Exciton–Phonon Coupling and Carrier Relaxation in PbS Quantum Dots: The Case of Carboxylate Ligands

Kennehan, Eric R.; Munson, Kyle T.; Grieco, Christopher; Doucette, Grayson S.; Marshall, Ashley R.; Beard, Matthew C.; Asbury, John B.

doi:10.1021/acs.jpcc.1c05803

Title: Exciton–Phonon Coupling and Carrier Relaxation in PbS Quantum Dots: The Case of Carboxylate Ligands

Journal Article · Fri Oct 08 00:00:00 EDT 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c05803· OSTI ID:1839362

Kennehan, Eric R. ^[1]; Munson, Kyle T. ^[2]; Grieco, Christopher ^[1]; Doucette, Grayson S. ^[2]; Marshall, Ashley R. ^[3];

^[3];

^[2]

Magnitude Instruments, State College, PA (United States); Pennsylvania State Univ., University Park, PA (United States)
Pennsylvania State Univ., University Park, PA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)

Some ligand-nanocrystal combinations exhibit rapid cooling of highly excited electronic states while other nanocrystal/shell combinations do not appear to have this effect. There remains a need to identify the distinguishing properties of ligand-nanocrystal interactions that avoid such rapid relaxation processes to guide the design of colloidal quantum dots (QDs) that take advantage of multiple exciton generation or hot-carrier extraction processes. Here, we use mid-infrared transient absorption spectroscopy to investigate the influence that carboxylate ligands with distinct excited state surface chemistries has on exciton-phonon coupling and hot exciton relaxation in PbS quantum dot (QD) films. Our findings reveal that despite significant differences in the excited state surface chemistry of oleate (OA) and iodide/mercaptopropionic acid (I-/MPA) ligands, PbS QD films passivated with both ligand types exhibit identical electronic relaxation rates and exciton-phonon coupling strengths within experimental precision. The data suggest that the inorganic lattice is the principal source of exciton-phonon coupling that influences hot exciton relaxation, rather than the vibronic modes of carboxylate ligands. The size-dependent nature of the exciton-phonon coupling strength is consistent with the localization of charge on the QD surfaces, which enhances the mixing of electronic and nuclear coordinates particularly when the electronic states are more quantum confined in smaller nanocrystals.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)

Grant/Contract Number:: SC0019349; DGE1255832; AC36-08GO28308

OSTI ID:: 1839362

Alternate ID(s):: OSTI ID: 1832229

Report Number(s):: NREL/JA-5900-80431; DGE1255832

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 41; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Exciton–Phonon Coupling and Carrier Relaxation in PbS Quantum Dots: The Case of Carboxylate Ligands

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