Single-Molecule Measurements Spatially Probe States Involved in Electron Transfer from CdSe/CdS Core/Shell Nanorods
| dc.contributor.author | Morin, Rachel M. | |
| dc.contributor.author | Bryant, Garnett W. | |
| dc.contributor.author | Shevchenko, Elena V. | |
| dc.contributor.author | Sha, Yuchen | |
| dc.contributor.author | Pelton, Matthew | |
| dc.date.accessioned | 2021-10-20T16:01:26Z | |
| dc.date.available | 2021-10-20T16:01:26Z | |
| dc.date.issued | 2021-09-16 | |
| dc.description.abstract | Semiconductor nanorods with charge-accepting molecules adsorbed on their surfaces serve as model systems for solar energy conversion. An electron photoexcited from the valence band of the nanorod to a high-energy state in the conduction band will relax and transfer to a state in the molecule, producing a long-lived charge-separated state that facilitates charge extraction and thereby enables photochemical reactions. Characterizing the dynamics of the charge-separation process and the electronic states involved is essential for a microscopic understanding of photocatalysis involving these materials, but this information is obscured in ensemble measurements due to the random placement of molecules on the nanorod surfaces. Here, we show that measurements on individual CdSe/CdS core/shell nanorods functionalized by single methyl viologen molecules provide information about the distribution of electron-transfer rates from confined states in the nanorods to states in the molecules. By comparing this transfer-rate distribution to the predictions of a tight-binding model, we find that charge transfer most likely involves hot electrons in an excited conduction-band state, rather than electrons that have fully thermalized to the conduction-band edge. The ability to extract hot electrons from semiconductor nanocrystals may help enable energy-efficient photocatalysis, and the single-particle charge-transfer method may serve as a widely applicable tool to probe the spatial distribution of electronic states in nanocrystals. | en_US |
| dc.description.sponsorship | We thank Haixu Leng and Vijin Kizhake Veetil for experimental assistance. R.M.M. acknowledges support from UMBC through the URA program. Work at the Center for Nanoscale Materials was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract DE-AC0206CH-11357. Product names are mentioned to provide an accurate record of what was done. Reference of product names does not constitute validation or endorsement. | en_US |
| dc.description.uri | https://pubs.acs.org/doi/10.1021/acs.jpcc.1c06581?ref=PDF# | en_US |
| dc.format.extent | 8 pages | en_US |
| dc.genre | journal articles | en_US |
| dc.identifier | doi:10.13016/m2ndzt-pyvu | |
| dc.identifier.citation | Morin, Rachel M. et al.; Single-Molecule Measurements Spatially Probe States Involved in Electron Transfer from CdSe/CdS Core/Shell Nanorods; The Journal of Physical Chemistry C, 125, 38, 21246–21253, 16 September, 2021; https://doi.org/10.1021/acs.jpcc.1c06581 | en_US |
| dc.identifier.uri | https://doi.org/10.1021/acs.jpcc.1c06581 | |
| dc.identifier.uri | http://hdl.handle.net/11603/23134 | |
| dc.language.iso | en_US | en_US |
| dc.publisher | ACS Publications | en_US |
| dc.relation.isAvailableAt | The University of Maryland, Baltimore County (UMBC) | |
| dc.relation.ispartof | UMBC Physics Department Collection | |
| dc.relation.ispartof | UMBC Faculty Collection | |
| dc.rights | This item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author. | en_US |
| dc.rights | Public Domain Mark 1.0 | * |
| dc.rights | This work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law. | |
| dc.rights.uri | http://creativecommons.org/publicdomain/mark/1.0/ | * |
| dc.title | Single-Molecule Measurements Spatially Probe States Involved in Electron Transfer from CdSe/CdS Core/Shell Nanorods | en_US |
| dc.type | Text | en_US |
| dcterms.creator | https://orcid.org/0000-0002-6370-8765 | en_US |