时依赖的相对论二组分方程运动耦合簇方法用于开放壳层系统：TD-EA/IP-EOMCC
Time-Dependent Relativistic Two-Component Equation-of-Motion Coupled-Cluster for Open-Shell Systems: TD-EA/IP-EOMCC
AI总结：
本文提出了一种基于虚时间/实时间时间依赖方法的相对论二组分方程运动耦合簇方法，用于计算开放壳层系统的线性吸收光谱，并探讨了低能态对初始态传播的影响。
摘要：
我们提出了一种结合虚时间/实时间时间依赖（TD）方法，用于在电子附加（EA）和电离势（IP）方程运动耦合簇（EOMCC）理论水平上评估开放壳层系统的线性吸收光谱，并在精确的二组分相对论框架内进行。吸收线形由电偶极子自相关函数的傅里叶变换给出，该函数来源于实时间模拟。近似生成最低能量EA-和IP-EOMCC本征态，这些本征态是实时间模拟的初始态，是通过在虚时间中传播Koopman EA/IP态得到的。TD-EA/IP-EOMCC线性吸收光谱对开放壳层原子系统（Na、K、Rb、F、Cl和Br）的吸收光谱能很好地重现标准TD-EA/IP过程在频域中的结果。我们发现，低能态与Koopman行列式有非可忽略的重叠，影响了获得产生正确绝对能量和峰值高度强度的初始态所需的虚时间传播长度。
英文摘要：
We present a combined imaginary-time/real-time time-dependent (TD) approach for evaluating linear absorption spectra of open-shell systems at the electron attachment (EA) and ionization potential (IP) equation-of-motion coupled-cluster (EOMCC) levels of theory and within the exact two-component relativistic framework. The absorption lineshape is given by the Fourier transform of the electric dipole autocorrelation function, which is obtained from a real-time simulation. Approximations of the lowest-energy EA- and IP-EOMCC eigenstates, which are required as initial states for the real-time simulation, are generated by propagating a Koopman EA/IP state in imaginary time. TD-EA/IP-EOMCC linear absorption spectra of open-shell atomic systems (Na, K, Rb, F, Cl, and Br) closely reproduce those obtained from standard TD-EA/IP procedures carried out in the frequency domain. We find that the existence of low-lying states with non-negligible overlap with the Koopman determinant impacts the length of the imaginary-time propagation required to obtain an initial state that produces correct absolute energies and peak height intensities in spectra extracted from the subsequent real-time TD-EA/IP-EOMCC calculations.
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