TY - JOUR

T1 - Development of polaron-transformed explicitly correlated full configuration interaction method for investigation of quantum-confined Stark effect in GaAs quantum dots

AU - Blanton, Christopher J.

AU - Brenon, Christopher

AU - Chakraborty, Arindam

PY - 2013/2/7

Y1 - 2013/2/7

N2 - The effect of external electric field on electron-hole (eh) correlation in gallium arsenide quantum dots is investigated. The electron-hole Schrodinger equation in the presence of an external electric field is solved using explicitly correlated full configuration interaction method and accurate exciton binding energy and electron-hole recombination probability are obtained. The effect of the electric field was included in the 1-particle single component basis functions by performing variational polaron transformation. The quality of the wavefunction at small inter-particle distances was improved by using Gaussian-type geminal function that depended explicitly on the electron-hole separation distance. The parameters of the explicitly correlated function were determined variationally at each field strength. The scaling of total exciton energy, exciton binding energy, and electron-hole recombination probability with respect to the strength of the electric field was investigated. It was found that a 500 kV/cm change in field strength reduces the binding energy and recombination probability by a factor of 2.6 and 166, respectively. The results show that the eh-recombination probability is affected much more strongly by the electric field than the exciton binding energy. Analysis using the polaron-transformed basis indicates that the exciton binding should asymptotically vanish in the limit of large field strength.

AB - The effect of external electric field on electron-hole (eh) correlation in gallium arsenide quantum dots is investigated. The electron-hole Schrodinger equation in the presence of an external electric field is solved using explicitly correlated full configuration interaction method and accurate exciton binding energy and electron-hole recombination probability are obtained. The effect of the electric field was included in the 1-particle single component basis functions by performing variational polaron transformation. The quality of the wavefunction at small inter-particle distances was improved by using Gaussian-type geminal function that depended explicitly on the electron-hole separation distance. The parameters of the explicitly correlated function were determined variationally at each field strength. The scaling of total exciton energy, exciton binding energy, and electron-hole recombination probability with respect to the strength of the electric field was investigated. It was found that a 500 kV/cm change in field strength reduces the binding energy and recombination probability by a factor of 2.6 and 166, respectively. The results show that the eh-recombination probability is affected much more strongly by the electric field than the exciton binding energy. Analysis using the polaron-transformed basis indicates that the exciton binding should asymptotically vanish in the limit of large field strength.

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U2 - 10.1063/1.4789540

DO - 10.1063/1.4789540

M3 - Article

C2 - 23406105

AN - SCOPUS:84873626898

SN - 0021-9606

VL - 138

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

IS - 5

M1 - 054114

ER -