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Helical-photon-dressed states determining unidirectional π-electron rotations in aromatic ring molecules. 决定芳香环分子中单向π电子旋转的螺旋光子抑制态。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0215065
Hirobumi Mineo, Quang Huy Ho, Ngoc Loan Phan, Gap-Sue Kim, Yuichi Fujimura
{"title":"Helical-photon-dressed states determining unidirectional π-electron rotations in aromatic ring molecules.","authors":"Hirobumi Mineo, Quang Huy Ho, Ngoc Loan Phan, Gap-Sue Kim, Yuichi Fujimura","doi":"10.1063/5.0215065","DOIUrl":"https://doi.org/10.1063/5.0215065","url":null,"abstract":"<p><p>We theoretically demonstrated that helical-photon-dressed states determine the rotational directions of the π-electrons of aromatic ring molecules formed by a circularly polarized or an elliptically polarized laser. This theory was verified using a minimal three-electronic-state model under the frozen nuclei condition. The model consists of the ground state and either a doubly degenerate electronic excited state or two quasi-degenerate excited states. Three helical-photon-dressed states were derived by solving the time-dependent Schrödinger equation within the semi-classical treatment of light-molecule interactions and rotating wave approximation. The angular momenta of the two helical-photon-dressed states represent the classical rotational direction, and that of the remaining state represents the opposite rotation, that is, non-classical rotation. Classical rotation means that π-electrons have the same rotational direction as that of a given helical electric field vector and obeys the classical equations of motion. Non-classical rotation indicates that the rotational direction is opposite to that of the helical electric field vector. Non-classical rotation is forbidden in an aromatic ring molecule with high symmetry formed by a circularly polarized laser but is allowed in a low symmetric aromatic ring molecule. The sum of the angular momenta of the three dressed states is zero. This is called the sum law for the angular momentum components in this paper. Benzene (D6h) and toluene (CS) were adopted as typical aromatic ring molecules of high and low symmetries, respectively. Finally, considering the effects of nuclear vibrations in the adiabatic approximation, an expression for the π-electron angular momentum was derived and applied to toluene.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142681913","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
Second harmonic generation null angle polarization analysis for determining interfacial potential at charged interfaces. 用于确定带电界面的界面电势的二次谐波发生空角极化分析。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0231408
Celestine C Egemba, Paul E Ohno
{"title":"Second harmonic generation null angle polarization analysis for determining interfacial potential at charged interfaces.","authors":"Celestine C Egemba, Paul E Ohno","doi":"10.1063/5.0231408","DOIUrl":"https://doi.org/10.1063/5.0231408","url":null,"abstract":"<p><p>Methods of quantifying the electrostatics of charged interfaces are important in a range of research areas. The surface-selective nonlinear optical technique second harmonic generation (SHG) is a sensitive probe of interfacial electrostatics. Recent work has shown that detection of the SHG phase in addition to its amplitude enables direct quantification of the interfacial potential. However, the experimental challenge of directly detecting the phase interferometrically with sufficient precision and stability has led to the proposal and development of alternative techniques to recover the same information, notably through wavelength scanning or angle scanning, each of which has their own associated experimental challenges. Here, we propose a new polarization-based approach to recover the required phase information, building upon the previously established nonlinear optical null ellipsometry (NONE) technique. Although NONE directly returns only relative phase information between different tensor elements of the second-order susceptibility, it is shown that a symmetry relation that connects the tensor elements of the potential-dependent third-order susceptibility can be used to generate the absolute phase reference required to calculate the interfacial potential. The sensitivity of the technique to potential at varying surface charge densities and ionic strengths is explored by means of simulated data of the silica:water interface. The error associated with the use of the linearized Poisson-Boltzmann approximation is discussed and compared to the error associated with the precision of the measured NONE null angles. Overall, the results suggest that NONE is a promising approach for performing phase-resolved SHG based quantification of interfacial potentials that experimentally requires only the addition of standard polarization optics to the basic single-wavelength, fixed-angle SHG apparatus.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142681942","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 parameter aging and density scaling. 单参数老化和密度缩放。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0234620
Tina Hecksher, Kristine Niss
{"title":"Single parameter aging and density scaling.","authors":"Tina Hecksher, Kristine Niss","doi":"10.1063/5.0234620","DOIUrl":"https://doi.org/10.1063/5.0234620","url":null,"abstract":"<p><p>In a recent paper, Di Lisio et al. [J. Chem. Phys. 159, 064505 (2023)] analyzed a series of temperature down-jumps using the single-parameter aging (SPA) ansatz combined with a specific assumption about density scaling in the out-of-equilibrium system and did not find a good prediction for the largest down-jumps. In this paper, we show that SPA in its original form does work for all their data, including large jumps of ΔT > 20 K. Furthermore, we discuss different approaches to the extension of the density scaling concept to out-of-equilibrium systems.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142675946","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
Is the mechanism of "fast sound" the same in liquids with long-range interactions and disparate mass metallic alloys? 在具有长程相互作用的液体和不同质量的金属合金中,"快速发声 "的机制是否相同?
