具有频率相关二阶Bethe-Salpeter关联核的距离分离含时密度泛函理论
Range-separated time-dependent density-functional theory with a frequency-dependent second-order Bethe-Salpeter correlation kernel
摘要：
我们提出了一个距离分离的线性响应时间相关的密度泛函理论（TDDFT），它结合了密度泛函近似的短程响应内核和频率相关的二阶Bethe-Salpeter近似的长程响应内核。该方法超越了线性响应TDDFT中常用的绝热近似，旨在提高分子体系电子激发能的计算精度。利用多体格林函数理论，详细推导了频率相关的二阶Bethe-Salpeter相关核。初步测试的距离分离TDDFT方法的计算激发能的He和Be原子和小分子（H2，N2，CO2，H2 CO，和C2 H4）。结果表明，添加长程二阶Bethe-Salpeter相关核总体上略微改善了激发能。
英文摘要：
We present a range-separated linear-response time-dependent density-functional theory (TDDFT) which combines a density-functional approximation for the short-range response kernel and a frequency-dependent second-order Bethe-Salpeter approximation for the long-range response kernel. This approach goes beyond the adiabatic approximation usually used in linear-response TDDFT and aims at improving the accuracy of calculations of electronic excitation energies of molecular systems. A detailed derivation of the frequency-dependent second-order Bethe-Salpeter correlation kernel is given using many-body Green-function theory. Preliminary tests of this range-separated TDDFT method are presented for the calculation of excitation energies of the He and Be atoms and small molecules (H2, N2, CO2, H2CO, and C2H4). The results suggest that the addition of the long-range second-order Bethe-Salpeter correlation kernel overall slightly improves the excitation energies.
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