Modulation of High-Intensity Optical Properties in CdS/CdSe/CdS Spherical Quantum Wells by CdSe Layer Thickness.

Spherical quantum wells (SQWs) have proven to be excellent materials for suppressing Auger recombination due to their expanded confinement volume. However, research on the factors and mechanisms of their high-intensity optical properties, such as multiexciton properties and third-order optical nonlinearities, remains incomplete, limiting further optimization of these properties. Here, a series of CdS/CdSe (xML)/CdS SQWs with varying CdSe layer thicknesses were prepared. The modulation effects of CdSe shell variations on the PL properties, defect distribution, biexciton binding energy, and third-order optical nonlinearities of the SQWs were investigated, and their impact on the material's multiexciton properties was further analyzed. Results showed that the typical CdS/CdSe(3ML)/CdS sample exhibited a large volume-normalized two-photon absorption cross-section (18.17 × 10 GM/nm) and favorable biexciton characteristics. Optical amplification was observed at 12.4 μJ/cm and 1.02 mJ/cm under one-photon (400 nm) and two-photon (800 nm) excitation, respectively. Furthermore, different amplified spontaneous emission spectra were observed for the first time under one/two-photon excitation. This phenomenon was attributed to thermal effects overcoming the biexciton binding energy. This study provides valuable insights for further optimizing multiexciton gain characteristics in SQWs and developing optical gain applications.