### Abstract

The electron-hole explicitly correlated Hartree-Fock method (eh-XCHF) is presented as a general strategy for investigation of electron-hole correlation and computation of electron-hole recombination probability. The eh-XCHF method is a variational method which uses explicitly correlated wavefunction that depends on the electron-hole inter-particle distances. It is shown that the explicitly correlated ansatz provides a systematic route to variationally minimize the total energy. The parabolic quantum dot is used as the benchmark system and the eh-XCHF method is used for computation of the ground state energy and electron-hole recombination probability. The results are compared to Hartree-Fock and explicitly correlated full configuration interaction (R12-FCI) calculations. The results indicate that an accurate description of the electron-hole wavefunction at short electron-hole inter-particle distances is crucial for qualitative description of the electron-hole recombination probability. The eh-XCHF method successfully addresses this issue and comparison of eh-XCHF calculations with R12-FCI shows good agreement. The quality of the mean field approximation for electron-hole system is also investigated by comparing HF and R12-FCI energies for electron-electron and electron-hole systems. It was found that performance of the mean field approximation is worse for the electron-hole system as compared to the corresponding electron-electron system.

Original language | English (US) |
---|---|

Article number | 124105 |

Journal | The Journal of Chemical Physics |

Volume | 136 |

Issue number | 12 |

DOIs | |

State | Published - Mar 28 2012 |

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### ASJC Scopus subject areas

- Physics and Astronomy(all)
- Physical and Theoretical Chemistry

### Cite this

*The Journal of Chemical Physics*,

*136*(12), [124105]. https://doi.org/10.1063/1.3693765

**Calculation of electron-hole recombination probability using explicitly correlated Hartree-Fock method.** / Elward, Jennifer M.; Thallinger, Barbara; Chakraborty, Arindam.

Research output: Contribution to journal › Article

*The Journal of Chemical Physics*, vol. 136, no. 12, 124105. https://doi.org/10.1063/1.3693765

}

TY - JOUR

T1 - Calculation of electron-hole recombination probability using explicitly correlated Hartree-Fock method

AU - Elward, Jennifer M.

AU - Thallinger, Barbara

AU - Chakraborty, Arindam

PY - 2012/3/28

Y1 - 2012/3/28

N2 - The electron-hole explicitly correlated Hartree-Fock method (eh-XCHF) is presented as a general strategy for investigation of electron-hole correlation and computation of electron-hole recombination probability. The eh-XCHF method is a variational method which uses explicitly correlated wavefunction that depends on the electron-hole inter-particle distances. It is shown that the explicitly correlated ansatz provides a systematic route to variationally minimize the total energy. The parabolic quantum dot is used as the benchmark system and the eh-XCHF method is used for computation of the ground state energy and electron-hole recombination probability. The results are compared to Hartree-Fock and explicitly correlated full configuration interaction (R12-FCI) calculations. The results indicate that an accurate description of the electron-hole wavefunction at short electron-hole inter-particle distances is crucial for qualitative description of the electron-hole recombination probability. The eh-XCHF method successfully addresses this issue and comparison of eh-XCHF calculations with R12-FCI shows good agreement. The quality of the mean field approximation for electron-hole system is also investigated by comparing HF and R12-FCI energies for electron-electron and electron-hole systems. It was found that performance of the mean field approximation is worse for the electron-hole system as compared to the corresponding electron-electron system.

AB - The electron-hole explicitly correlated Hartree-Fock method (eh-XCHF) is presented as a general strategy for investigation of electron-hole correlation and computation of electron-hole recombination probability. The eh-XCHF method is a variational method which uses explicitly correlated wavefunction that depends on the electron-hole inter-particle distances. It is shown that the explicitly correlated ansatz provides a systematic route to variationally minimize the total energy. The parabolic quantum dot is used as the benchmark system and the eh-XCHF method is used for computation of the ground state energy and electron-hole recombination probability. The results are compared to Hartree-Fock and explicitly correlated full configuration interaction (R12-FCI) calculations. The results indicate that an accurate description of the electron-hole wavefunction at short electron-hole inter-particle distances is crucial for qualitative description of the electron-hole recombination probability. The eh-XCHF method successfully addresses this issue and comparison of eh-XCHF calculations with R12-FCI shows good agreement. The quality of the mean field approximation for electron-hole system is also investigated by comparing HF and R12-FCI energies for electron-electron and electron-hole systems. It was found that performance of the mean field approximation is worse for the electron-hole system as compared to the corresponding electron-electron system.

UR - http://www.scopus.com/inward/record.url?scp=84859542854&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84859542854&partnerID=8YFLogxK

U2 - 10.1063/1.3693765

DO - 10.1063/1.3693765

M3 - Article

C2 - 22462833

AN - SCOPUS:84859542854

VL - 136

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 12

M1 - 124105

ER -