Journal
NANO LETTERS
Volume 17, Issue 2, Pages 909-914Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.6b04213
Keywords
Hole transfer; dithiocarbamate; CdSe/CdS nanorod; density functional theory; midgap states
Categories
Funding
- Department of Energy [DE-FG02-09ER46554]
- McMinn Endowment at VanFlerbilt
- National Science Foundation [ACI-1053575]
- National Energy Research Scientific Computing Center (NERSC), a DOE office of Science User Facility - Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- TN-SCORE [NSF EPS-1004083]
- NSF [EPS 1004083]
- Stanley and Ann T. Tarbell Endowment Fund
- [NSF-CHE 1506587]
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A new ligand that covalently attaches to the surface of colloidal CdSe/CdS nanorods and can simultaneously chelate a molecular metal center is described. The dithiocarbamate bipyridine ligand system facilitates hole transfer through energetic overlap at the inorganic organic interface and conjugation through the organic ligand to a chelated metal center. Density functional theory calculations show that the coordination of the free ligand to a CdS surface causes the formation of two hybridized molecular states that lie in the band gap of CdS. The further chelation of Fe(II) to the bipyridine moiety causes the presence of seven midgap states. Hole transfer from the CdS valence band to the midgap states is dipole allowed and occurs at a faster rate than what is experimentally known for the CdSe/CdS band-edge radiative recombination. In the case of the ligand bound with iron, a two-step process emerges that places the hole on the iron, again at rates much faster than band gap recombination. The system was experimentally assembled and characterized via UV vis absorbance spectroscopy, fluorescence spectroscopy, time-resolved photoluminescence spectroscopy, and energy dispersive X-ray spectroscopy. Theoretically predicted red shifts in absorbance were observed expected quench in photoluminescence and lifetimes in time-resolved photoluminescence. experimentally, as well as the expected quench in photoluminescence and lifetimes in time-resolved photoluminescence.
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