论文标题
水分子的快速电离轨道中的非单调直流变速
Non-monotonic dc Stark shifts in the rapidly ionizing orbitals of the water molecule
论文作者
论文摘要
我们扩展了一个先前开发的水分子共振模型。该方法使用球形谐波采用单粒轨道的部分波扩展。为了找到共振位置和衰减速率，我们使用了外部复合体缩放方法，该方法涉及将径向变量分析到复杂平面的分析延续，并产生非富甲米的哈密顿矩阵。特征值的真实部分提供了共振位置（因此是鲜明的变化），而虚部$-γ/2 $与衰减率$γ$，即，全宽度的全宽度为Breit-Wigner共振的最大最大。我们专注于三个最外面的（价）轨道，因为它们主导了电离过程。我们发现，对于针对三个笛卡尔坐标中的力，最快的电离轨道总是显示出非单调的鲜明变化。对于沿分子轴的字段，我们还将结果比较的结果是所包括的球形谐波数量（$ \ ell _ {\ max} = 3,4 $）。我们还将结果与Hartree-fock和耦合群集方法的总分子stark偏移进行了比较。
We extend a previously developed model for the Stark resonances of the water molecule. The method employs a partial-wave expansion of the single-particle orbitals using spherical harmonics. To find the resonance positions and decay rates, we use the exterior complex scaling approach which involves the analytic continuation of the radial variable into the complex plane and yields a non-hermitian Hamiltonian matrix. The real part of the eigenvalues provides the resonance positions (and thus the Stark shifts), while the imaginary parts $-Γ/2$ are related to the decay rates $Γ$, i.e., the full-widths at half-maximum of the Breit-Wigner resonances. We focus on the three outermost (valence) orbitals, as they are dominating the ionization process. We find that for forces directed in the three Cartesian co-ordinates, the fastest ionizing orbital always displays a non-monotonic Stark shift. For the case of fields along the molecular axis we also compare results as a function of the number of spherical harmonics included ($\ell_{\max}=3,4$). We also compare our results to the total molecular Stark shifts for the Hartree-Fock and coupled cluster methods.
