Vibronic Excitons and Conical Intersections in Semiconductor Quantum Dots

Tilluck, Ryan W.; Mohan T. M., Nila; Hetherington, Caitlin V.; Leslie, Chase H.; Sil, Sourav; Frazier, Jared; Zhang, Mengliang; Levine, Benjamin G.; Van Patten, P. Gregory; Beck, Warren F.

doi:10.1021/acs.jpclett.1c02630

Vibronic Excitons and Conical Intersections in Semiconductor Quantum Dots

Journal Article · Thu Sep 30 00:00:00 EDT 2021 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.1c02630· OSTI ID:1864694

Tilluck, Ryan W. ^[1]; Mohan T. M., Nila ^[2]; Hetherington, Caitlin V. ^[3]; Leslie, Chase H. ^[2]; Sil, Sourav ^[2]; Frazier, Jared ^[4]; ^[4]; ^[3]; ^[4]; ^[2]

Michigan State Univ., East Lansing, MI (United States); Michigan State University
Michigan State Univ., East Lansing, MI (United States)
Stony Brook Univ., NY (United States)
Middle Tennessee State Univ., Murfreesboro, TN (United States)

Surface defects and organic surface-capping ligands affect the photoluminescence properties of semiconductor quantum dots (QDs) by altering the rates of competing nonradiative relaxation processes. In this study, broadband two-dimensional electronic spectroscopy reveals that absorption of light by QDs prepares vibronic excitons, excited states derived from quantum coherent mixing of the core electronic and ligand vibrational states. Rapidly damped coherent wavepacket motions of the ligands are observed during hot-carrier cooling, with vibronic coherence transferred to the photoluminescent state. These findings suggest a many-electron, molecular theory for the electronic structure of QDs, which is supported by calculations of the structures of conical intersections between the exciton potential surfaces of a small ammonia-passivated model CdSe nanoparticle.

View Accepted Manuscript (DOE)

Research Organization:: Michigan State Univ., East Lansing, MI (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0021197; SC0010847

OSTI ID:: 1864694

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 39 Vol. 12; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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