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0239921
Taras Bryk, Ari Paavo Seitsonen, Giancarlo Ruocco
{"title":"Is the mechanism of \"fast sound\" the same in liquids with long-range interactions and disparate mass metallic alloys?","authors":"Taras Bryk, Ari Paavo Seitsonen, Giancarlo Ruocco","doi":"10.1063/5.0239921","DOIUrl":"10.1063/5.0239921","url":null,"abstract":"<p><p>We present ab initio simulations of a large system of 2400 particles of molten NaCl to investigate the behavior of collective mode dispersion beyond the hydrodynamic regime. In particular, we aim to explain the unusually strong increase in the apparent speed of sound with wave number, which significantly exceeds the typical positive sound dispersion of 10%-25% observed in simple liquids. We compare dispersions of \"bare\" acoustic and optic modes in NaCl with ab initio simulations of other ionic melts such as CuCl and LiBr, metallic liquid alloys such as Pb44Bi56 and Li4Tl, and the regular Lennard-Jones KrAr liquid simulated by classical molecular dynamics. Analytical expressions for the \"bare\" acoustic and optic branches of collective excitations help us to identify the impact of the high-frequency optic branch on the emergence of \"fast sound\" in binary melts. Our findings show that in ionic melts, the high-frequency speed of sound is much larger than in the simple Lennard-Jones liquids and metallic melts, leading to an observed strong viscoelastic increase in the apparent speed of sound-more than double its adiabatic value.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666757","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
Transferable performance of machine learning potentials across graphene-water systems of different sizes: Insights from numerical metrics and physical characteristics. 机器学习潜力在不同尺寸的石墨烯-水系统中的可迁移性能:从数值指标和物理特性中窥见一斑。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0233395
Dongfei Liu, Jianzhong Wu, Diannan Lu
{"title":"Transferable performance of machine learning potentials across graphene-water systems of different sizes: Insights from numerical metrics and physical characteristics.","authors":"Dongfei Liu, Jianzhong Wu, Diannan Lu","doi":"10.1063/5.0233395","DOIUrl":"10.1063/5.0233395","url":null,"abstract":"<p><p>Machine learning potentials (MLPs) are promising for various chemical systems, but their complexity and lack of physical interpretability challenge their broad applicability. This study evaluates the transferability of the deep potential (DP) and neural equivariant interatomic potential (NequIP) models for graphene-water systems using numerical metrics and physical characteristics. We found that the data quality from density functional theory calculations significantly influences MLP predictive accuracy. Prediction errors in transferring systems reveal the particularities of quantum chemical calculations on the heterogeneous graphene-water systems. Even for supercells with non-planar graphene carbon atoms, k-point mesh is necessary to obtain accurate results. In contrast, gamma-point calculations are sufficiently accurate for water molecules. In addition, we performed molecular dynamics (MD) simulations using these two models and compared the physical features such as atomic density profiles, radial distribution functions, and self-diffusion coefficients. It was found that although the NequIP model has higher accuracy than the DP model, the differences in the above physical features between them were not significant. Considering the stochasticity and complexity inherent in simulations, as well as the statistical averaging of physical characteristics, this motivates us to explore the meaning of accurately predicting atomic force in aligning the physical characteristics evolved by MD simulations with the actual physical features.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142667483","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
Structuring in thin films during meniscus-guided deposition. 半月板引导沉积过程中的薄膜结构。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0225995
René de Bruijn, Anton A Darhuber, Jasper J Michels, Paul van der Schoot
