Excitation Energy Dependence of Semiconductor Nanocrystal Emission Quantum Yields

Accurate measurements of semiconductor nanocrystal (NC) emission quantum yields (QYs) are critical to condensed phase optical refrigeration. Of particular relevance to measuring NC QYs is a longstanding debate as to whether an excitation energy-dependent (EED) QY exists. Various reports indicate existence of NC EED QYs, suggesting that the phenomenon is linked to specific ensemble properties. We therefore investigate here the existence of EED QYs in two NC systems (CsPbBr₃ and CdSe) that are possible candidates for use in optical refrigeration. The influence of NC size, size-distribution, surface ligand, and as-made emission QYs are investigated. Existence of EED QYs is assessed using two approaches (an absolute approach using an integrating sphere and a relative approach involving excitation spectroscopy). Altogether, our results show no evidence of EED QYs across samples. This suggests that parameters beyond those mentioned above are responsible for observations of NC EED QYs.