Thermal Stability of Colloidal InP Nanocrystals: Small Inorganic Ligands Boost High-Temperature Photoluminescence

Abstract

We examine the stability of excitons in quantum-confined InP nanocrystals as a function of temperature elevation up to 800 K. Through the use of static and time-resolved spectroscopy, we find that small inorganic capping ligands substantially improve the temperature dependent photoluminescence quantum yield relative to native organic ligands and perform similarly to a wide band gap inorganic shell. For this composition, we identify the primary exciton loss mechanism as electron trapping through a combination of transient absorption and transient photoluminescence measurements. Density functional theory indicates little impact of studied inorganic ligands on InP core states, suggesting that reduced thermal degradation relative to organic ligands yields improved stability; this is further supported by a lack of size dependence in photoluminescence quenching, pointing to the dominance of surface processes, and by relative thermal stabilities of the surface passivating media. Thus, small inorganic ligands, which benefit device applications due to improved carrier access, also improve the electronic integrity of the material during elevated temperature operation and subsequent to high temperature material processing.