Abstract
Two-Dimensional Electronic Spectroscopy (2DES) is performed on CdSe colloidal quantum dots. These experiments reveal new observations on exciton structure and dynamics in quantum dots, expanding upon prior transient absorption measurements of excitonics in these systems. The 2DES method enables the separation of line broadening mechanisms, thereby better revealing the excitonic lineshapes and biexcitonic interactions. 2DES enables more information rich spectral probing of coherent phonons and their coupling to excitons. The data show spectral modulations and drifts, with differences based upon whether one monitors the excitation energy (E1) or emission energy (E3). These measurements reveal both homogeneous and inhomogeneous broadenings, as well as static and dynamic line broadening. The longitudinal optical phonon modulates the dynamic absorption spectrum both in energy and linewidth. These experiments enable measurement of hot exciton cooling with improved resolution in energy and time. These 2DES results are consistent with prior excitonic state-resolved transient absorption measurements, albeit with the addition of contributions due to coherent phonons. Finally these 2DES experiments enable disentangling of coupling versus relaxation contributions to the signals, further offering a test of electronic structure theory.
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