We perform ab initio calculations of high-harmonic spectroscopy (HHS) of two-center interference phenomena in oriented carbon-dichalcogen molecules, using time-dependent density functional theory (TDDFT). We show that by resolving the harmonic response into contributions from individual Kohn-Sham orbitals, we can extract target-specific characteristics for both the spectral amplitude and phase. We also discuss that this extraction is predicated on a careful analysis and normalization of the harmonic spectrum. Finally, we present field-free scattering calculations that mimic the recollision step in high-order-harmonic generation and allow the calculation of recombination dipole matrix elements without explicitly calculating the scattering states of a molecule. We show that the orbital-resolved TDDFT HHS results and results based on our field-free scattering calculations are in very good agreement with each other.

中文翻译：

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线性三原子分子中双中心干涉的轨道分辨计算

我们从头开始使用时间相关密度泛函理论 (TDDFT) 计算定向碳二硫属元素分子中双中心干涉现象的高谐波光谱 (HHS)。我们表明，通过将谐波响应分解为来自单个 Kohn-Sham 轨道的贡献，我们可以提取光谱幅度和相位的特定目标特征。我们还讨论了这种提取基于对谐波频谱的仔细分析和归一化。最后，我们提出了模拟高阶谐波生成中的再碰撞步骤的无场散射计算，并允许在不明确计算分子散射状态的情况下计算复合偶极子矩阵元素。