Here, we introduce a new Cu(II) spin label, in which the divalent metal is coordinated equatorially by four nitrogen atoms. Such chelation reduces the g anisotropy of the Cu(II) spin, which reduces the spectral width. We show that the complex coordinates to target labeling sites on a protein and provides narrow distance distributions on proteins. DEER data acquired across different fields at Q-band show the same period of modulation, which suggests proper orientational averaging. Thus, a single measurement at the magnetic field corresponding to the maximum intensity is sufficient to measure the distance distribution. Although the label does not bind stoichiometrically, we observe a 2.3-fold improvement in sensitivity in half the data acquisition time compared to those of existing Cu(II) spin labels.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10256–10264"},"PeriodicalIF":4.6,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.jpclett.5c02221","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anomalous Temperature-Dependent Thermal Transport in Crystalline Polyethylene Driven by Strong Anharmonicity 由强非调和性驱动的结晶聚乙烯反常温度相关热输运。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-25 DOI: 10.1021/acs.jpclett.5c02084

Shouhang Li*, , , Philippe Dollfus, , , Jérôme Saint-Martin, , and , Davide Romanin,

{"title":"Anomalous Temperature-Dependent Thermal Transport in Crystalline Polyethylene Driven by Strong Anharmonicity","authors":"Shouhang Li*, , , Philippe Dollfus, , , Jérôme Saint-Martin, , and , Davide Romanin, ","doi":"10.1021/acs.jpclett.5c02084","DOIUrl":"10.1021/acs.jpclett.5c02084","url":null,"abstract":"Thermal conductivity typically decreases with increasing temperature along the three principal crystalline directions, primarily due to enhanced phonon anharmonicity. In this work, we conducted a comprehensive first-principles investigation of thermal transport in crystalline polyethylene by solving the Wigner transport equation, assisted with the stochastic self-consistent harmonic approximation. It is found that the thermal conductivity of crystalline polyethylene decreases along the chain direction, but increases nearly linearly in the out-of-chain directions. This anomalous contrasting behavior stems from the dominance of particle-like transport along the chain and wave-like transport in the out-of-chain directions. The strong anharmonicity facilitates phonon tunneling between high- and low-frequency modes in the out-of-plane directions. Therefore, further enhancement of thermal conductivity in those directions could benefit from increased anharmonicity and the introduction of additional disorder. These findings provide fundamental insights into the thermal transport mechanisms of anisotropic crystalline polymers, offering valuable guidance for rationally engineering their thermal properties.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10210–10215"},"PeriodicalIF":4.6,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140149","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

Single-Molecule Fluorescence Spectroscopy of 4-Cyanotryptophan and Its Application in Photoinduced Electron Transfer Fluorescence Correlation Spectroscopy 4-氰色氨酸的单分子荧光光谱及其在光致电子转移荧光相关光谱中的应用。

IF 4.6 2区化学

The Journal of Physical Chemistry Letters Pub Date : 2025-09-25 DOI: 10.1021/acs.jpclett.5c02528

Kailin Tang, , , Manxi Wang, , and , Feng Gai*,

{"title":"Single-Molecule Fluorescence Spectroscopy of 4-Cyanotryptophan and Its Application in Photoinduced Electron Transfer Fluorescence Correlation Spectroscopy","authors":"Kailin Tang, , , Manxi Wang, , and , Feng Gai*, ","doi":"10.1021/acs.jpclett.5c02528","DOIUrl":"10.1021/acs.jpclett.5c02528","url":null,"abstract":"Single-molecule fluorescence spectroscopy is a powerful tool to study the conformational dynamics of proteins. However, the protein in question was normally labeled with one or two fluorescent dyes, which may induce undesirable perturbation toward the protein’s native property. Therefore, a long-sought goal is to use tryptophan, a natural fluorescent amino acid, for single-molecule fluorescence studies. Nevertheless, this has been shown to be challenging. Herein, we demonstrate that 4-cyanotryptophan, a genetically incorporable blue fluorescent amino acid with a large fluorescence quantum yield (>0.8), is bright enough for single-molecule fluorescence detection. In particular, we demonstrate its utility in florescence correlation spectroscopy (FCS) and use it to probe the conformational dynamics of the Pin1 WW domain via PET–FCS. We find that the transient hydrophobic interactions in the unfolded state of this protein occur on a time scale of ca. 10 μs, which provides insight into the earliest events in protein folding.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 39","pages":"10240–10245"},"PeriodicalIF":4.6,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145140204","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