Degenerate four-wave mixing and two-photon induced gratings in colloidal quantum dots CdSe/ZnS

Abstract

The features of nonlinear and electro-optical processes has been discovered in the case of two-photon resonant excitation of the excitons in colloidal CdSe/ZnS quantum dots. Self-diffraction arises for two laser beams intersecting in the cell with colloidal CdSe/ZnS quantum dots (QDs) due to the dynamic phase grating formatting. The calculated induced change in the refractive is sufficient to form a phase diffraction grating. Such a large value of χ(3) as compared to the third-order nonlinear susceptibility for the solvent (hexane) is due to the increase in χ(3) occurring when the intermediate resonance is attained in a medium transparent for laser radiation. In order to identify physical processes responsible for the induced grating formation and the diffraction efficiency self-diffracted pulse intensity dependences on the incident pulse intensity were measured for two samples of colloidal QD CdSe/ZnS, which frequency of the fundamental exciton transition is tuned to the high-frequency and low-frequency region from the double laser frequency. The discovered cubic dependence of the self-diffracted pulse intensity on the incident pulse intensity was explained by four-wave mixing process. Discovered above 5-th index of power dependence of the self-diffracted pulse intensity on the excitation pulses intensity we explained by the increasing magnitude of two-photon absorption (due to shifting of two photons energy of laser radiation to the exact exciton absorption resonance by red Stark shift of the exciton absorption), accompanied by the growth absorption by two-photon excited carriers that leads to the induced amplitude grating formation in addition to the phase grating.