Unitary coupled-cluster based self-consistent polarization propagator theory: a quadratic unitary coupled-cluster singles and doubles scheme
Fuente:
arXiv
Guardado en:
| Autores principales: | , |
|---|---|
| Formato: | Preprint |
| Publicado: |
2021
|
| Materias: | |
| Acceso en línea: | |
| Etiquetas: |
Agregar Etiqueta
Sin Etiquetas, Sea el primero en etiquetar este registro!
|
| _version_ | 1866916291627974656 |
|---|---|
| author | Liu, Junzi Cheng, Lan |
| author_facet | Liu, Junzi Cheng, Lan |
| contents | The development of a quadratic unitary coupled-cluster singles and doubles (qUCCSD) based self-consistent polarization propagator method is reported. We present a simple strategy for truncating the commutator expansion of the UCC transformed Hamiltonian $\bar{H}$. The qUCCSD method for the electronic ground-state includes up to double commutators for the amplitude equations and up to cubic commutators for the energy expression. The qUCCSD excited-state eigenvalue equations include up to double commutators for the singles-singles block of $\bar{H}$, single commutators for the singles-doubles and doubles-singles blocks, and the bare Hamiltonian for the doubles-doubles block. Benchmark qUCCSD calculations of the ground-state properties and excitation energies for representative molecules demonstrate significant improvement of the accuracy and robustness over the previous UCC3 scheme derived using Møller-Plesset perturbation theory. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2107_01099 |
| institution | arXiv |
| publishDate | 2021 |
| record_format | arxiv |
| spellingShingle | Unitary coupled-cluster based self-consistent polarization propagator theory: a quadratic unitary coupled-cluster singles and doubles scheme Liu, Junzi Cheng, Lan Chemical Physics The development of a quadratic unitary coupled-cluster singles and doubles (qUCCSD) based self-consistent polarization propagator method is reported. We present a simple strategy for truncating the commutator expansion of the UCC transformed Hamiltonian $\bar{H}$. The qUCCSD method for the electronic ground-state includes up to double commutators for the amplitude equations and up to cubic commutators for the energy expression. The qUCCSD excited-state eigenvalue equations include up to double commutators for the singles-singles block of $\bar{H}$, single commutators for the singles-doubles and doubles-singles blocks, and the bare Hamiltonian for the doubles-doubles block. Benchmark qUCCSD calculations of the ground-state properties and excitation energies for representative molecules demonstrate significant improvement of the accuracy and robustness over the previous UCC3 scheme derived using Møller-Plesset perturbation theory. |
| title | Unitary coupled-cluster based self-consistent polarization propagator theory: a quadratic unitary coupled-cluster singles and doubles scheme |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2107.01099 |