Computational Study of Magic-Size CdSe Clusters with Complementary Passivation by Carboxylic and Amine Ligands

Handle URI:
http://hdl.handle.net/10754/621534
Title:
Computational Study of Magic-Size CdSe Clusters with Complementary Passivation by Carboxylic and Amine Ligands
Authors:
Voznyy, Oleksandr; Mokkath, Junais Habeeb; Jain, Ankit; Sargent, Edward H.; Schwingenschlögl, Udo ( 0000-0003-4179-7231 )
Abstract:
The electronic and optical properties of tetrahedral CdSe magic clusters (average diameter.5 nm) protected by carboxyl and amine ligands, which correspond to previously reported experimental structures, are studied using density functional theory. We find extreme ligand packing densities, capping every single dangling bond of the inorganic core, strong dependence of the Z-type metal carboxylate binding on the amount of excess amine, and potential for improved photoluminescence upon replacing phenyl ligands with alkanes. The computed absorption spectra of the Cd35Se20 cluster agree well with experiments, resolving the 0.2 eV splitting of the first exciton peak due to spin-orbit coupling. We discuss the origin of the significant broadening of the optical spectra as due to phonons and structural variations in the ligand configurations and inorganic core apexes. © 2016 American Chemical Society.
KAUST Department:
Physical Sciences and Engineering (PSE) Division
Citation:
Voznyy O, Mokkath JH, Jain A, Sargent EH, Schwingenschlögl U (2016) Computational Study of Magic-Size CdSe Clusters with Complementary Passivation by Carboxylic and Amine Ligands. The Journal of Physical Chemistry C 120: 10015–10019. Available: http://dx.doi.org/10.1021/acs.jpcc.5b10908.
Publisher:
American Chemical Society (ACS)
Journal:
The Journal of Physical Chemistry C
Issue Date:
28-Apr-2016
DOI:
10.1021/acs.jpcc.5b10908
Type:
Article
ISSN:
1932-7447; 1932-7455
Sponsors:
We thank Jonathan Owen and Alex Beecher for fruitful discussions. The research reported in this publication was supported by funding from King Abdullah University of Science and Technology (KAUST), Award KUS-11-009-21, the Ontario Research Fund - Research Excellence Program, and the Natural Sciences and Engineering Research Council (NSERC) of Canada. Computational resources provided by KAUST IT and the SciNet HPC Consortium are gratefully acknowledged. SciNet is funded by the Canada Foundation for Innovation under the auspices of Compute Canada, the Government of Ontario, the Ontario Research Fund - Research Excellence Program, and the University of Toronto.
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorVoznyy, Oleksandren
dc.contributor.authorMokkath, Junais Habeeben
dc.contributor.authorJain, Ankiten
dc.contributor.authorSargent, Edward H.en
dc.contributor.authorSchwingenschlögl, Udoen
dc.date.accessioned2016-11-03T08:31:36Z-
dc.date.available2016-11-03T08:31:36Z-
dc.date.issued2016-04-28en
dc.identifier.citationVoznyy O, Mokkath JH, Jain A, Sargent EH, Schwingenschlögl U (2016) Computational Study of Magic-Size CdSe Clusters with Complementary Passivation by Carboxylic and Amine Ligands. The Journal of Physical Chemistry C 120: 10015–10019. Available: http://dx.doi.org/10.1021/acs.jpcc.5b10908.en
dc.identifier.issn1932-7447en
dc.identifier.issn1932-7455en
dc.identifier.doi10.1021/acs.jpcc.5b10908en
dc.identifier.urihttp://hdl.handle.net/10754/621534-
dc.description.abstractThe electronic and optical properties of tetrahedral CdSe magic clusters (average diameter.5 nm) protected by carboxyl and amine ligands, which correspond to previously reported experimental structures, are studied using density functional theory. We find extreme ligand packing densities, capping every single dangling bond of the inorganic core, strong dependence of the Z-type metal carboxylate binding on the amount of excess amine, and potential for improved photoluminescence upon replacing phenyl ligands with alkanes. The computed absorption spectra of the Cd35Se20 cluster agree well with experiments, resolving the 0.2 eV splitting of the first exciton peak due to spin-orbit coupling. We discuss the origin of the significant broadening of the optical spectra as due to phonons and structural variations in the ligand configurations and inorganic core apexes. © 2016 American Chemical Society.en
dc.description.sponsorshipWe thank Jonathan Owen and Alex Beecher for fruitful discussions. The research reported in this publication was supported by funding from King Abdullah University of Science and Technology (KAUST), Award KUS-11-009-21, the Ontario Research Fund - Research Excellence Program, and the Natural Sciences and Engineering Research Council (NSERC) of Canada. Computational resources provided by KAUST IT and the SciNet HPC Consortium are gratefully acknowledged. SciNet is funded by the Canada Foundation for Innovation under the auspices of Compute Canada, the Government of Ontario, the Ontario Research Fund - Research Excellence Program, and the University of Toronto.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleComputational Study of Magic-Size CdSe Clusters with Complementary Passivation by Carboxylic and Amine Ligandsen
dc.typeArticleen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalThe Journal of Physical Chemistry Cen
dc.contributor.institutionDepartment of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, Ontario, Canadaen
kaust.authorMokkath, Junais Habeeben
kaust.authorSchwingenschlögl, Udoen
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