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Coupling to phonon modes is a primary mechanism of excitonic dephasing andenergy loss in semiconductors. However, low-energy phonons in colloidal quantumdots and their coupling to excitons are poorly understood, since theirexperimental signatures are weak and usually obscured by unavoidableinhomogeneous broadening of colloidal dot ensembles. We use multi-dimensionalcoherent spectroscopy at cryogenic temperatures to extract the homogeneousnonlinear optical response of excitons in a CdSe/CdZnS core/shell colloidalquantum dot ensemble. Comparison to simulation provides evidence that theobserved lineshapes arise from the co-existence of confined and delocalizedvibrational modes, both of which couple strongly to excitons in CdSe/CdZnScolloidal quantum dots.

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