## Abstract

Using state-of-the-art antisymmetrized multiconfiguration time-dependent Hartree (MCTDH) electron dynamics calculations we study the interdependence of the intermolecular Coulombic decay (ICD) process on the geometric parameters of a doubly-charged paired quantum dot (PQD) model system in the framework of the effective mass approximation (EMA). We find that ICD displays a maximum rate for a certain geometry of the electron-emitting quantum dot, which is simultaneously dependent on both the distance between the quantum dots as well as the photon-absorbing quantum dot's geometry. The rate maximum is shown to be caused by the competing effects of polarization of electron density and Coulomb repulsion. The ICD rate-maximized PQD geometry in GaAs QDs yields a decay time of 102.39 ps. It is given by two vertically-aligned cylindrical QDs with radii of 14.42 nm separated by 86.62 nm. The photon absorbing QD then has a height of 46.59 nm and the electron emitting QD a height of 16.33 nm.

Original language | English |
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Pages (from-to) | 2141-2150 |

Number of pages | 10 |

Journal | Journal of Computational Chemistry |

Volume | 38 |

Issue number | 25 |

DOIs | |

State | Published - 30 Sep 2017 |

Externally published | Yes |

## Keywords

- electron dynamics
- geometric control
- intermolecular Coulombic decay
- quantum dots
- quantum size effect