Dynamic mediation 4f electron configurations in cerium monosulfide via temperature-dependent many-body effects

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry Pub Date : 2025-08-09 DOI:10.1016/j.comptc.2025.115424

Ru-song Li , Rong Guo , Zheng Xie , Jin-tao Wang , Fei Wang

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Abstract

This study investigate temperature-dependent electronic correlations and 4f electron dynamics in cerium monosulfide (CeS) by using a combination of density functional theory (DFT) and dynamical mean-field theory (DMFT). The spin-orbit-split 4f states exhibit a dichotomy: the j = 5/2 manifold transitions from strong to weak correlations with increasing temperature (116–800 K), displaying metallic behavior, while the j = 7/2 states remain insulating with intermediate-to-strong correlations. Localized 4f occupancy (1.060–1.071) coexists with minor valence fluctuations due to slight hybridization between 4f and itinerant spd electrons. Spectral functions near the Fermi level reveal Kondo quasiparticle resonances, Hubbard bands, and temperature-driven spectral weight redistribution, emphasizing spin-orbit coupling and orbital-selective correlations as key modulation for the electronic structure.

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温度相关多体效应对单硫化铈中4f电子构型的动态中介作用

本研究结合密度泛函理论（DFT）和动力学平均场理论（DMFT）研究了单硫化铈（CeS）中温度相关电子和4f电子动力学。自旋轨道分裂的4f态表现出两分法：随着温度的升高（116-800 K）， j = 5/2流形从强相关转变为弱相关，表现出金属行为，而j = 7/2态保持绝缘，具有中强相关。局域化的4f占有（1.060-1.071）与较小的价涨落共存，这是由于4f和流动的spd电子之间存在轻微的杂化。费米能级附近的谱函数揭示了近藤准粒子共振、哈伯德带和温度驱动的谱重分布，强调了自旋轨道耦合和轨道选择相关性是电子结构的关键调制。

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来源期刊

Computational and Theoretical Chemistry CHEMISTRY, PHYSICAL-

CiteScore

4.20

自引率

10.70%

发文量

331

审稿时长

31 days

期刊介绍： Computational and Theoretical Chemistry publishes high quality, original reports of significance in computational and theoretical chemistry including those that deal with problems of structure, properties, energetics, weak interactions, reaction mechanisms, catalysis, and reaction rates involving atoms, molecules, clusters, surfaces, and bulk matter.