Effect of Dot Size on Exciton Binding Energy and Electron-Hole Recombination Probability in CdSe Quantum Dots.

Radius of quantum dot Exciton binding energy and electron-hole recombination probability are presented as the two important metrics for investigating effect of dot size on electronhole interaction in CdSe quantum dots. Direct computation of electron-hole recombination probability is challenging because it requires an accurate mathematical description of electron-hole wavefunction in the neighborhood of the electron-hole coalescence point. In this work, we address this challenge by solving the electron-hole Schrodinger equation using the electron-hole explicitly correlated Hartree-Fock (ehXCHF) method. The calculations were performed for a series of CdSe clusters ranging from Cd20Se19 to Cd74608Se74837 that correspond to dot diameter range of 1− 20 nm. The calculated exciton binding energies and electron-hole recombination probabilities were found to decrease with increasing dot size. Both of these quantities were found to scale as D−n dot with respect to the dot diameter D. One of the key insights from this study is that the electron-hole recombination probability decreases at a much faster rate than the exciton binding energy as a function of dot size. It was found that an increase in the dot size by a factor of 16.1, resulted in a decrease in the exciton binding energy and electron-hole recombination probability by a factor of 14.4 and 5.5×106, respectively.