论文标题

在较强的均匀磁场中

Time-Dependent Nuclear-Electronic Orbital Hartree-Fock Theory in a Strong Uniform Magnetic Field

论文作者

Culpitt, Tanner, Peters, Laurens D. M., Tellgren, Erik I., Helgaker, Trygve

论文摘要

在存在强磁场的情况下,出生的苯二聚体(BO)近似比没有磁场的准确性较差。这是由于电子结构对田地的复杂且不可预测的响应,尤其是在混合体制中$ b \ b_0 = 2.35 \ times 10^5 \,$ t。因此,希望探索磁场中的非BO方法。在这项工作中,核电子轨道(NEO)方法用于在存在强磁场的情况下研究质子振动激发能。 NEO广义的Hartree-fock理论和时间依赖性的Hartree-fock理论得出了和实施,这考虑了所有术语,这是由于磁场中分子系统的非扰动处理而导致的所有术语。将HCN和FHF $^ - $带有夹紧重核的NEO结果与二次特征值问题(QEP)进行了比较。每个分子由于氢而具有三种半古典模式 - 在没有田间和一个拉伸模式的情况下,它们退化了两种。发现NEO -TDHF模型的性能很好 - 特别是它会自动捕获电子对细胞核的筛选效果,这些效果是通过进液模式的能量差来量化的。

The Born-Oppenheimer (BO) approximation is less accurate in the presence of a strong magnetic field than in the absence of a field. This is due to the complicated and unpredictable response of electronic structure to the field, especially in the mixed regime $B \approx B_0 = 2.35 \times 10^5\,$T. Therefore, it is desirable to explore non-BO methods in magnetic fields. In this work, the nuclear-electronic orbital (NEO) method is employed to study protonic vibrational excitation energies in the presence of a strong magnetic field. NEO Generalized Hartree-Fock theory and time-dependent Hartree-Fock theory are derived and implemented, accounting for all terms that result as a consequence of the nonperturbative treatment of molecular systems in a magnetic field. The NEO results for HCN and FHF$^-$ with clamped heavy nuclei are compared against the quadratic eigenvalue problem (QEP). Each molecule has three semi-classical modes owing to the hydrogen - two precession modes that are degenerate in the absence of a field and one stretching mode. The NEO-TDHF model is found to perform well - in particular it automatically captures the screening effects of the electrons on the nuclei, which are quantified through the difference in energy of the precession modes.

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