Exciton spin relaxation in quantum dots measured using ultrafast transient polarization grating spectroscopy

On the basis of quantum dot exciton states and selection rules for their excitation, a microscopic picture of a nonlinear optical spectroscopy that provides a direct probe of spin relaxation among quantum dot exciton states is described. Equations of motion which govern the evolution of the third order exciton population density are solved numerically to simulate the measured signals. It is shown how cross linearly-polarized pulse sequences in three-pulse transient grating experiments form a polarization grating that monitors the history of the bright exciton (F=±1) spin states. Spin flips among those states lead to a decay of the grating, and consequently the diffracted probe signal. In the microscopic picture elucidated from the simulations, destructive interference between the third-order polarizations radiated by populations of excitons with flipped and conserved spin states causes the signal decay. The experiment permits the direct observation of the kinetics of exciton spin state flips in an isotropic ensemble of quantum dots. Such measurements are demonstrated for colloidal CdSe quantum dots at room temperature, and compared with results for a control experiment. The relationship between this experiment and a difference measurement based on circularly-polarized pump and probe pulses is established.