论文标题
有效实施带电激发的单参照代数图构造理论：对速度自由基和DNA碱基对的应用
Efficient implementation of the single-reference algebraic diagrammatic construction theory for charged excitations: Applications to the TEMPO radical and DNA base pairs
论文作者
论文摘要
我们介绍了电子附着（EA）和电离（IP）能量和光谱的二阶和三阶单参考代数构造理论的有效实现（EA/IP-ADC（N），n = 2，3）。我们的新EA/IP-ADC程序具有用于封闭系统的旋转适应性，密度拟合，用于有效处理两电子积分积分张量，以及量张量收缩的矢量和平行实现。我们通过应用EA/IP-ADC（n）（n = 2，3）方法来计算Tempo自由基的光电子光谱以及Tempo的垂直和绝热电子亲属和两个DNA碱基对（圭亚那 - 基因胺和腺嘌呤 - 腺苷和腺苷），通过应用EA/IP-ADC（n = 2，3）方法来证明我们有效实现的能力。发现使用大型扩散基集计算出的光谱和电子亲和力，最多可与实验和理论模拟的最佳可用结果相吻合。
We present an efficient implementation of the second- and third-order single-reference algebraic diagrammatic construction theory for electron attachment (EA) and ionization (IP) energies and spectra (EA/IP-ADC(n), n = 2, 3). Our new EA/IP-ADC program features spin adaptation for closed-shell systems, density fitting for efficient handling of the two-electron integral tensors, as well as vectorized and parallel implementation of tensor contractions. We demonstrate capabilities of our efficient implementation by applying the EA/IP-ADC(n) (n = 2, 3) methods to compute the photoelectron spectrum of the TEMPO radical, as well as the vertical and adiabatic electron affinities of TEMPO and two DNA base pairs (guanine-cytosine and adenine-thymine). The spectra and electron affinities computed using large diffuse basis sets with up to 1028 molecular orbitals are found to be in a good agreement with the best available results from the experiment and theoretical simulations.