{"title":"Structuring in thin films during meniscus-guided deposition.","authors":"René de Bruijn, Anton A Darhuber, Jasper J Michels, Paul van der Schoot","doi":"10.1063/5.0225995","DOIUrl":"10.1063/5.0225995","url":null,"abstract":"<p><p>We theoretically study the evaporation-driven phase separation of a binary fluid mixture in a thin film deposited on a moving substrate, as occurs in meniscus-guided deposition for solution-processed materials. Our focus is on the limit of rapid substrate motion where phase separation takes place far away from the coating device. In this limit, demixing takes place under conditions mimicking those in a stationary film because substrate and film move at the same speed. We account for the hydrodynamic transport of the mixture within the lubrication approximation. In the early stages of demixing, diffusive and evaporative mass transport predominates, consistent with earlier studies on evaporation-driven spinodal decomposition. In the late-stage coarsening of the demixing process, the interplay of solvent evaporation, diffusive, and hydrodynamic mass transport results in several distinct coarsening mechanisms. The effective coarsening rate is dictated by the dominant mass transport mechanism and therefore depends on the material properties, evaporation rate, and time: slow solvent evaporation results in initially diffusive coarsening that for sufficiently strong hydrodynamic transport transitions to hydrodynamic coarsening, whereas rapid solvent evaporation can preempt and suppress hydrodynamic and diffusive coarsening. We identify a novel hydrodynamic coarsening regime for off-critical mixtures, arising from the interaction of the interfaces between solute-rich and solute-poor regions in the film with the solution-gas interface. This interaction induces a directional motion of solute-rich droplets along gradients in the film thickness, from regions where the film is relatively thick to where it is thinner. The solute-rich domains subsequently accumulate and coalesce in the thinner regions.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142667543","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
Erratum: "Stress auto-correlation tensor in glass-forming isothermal fluids: From viscous to elastic response" [J. Chem. Phys. 149, 084502 (2018)]. 更正:"玻璃态等温流体中的应力自相关张量:从粘性响应到弹性响应" [J. Chem. Phys. 149, 084502 (2018)]。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0245831
M Maier, A Zippelius, M Fuchs
{"title":"Erratum: \"Stress auto-correlation tensor in glass-forming isothermal fluids: From viscous to elastic response\" [J. Chem. Phys. 149, 084502 (2018)].","authors":"M Maier, A Zippelius, M Fuchs","doi":"10.1063/5.0245831","DOIUrl":"https://doi.org/10.1063/5.0245831","url":null,"abstract":"","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142681909","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 and bonding properties of Ta2Cn-/0 (n = 1-7) clusters: Size-selected anion photoelectron spectroscopy and theoretical calculations. Ta2Cn-/0(n = 1-7)团簇的结构和成键特性:尺寸选择阴离子光电子能谱和理论计算。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0233496
Chao-Jiang Zhang, Hong-Guang Xu, Xi-Ling Xu, Wei-Jun Zheng
{"title":"Structural and bonding properties of Ta2Cn-/0 (n = 1-7) clusters: Size-selected anion photoelectron spectroscopy and theoretical calculations.","authors":"Chao-Jiang Zhang, Hong-Guang Xu, Xi-Ling Xu, Wei-Jun Zheng","doi":"10.1063/5.0233496","DOIUrl":"https://doi.org/10.1063/5.0233496","url":null,"abstract":"<p><p>The structures and chemical bond evolution of ditantalum doped carbon clusters Ta2Cn-/0 (n = 1-7) were studied via size-selected anion photoelectron spectroscopy and theoretical calculations. It is found that Ta2C-/0 has a triangular structure and Ta2C2-/0 has a quasi-rhombus structure with C2v symmetry. Ta2C3- has a quasi-planar structure with a carbon atom and a C2 unit interacting with two tantalum atoms, and the lowest-energy isomer of neutral Ta2C3 has a triangular bipyramid structure with three carbon atoms around the Ta2 unit. Ta2C4-/0 has two C2 units connected with the Ta2 unit in parallel. Two isomers of Ta2C5- are observed, where both isomers have one carbon atom and two C2 units bound to the Ta2 unit in different ways. The most stable structure of neutral Ta2C5 has one carbon atom added on top of the Ta2C4 cluster. The most stable structures of Ta2C6-7-/0 can be viewed as a C2 unit and a C3 unit capping a butterfly like Ta2C4 structure, respectively. Molecular orbital analysis shows that neutral Ta2C3 has a large gap between its highest occupied molecular orbital and lowest unoccupied molecular orbital. Chemical bonding analysis reveals that the Ta-Ta interactions in Ta2Cn-/0 (n = 1-7) clusters are slightly weaker than the Ta-Ta interaction in bare Ta2 due to the participation in forming multicenter bonds.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142675947","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
