Electron Dynamics Induced by Circularly Polarized Laser Pulses in Im-3m H3S in the Superconducting Pressure Regime

IF 4.8 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Journal of Computational Chemistry Pub Date : 2025-07-04 DOI:10.1002/jcc.70173

Lizhi Tang, Genwei Hong, Tianlv Xu, Herbert Früchtl, Tanja van Mourik, Steven R. Kirk, Samantha Jenkins

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Abstract

We investigated crystalline Im-3m H₃S at 200 GPa, a pressure regime where H₃S is generally considered to be an exotic superconductor. Simulated circularly polarized 10 femtosecond (fs) laser pulses were applied and we quantified the effects on the electron dynamics during the application of “pump” and candidate “probe” laser pulses to discover optimal “probe” laser pulses. This is undertaken for the first application of Next Generation Quantum Theory of Atoms in Molecules (NG-QTAIM) using the Hessian of the “spin-up” and “spin-down” contributions to the total electronic charge density ρ(r). The optimal “probe” pulse was found to possess a peak electric field E = 10.0 × 10⁻⁴ a.u. compared with the “pump” pulse of E = 200.0 × 10⁻⁴ a.u. Separately considering the spin-up and spin-down contributions doubles the values of the chirality-helicity C_helicity function relative to that of the total charge density contribution for the H-H bonding for the application of the “pump” laser pulse. Within the NG-QTAIM interpretation, a combination of highly responsive and coherent behaviors is associated with superconductivity. These behaviors were discovered from the very high values of the C_helicity function, near-linear scaling of the bond-flexing F and bond-chirality C values with peak E-field and all instances of the H-H bonding possessing R electronic chirality assignments. The “pump” pulse was found to magnify the effects associated with superconductivity within the NG-QTAIM interpretation. Future applications are discussed including chiral spin selective phenomena and exotic high temperature superconductivity where phonons do not play a significant role.

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超导压力下圆偏振激光脉冲在Im-3m H3S中诱导的电子动力学

我们在200 GPa的压力下研究了晶体Im-3m H3S，在这种压力下，H3S通常被认为是一种外来超导体。应用模拟的圆偏振10飞秒（fs）激光脉冲，量化“泵浦”和候选“探针”激光脉冲对电子动力学的影响，以寻找最佳的“探针”激光脉冲。这是下一代分子原子量子理论（NG-QTAIM）的第一次应用，使用“自旋向上”和“自旋向下”对总电子电荷密度ρ(r)的贡献。发现最佳“探针”脉冲具有峰值电场E = 10.0 × 10−4 a.u。与E = 200.0 × 10−4 a.u的“泵”脉冲进行比较。单独考虑自旋向上和自旋向下的贡献，相对于“泵浦”激光脉冲应用的H-H键的总电荷密度贡献，手性-螺旋度Chelicity函数的值翻了一番。在NG-QTAIM解释中，高响应和相干行为的组合与超导性有关。这些行为是通过螯合函数的非常高的值、键弯曲F和键手性C值的近线性缩放以及所有具有R电子手性赋值的H-H键的实例发现的。在NG-QTAIM解释中，发现“泵”脉冲放大了与超导相关的效应。讨论了未来的应用，包括手性自旋选择现象和外来高温超导，声子不发挥重要作用。

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来源期刊

Journal of Computational Chemistry 化学-化学综合

CiteScore

6.60

自引率

3.30%

发文量

247

审稿时长

1.7 months

期刊介绍： This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.