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Generalized spin σ-SCF method
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DOI：10.1063/5.0178264.png)
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摘要
En 中文
We introduce a generalization of the sigma-SCF method to approximate noncollinear spin ground and excited single-reference electronic states by minimizing the Hamiltonian variance. The new method is based on the sigma-SCF method, originally proposed by Ye et al. [J. Chem. Phys. 147, 214104 (2017)], and provides a prescription to determine ground and excited noncollinear spin states on an equal footing. Our implementation was carried out utilizing an initial simulated annealing stage followed by a mean-field iterative self-consistent approach to simplify the cumbersome search introduced by generalizing the spin degrees of freedom. The simulated annealing stage ensures a broad exploration of the Hilbert space spanned by the generalized spin single-reference states with random complex element-wise rotations of the generalized density matrix elements in the simulated annealing stage. The mean-field iterative self-consistent stage employs an effective Fockian derived from the variance, which is utilized to converge tightly to the solutions. This process helps us to easily find complex spin structures, avoiding manipulating the initial guess. As proof-of-concept tests, we present results for H-n (n = 3-7) planar rings and polyhedral clusters with geometrical spin frustration. We show that most of these systems have noncollinear spin excited states that can be interpreted in terms of geometric spin frustration. These states are not directly targeted by energy minimization methods, which are meant to converge to the ground state. This stresses the capability of the sigma-SCF methodology to find approximate noncollinear spin structures as mean-field excited states.
Keyword:
MOLECULAR SCHRODINGER-EQUATION
DENSITY-FUNCTIONAL THEORY
LOCAL-ENERGY METHOD
EXCITED-STATES
CONFIGURATION-INTERACTION
ELECTRONIC-ENERGY
WAVE-FUNCTIONS
GROUND-STATE
SYMMETRY
MATRIX
期刊
IF:
3.1
论文数:
7.2W
被引数:
23.2W
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分享收藏Variational calculations of excited states via direct optimization of the orbitals in DFT通过直接优化DFT中的轨道对激发态进行变分计算.png)
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