Hybrid neMD/MC lipid swapping algorithm to equilibrate membrane simulation with thermodynamic reservoir. 混合 neMD/MC 脂质交换算法,使膜模拟与热力学库达到平衡。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0230226
Florence Szczepaniak, François Dehez, Benoît Roux
{"title":"Hybrid neMD/MC lipid swapping algorithm to equilibrate membrane simulation with thermodynamic reservoir.","authors":"Florence Szczepaniak, François Dehez, Benoît Roux","doi":"10.1063/5.0230226","DOIUrl":"10.1063/5.0230226","url":null,"abstract":"<p><p>Molecular dynamics (MD) simulations based on detailed all-atom models offer a powerful approach to study the structure and dynamics of biological membranes. However, the complexity of biological membranes in terms of chemical diversity presents an outstanding challenge. Particularly, difficulties are encountered when a given lipid type is present at very low abundance. While considering a very large simulation system with a small number of the low abundance lipid may offer a practical solution in some cases, resorting to increasingly large system rapidly becomes computationally costly and impractical. More fundamentally, an additional issue may be encountered if the low abundance lipid displays a high affinity for some protein in the simulation system. What is needed is to treat the simulation box as an open system in which the number of lipids can naturally fluctuate, as in the Grand Canonical Monte Carlo (MC) algorithm. However, this approach, in which a whole lipid molecule needs to be inserted or annihilated, is essentially impractical in the context of an all-atom simulation. To enforce equilibrium between a simulated system and an infinite surrounding bath, we propose a hybrid non-equilibrium (neMD)-MC algorithm, in which a randomly chosen lipid molecule in the simulated system is swapped with a lipid picked in a separate system standing as a thermodynamic \"reservoir\" with the desired mole fraction for all lipid components. The neMD/MC algorithm consists in driving the system via short non-equilibrium trajectories to generate a new state of the system that are subsequently accepted or rejected via a Metropolis MC step. The probability of exchanges in the context of an infinite reservoir with the desired mole fraction for all lipid components is derived and tested with a few illustrative systems for phosphatidylcholine and phosphatidylglycerol lipid mixtures.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142647285","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
Hamiltonian non-Hermicity: Accurate dynamics with the multiple Davydov D2Ansätze. 哈密顿非恒定性:多重达维多夫 D2Ansätze 的精确动力学。
IF 3.1 2区 化学
Journal of Chemical Physics Pub Date : 2024-11-21 DOI: 10.1063/5.0243861
Lixing Zhang, Kaijun Shen, Yiying Yan, Kewei Sun, Maxim F Gelin, Yang Zhao
{"title":"Hamiltonian non-Hermicity: Accurate dynamics with the multiple Davydov D2Ansätze.","authors":"Lixing Zhang, Kaijun Shen, Yiying Yan, Kewei Sun, Maxim F Gelin, Yang Zhao","doi":"10.1063/5.0243861","DOIUrl":"10.1063/5.0243861","url":null,"abstract":"<p><p>We examine the applicability of the numerically accurate method of time dependent variation with multiple Davydov Ansätze (mDA) to non-Hermitian systems. As illustrative examples, three systems of interest have been studied, a non-Hermitian system of dissipative Landau-Zener transitions, a non-Hermitian multimode Jaynes-Cummings model, and a dissipative Holstein-Tavis-Cummings model, all of which are shown to be effectively described by the mDA method. Our findings highlight the versatility of the mDA as a powerful numerical tool for investigating complex many-body non-Hermitian systems, which can be extended to explore diverse phenomena such as skin effects, excited-state dynamics, and spectral topology in the non-Hermitian field.</p>","PeriodicalId":15313,"journal":{"name":"Journal of Chemical Physics","volume":"161 19","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142668169","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
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