Exciton Superposition States in CdSe Nanocrystals Measured Using Broadband Two-Dimensional Electronic Spectroscopy

Coherent superpositions among eigenstates are of interest in fields as diverse as photosynthesis and quantum computation. In this report, we used two-dimensional electronic spectroscopy (2D ES) to measure the decoherence time of a superposition of the two lowest-energy excitons in colloidal CdSe nanocrystals (cubic phase) in solution at room temperature. In the electron–hole representation, the quantum coherence is, remarkably, a twelve-particle correlation. By comparing the measured 2D ES to simulations, we also explored the effects of inhomogeneous broadening and examined the spectroscopic signatures of biexcitons.