Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

Abstract

Colloidal quantum shells are spherical semiconductor quantum wells, which have shown strong promise as optical materials, particularly in classes of experiments requiring multiple excitons. The two-photon properties of CdS/CdSe/CdS quantum shell samples are studied here to demonstrate large non-linear absorption cross-sections while retaining advantageous multiexciton physics conferred by the geometrical structure. The quantum shells have large two-phonon cross sections (0.4–7.9 × 10⁶ GM), which highlights their potential use in upconversion imaging in which large per particle two-photon absorption is critical. Time-resolved measurements confirmed that the quantum shells have long biexciton lifetime (>10 ns in the largest core samples reported here) and large gain bandwidth (>300 meV). The combination of these attributes with large two-photon cross sections makes the CdS/CdSe/CdS quantum shells excellent gain media for two-photon excitation. With a broad gain bandwidth and long gain lifetime, quantum shell solids support multimodal amplified spontaneous emission from excitons, biexcitons, and higher excited states. Thresholds for amplified spontaneous emission and lasing, which are as low as 1 mJ cm⁻², are comparable to, or lower than, the thresholds reported for other colloidal materials.