Arrow diagram method based on overlapping electronic groups: corrections to the linked AD theorem
Yu Wang, Lev Kantorovich
Abstract
Arrow diagram (AD) method (L. Kantorovich and B. Zapol, J. Chem. Phys. 96, 8420 (1992); ibid, 8427) provides a convenient means of systematic calculation of arbitrary matrix elements, <Ψ|O|Ψ>, of symmetrical operators, O, in quantum chemistry when the total system wavefunction Ψ is represented as an antisymmetrised product of overlapping many-electron group functions, ΦA, corresponding to each part (group) A of the system: Ψ=AΠAΦA. For extended (e.g. infinite) systems the calculation is somewhat difficult, however, as mean values of the operators require that each term of the diagram expansion is to be divided by the normalisation integral S=<Ψ|Ψ>, which is given by an AD expansion as well. A linked AD theorem suggested previously (L. Kantorovich, Int. J. Quant. Chem. 76, 511 (2000)) to deal with this problem is reexamined in this paper using a simple Hartree-Fock problem of a one-dimensional ring of infinite size which is found to be analytically solvable. We find that corrections to the linked AD theorem are necessary in a general case of a finite overlap between different electronic groups. A general method of constructing these corrections in a form of a power series expansion with respect to overlap is suggested. It is illustrated on the ring model system.
Create a lesson
Related papers
Accurate representation of the continuum orbital in a Gaussian basis set: application to Auger decay rates
Dibyendu Mahato, Saikat Roy, Wojciech Skomorowski
Bicarbonate/carbonic acid equilibria in aqueous solutions: Conformational Dynamics, Ion-Pair Speciation, and Free Energy Landscapes from Ab Initio Molecular Dynamics and Metadynamics
Prabhat Prakash, Karnamohit Ranka, Frances A. Houle et al.
Isothermal-Isobaric Molecular Dynamics with a Foundation Interatomic Potential in LAMMPS across NVIDIA and Intel GPUs
Xiaoli Yan, Eliu Huerta
Shadow Molecular Dynamics for General Nonlinear Flexible-Charge Models
Jos Thomas, Anthony P. Baldo, Rae A. Corrigan Grove et al.
FACTO: fast atom-centered tensor operator for accurate and efficient foundational machine-learned interatomic potentials
Siyuan Liu, Chang Han, Sheng Gong et al.
Relativistic Kohn--Sham Theory of Paramagnetic Magnetic-Resonance Properties
Christof Holzer, Yannick J. Franzke