Zero-Threshold Optical Gain in Electrochemically Doped Nanoplatelets and the Physics Behind It

Colloidal nanoplatelets (NPLs) are promising materials for lasing applications. The properties are usually discussed in the framework of 2D materials, where strong excitonic effects dominate the optical properties near the band edge. At the same time, NPLs have finite lateral dimensions such that NPLs are not true extended 2D structures. Here we study the photophysics and gain properties of CdSe/CdS/ZnS core-shell-shell NPLs upon electrochemical n doping and optical excitation. Steady-state absorption and PL spectroscopy show that excitonic effects are weaker in core-shell-shell nanoplatelets due to the decreased exciton binding energy. Transient absorption studies reveal a gain threshold of only one excitation per nanoplatelet. Using electrochemical n doping, we observe the complete bleaching of the band edge exciton transitions. Combining electrochemical doping with transient absorption spectroscopy, we demonstrate that the gain threshold is fully removed over a broad spectral range and gain coefficients of several thousand cm^-1 are obtained. These doped NPLs are the best performing colloidal nanomaterial gain medium reported to date, with the lowest gain threshold and broadest gain spectrum and gain coefficients that are 4 times higher than in n-doped colloidal quantum dots. The low exciton binding energy due to the CdS and ZnS shells, in combination with the relatively small lateral size of the NPLs, results in excited states that are effectively delocalized over the entire platelet. Core-shell NPLs are thus on the border between strong confinement in QDs and dominant Coulombic effects in 2D materials. We demonstrate that this limit is in effect ideal for optical gain and that it results in an optimal lateral size of the platelets where the gain threshold per nm² is minimal.