Oxygen Stabilizes Photoluminescence of CdSe/CdS Core/Shell Quantum Dots via Deionization

摘要

By taking advantage of well-defined spectroscopic signatures of high-quality CdSe/CdS core/shell QDs, the effects of oxygen on photoluminescence (PL) of QDs were studied systematically and quantitatively at both single-dot and ensemble (on substrate and in solution) levels, which reveals a unified yet simple picture. With a sufficient amount of oxygen in the system during photoexcitation, the core/shell QDs in all forms would be deionized timely from the photogenerated and inefficient trion state back to the efficient single-exciton state, with superoxide radicals as the reduction product of oxygen. Under a given excitation power, rates of both spontaneous deionization and photodeionization channels increased by increasing the oxygen pressure, but photoionization of the QDs was barely affected by the oxygen pressure. While stabilizing PL by oxygen was identified for both CdSe plain core and CdSe/CdS core/shell QDs, irreversible photocorrosion was only observed for CdSe plain core QDs, suggesting the importance of high-quality epitaxial shells for QDs in various applications.