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

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

Authors :
Liu A
Almeida DB
Bae WK
Padilha LA
Cundiff ST
Source :
Physical review letters [Phys Rev Lett] 2019 Aug 02; Vol. 123 (5), pp. 057403.
Publication Year :
2019

Abstract

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

Details

Language :
English
ISSN :
1079-7114
Volume :
123
Issue :
5
Database :
MEDLINE
Journal :
Physical review letters
Publication Type :
Academic Journal
Accession number :
31491330
Full Text :
https://doi.org/10.1103/PhysRevLett.123.057403