Conical intersections shed light on hot carrier cooling in quantum dots

Hetherington, Caitlin V.; Mohan T. M., Nila; Shameem, Shanu A.; Beck, Warren F.; Levine, Benjamin G.

doi:10.1063/5.0295696

Conical intersections shed light on hot carrier cooling in quantum dots

Journal Article · Mon Dec 01 00:00:00 EST 2025 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0295696· OSTI ID:3012974

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Stony Brook Univ., NY (United States)
Michigan State Univ., East Lansing, MI (United States)

Experimental observations of vibronic coherences in electronically excited colloidal semiconductor nanocrystals offer a window into the ultrafast dynamics of hot carrier cooling. In previous work, we showed that, in amine-passivated quantum dots (QDs), these coherences arise during relaxation through a cascade of conical intersections between electronically excited states. Here, in this work, we demonstrate the generality of this framework by application to QDs with surface-bound carboxylate ligands. A model involving a similar cascade of conical intersections accurately reproduces the frequencies of vibronic coherences observed with broadband multidimensional spectroscopy. The impact of ligands on the relaxation dynamics is attributed to two distinct mechanisms involving either electronic or vibrational coupling between the core and ligands. Compared to the amine-passivated QDs studied previously, the electronic coupling mechanism is less prominent in carboxylate-passivated QDs. Furthermore, comparison of acetate and formate ligands reveals that truncating the ligand alkyl chains alters the relaxation behavior predicted by the model.

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)

Grant/Contract Number:: SC0021197

OSTI ID:: 3012974

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 21 Vol. 163; ISSN 1089-7690; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Conical intersections shed light on hot carrier cooling in quantum dots

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