Spin-density calculation via the graphical unitary group approach
Spin-density calculation via the graphical unitary group approach
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DOI：
10.1080/00268976.2022.2091049
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发表时间：
2022-06
影响因子：
1.7
通讯作者：
R. F. Spada;Maurício P. Franco;Reed Nieman;A. Aquino;R. Shepard;F. Plasser;H. Lischka
中科院分区：
文献类型：
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作者：
R. F. Spada;Maurício P. Franco;Reed Nieman;A. Aquino;R. Shepard;F. Plasser;H. Lischka
在这项工作中，我们讨论了计算的自旋密度矩阵的基本自旋原则，在哥伦布计划系统采用图形酉群方法（GUGA）。首先，自旋密度矩阵的一般方程推导出的一个和两个粒子的约化密度矩阵，数量是自旋无关的，很容易在GUGA形式主义。接下来，讨论使用Shavitt回路值的该方程的评估。最后，空间分辨的自旋密度矩阵，自旋分布，计算的phenalenyl自由基和结构产生的杂原子与单和双取代。自旋密度的物理意义沿着与它的计算描述，使用各种方法进行了讨论，特别强调的负贡献的自旋密度和它们的量化通过自旋促进指数。图形摘要
In this work we discuss the calculation of the spin-density matrix from fundamental spin principles as implemented in the COLUMBUS Program System employing the graphical unitary group approach (GUGA). First, a general equation for the spin-density matrix is derived in terms of the one-and two-particle reduced density matrices, quantities that are spin-independent and readily available within the GUGA formalism. Next, the evaluation of this equation using the Shavitt loop values is discussed. Finally, the spatially resolved counterpart of the spin-density matrix, the spin distribution, is calculated for the phenalenyl radical and structures produced by heteroatoms with mono- and di-substitutions. The physical meaning of the spin-density along with its computational description using various methods is discussed putting special emphasis on negative contributions to the spin-density and their quantification via a spin-promotion index. GRAPHICAL ABSTRACT