Non-Markovian Exciton-Phonon Interactions in Core-Shell Colloidal Quantum Dots at Femtosecond Timescales

CNPQ - CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICOFAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOWe perform two-dimensional coherent spectroscopy on CdSe/CdZnS core-shell colloidal quantum dots at cryogenic temperatures. In the two-dimensional spectra, sidebands due to electronic coupling with CdSe lattice LO-phonon modes are observed to have evolutions deviating from the exponential dephasing expected from Markovian spectral diffusion, which is instantaneous and memoryless. Comparison to simulations provides evidence that LO-phonon coupling induces energy-gap fluctuations on the finite timescales of nuclear motion. The femtosecond resolution of our technique probes exciton dynamics directly on the timescales of phonon coupling in nanocrystals.123516CNPQ - CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICOFAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOCNPQ - CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICOFAPESP - FUNDAÇÃO DE AMPARO À PESQUISA DO ESTADO DE SÃO PAULOSem informação2013/16911-22016/50011-7This work was supported by the Department of Energy Grant No. DE-SC0015782. D. B. A. acknowledges support by a fellowship from the Brazilian National Council for Scientific and Technological Development (CNPq). L. A. P. acknowledges support from FAPESP (Projects No. 2013/16911-2 and No. 2016/50011-7)

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We have investigated the threshold of photodetachment of Li^- leading to the formation of the residual Li atom in the $2p ^2P$ state. The excited residual atom was selectively photoionized via an intermediate Rydberg state and the resulting Li^+ ion was detected. A collinear laser-ion beam geometry enabled both high resolution and sensitivity to be attained. We have demonstrated the potential of this state selective photodetachment spectroscopic method by improving the accuracy of Li electron affinity measurements an order of magnitude. From a fit to the Wigner law in the threshold region, we obtained a Li electron affinity of 0.618 049(20) eV.Comment: 5 pages,6 figures,22 reference