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

Liu, A.; Almeida, D. B.; Bae, W. K.; Padilha, L. A.; Cundiff, S. T.

doi:10.1103/physrevlett.123.057403

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

Journal Article · Fri Aug 02 00:00:00 EDT 2019 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.123.057403· OSTI ID:1612329

Liu, A. ^[1]; Almeida, D. B. ^[1]; Bae, W. K. ^[2]; Padilha, L. A. ^[3]; Cundiff, S. T. ^[1]

Univ. of Michigan, Ann Arbor, MI (United States)
Sungkyunkwan Univ., Gyeonggi (Korea)
Univ. Estadual de Campinas, Sao Paulo (Brazil)

We 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. Furthermore, the femtosecond resolution of our technique probes exciton dynamics directly on the timescales of phonon coupling in nanocrystals.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0015782

OSTI ID:: 1612329

Alternate ID(s):: OSTI ID: 1546822

Journal Information:: Physical Review Letters, Vol. 123, Issue 5; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 21 works

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

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