Enhancement of Optical Gain in Colloidal CdSe/CdS/ZnS Quantum Dots through Nanosecond Optical Pumping

J Phys Chem Lett. 2024 Feb 15;15(6):1741-1747. doi: 10.1021/acs.jpclett.4c00123. Epub 2024 Feb 7.

Abstract

Optical gain and lasing in colloidal nanocrystals are often hindered by sub-nanosecond rapid Auger non-radiative recombination, especially under continuous wave optical or electrical excitation. This study demonstrates amplified spontaneous emission (ASE) from CdSe/CdS/ZnS quantum dot (QD) solids through prolonged pulsed optical pumping over 10 ns. The incorporation of CdS and ZnS double shells on CdSe QDs effectively decelerates the Auger process in multiexcitonic states by extending the electron wave function and enhancing dielectric screening. Furthermore, we engineer smooth, densely packed QD solid films that efficiently guide the optical mode, achieving substantial net gain values under nanosecond pumping. The proposed approach helps observe ASE with gain thresholds of 0.84 and 1.5 mJ/cm2 under optical pumping pulse widths of 6 and 15 ns, respectively. This advancement can promote continuous pumping in colloidal QD gain systems, opening new avenues for optoelectronic applications.