Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 10, Issue 20, Pages 6144-6150Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.9b02474
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Funding
- Department of Energy [DE-SC0015782]
- Brazilian National Council for Scientific and Technological Development (CNPq)
- FAPESP [2013/16911-2, 2016/50011-7]
- U.S. Department of Energy (DOE) [DE-SC0015782] Funding Source: U.S. Department of Energy (DOE)
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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.
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