Deciphering Charging Status, Absolute Quantum Efficiency, and Absorption Cross Section of MultiCarrier States in Single Colloidal Quantum Dot

Abstract: Upon photo- or electrical-excitation, colloidal quantum dots (QDs) are often found in multi-carrier states due to multi-photon absorption and photo-charging of the QDs. While many of these multi-carrier states are observed in single-dot spectroscopy, their properties are not well studied due to random charging/discharging, emission intensity intermittency, and uncontrolled surface defects of single QD. Here we report in-situ deciphering the charging status, and precisely assessing the absorption cross section, and determining the absolute emission quantum yield of mono-exciton and biexciton states for neutral, positively-charged, and negatively-charged single core/shell CdSe/CdS QD. We uncover very different photon statistics of the three charge states in single QD and unambiguously identify their charge sign together with the information of their photoluminescence decay dynamics. We then show their distinct photoluminescence saturation behaviors and evaluated the absolute values of absorption cross sections and quantum efficiencies of monoexcitons and biexcitons. We demonstrate that addition of an extra hole or electron in a QD changes not only its emission properties but also varies its absorption cross section.