Effect of dipole–dipole interactions on the one-photon and two-photon photoluminescence in an ensemble of quantum dots doped in a polymer matrix

Abstract

We have developed a theory for the one-photon and two-photon fluorescence of a nanohybrid composite comprised of an ensemble of quantum dots encased in a matrix of polymer. The quantum dots are comprised of four-level quantum emitters encased within a coating of dielectric material. The fluorescence of the quantum dot system is calculated using the master equation method where dipole–dipole interaction (DDI) coupling is present. The application of a probe field to the nanohybrid composite material in conjunction with the DDI between the quantum dots generates an enhancement of both the single-photon and double-photon fluorescence, and in certain conditions causes spectrum splitting. With a strong DDI field, the two-photon emission spectrum experiences slight quenching and shifts from one peak to two peaks. The dressed states are a result of strong coupling effects between the DDI field and the quantum dots. We generated an analytical expression for the fluorescence spectrum and intensity, and quantitatively compared it to experimental data in which ZnSe quantum dots were embedded within a P3HT polymer film, with our theory strongly correlating with the experiment. We also quantitatively compared our theory with experimental data that demonstrated the single-photon emission spectrum of colloidal quantum dots comprised of a CdZnS/ZnS gradient structure in varying probe field strengths. We found that our theory predicted the spectrum peak splitting that the experiment produced.