Simultaneous Existence of Confined and Delocalized Vibrational Modes in Colloidal Quantum Dots.

Coupling to phonon modes is a primary mechanism of excitonic dephasing and energy loss in semiconductors. However, low-energy phonons in colloidal quantum dots and their coupling to excitons are poorly understood because their experimental signatures are weak and usually obscured by the unavoidable inhomogeneous broadening of colloidal dot ensembles. We use multidimensional coherent spectroscopy at cryogenic temperatures to extract the homogeneous nonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidal quantum dot ensemble. A comparison to the simulation provides evidence that the observed lineshapes arise from the coexistence of confined and delocalized vibrational modes, both of which couple strongly to excitons in CdSe/CdZnS colloidal quantum dots.