The superatomic state beyond conventional magic numbers: Ligated metal chalcogenide superatoms
Abstract
The field of cluster science is drawing increasing attention due to the strong size and composition-dependent properties of clusters and the exciting prospect of clusters serving as the building blocks for materials with tailored properties. However, identifying a unifying central paradigm that provides a framework for classifying and understanding the diverse behaviors is an outstanding challenge. One such central paradigm is the superatom concept that was developed for metallic and ligand-protected metallic clusters. The periodic electronic and geometric closed shells in clusters result in their properties being based on the stability they gain when they achieve closed shells. This stabilization results in the clusters having a well-defined valence allowing them to be classified as superatoms – thus, extending the periodic table to a third dimension. This perspective focuses on extending the superatomic concept to ligated metal-chalcogen clusters that have recently been synthesized in solutions and form assemblies with counterions that have wide-ranging applications. Here we illustrate that the periodic patterns emerge in the electronic structure of ligated metal-chalcogenide clusters. The stabilization gained by the closing of their electronic shells allows for the prediction of their redox properties. Further investigations reveal how the selection of ligands may control the redox propertiesmore »
- Authors:
-
- Virginia Commonwealth Univ., Richmond, VA (United States)
- Publication Date:
- Research Org.:
- Virginia Commonwealth Univ., Richmond, VA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1824338
- Alternate Identifier(s):
- OSTI ID: 1822545
- Grant/Contract Number:
- SC0006420
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 155; Journal Issue: 12; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Cluster; superatoms; electronic structure; electronic properties; chemical dopants; photoelectron spectroscopy; electronic shell; HOMO and LUMO; semiconductors; P-N junctions; free electron model; electronic band structure
Citation Formats
Khanna, Shiv N., Reber, Arthur C., Bista, Dinesh, Sengupta, Turbasu, and Lambert, Ryan. The superatomic state beyond conventional magic numbers: Ligated metal chalcogenide superatoms. United States: N. p., 2021.
Web. doi:10.1063/5.0062582.
Khanna, Shiv N., Reber, Arthur C., Bista, Dinesh, Sengupta, Turbasu, & Lambert, Ryan. The superatomic state beyond conventional magic numbers: Ligated metal chalcogenide superatoms. United States. https://doi.org/10.1063/5.0062582
Khanna, Shiv N., Reber, Arthur C., Bista, Dinesh, Sengupta, Turbasu, and Lambert, Ryan. Tue .
"The superatomic state beyond conventional magic numbers: Ligated metal chalcogenide superatoms". United States. https://doi.org/10.1063/5.0062582. https://www.osti.gov/servlets/purl/1824338.
@article{osti_1824338,
title = {The superatomic state beyond conventional magic numbers: Ligated metal chalcogenide superatoms},
author = {Khanna, Shiv N. and Reber, Arthur C. and Bista, Dinesh and Sengupta, Turbasu and Lambert, Ryan},
abstractNote = {The field of cluster science is drawing increasing attention due to the strong size and composition-dependent properties of clusters and the exciting prospect of clusters serving as the building blocks for materials with tailored properties. However, identifying a unifying central paradigm that provides a framework for classifying and understanding the diverse behaviors is an outstanding challenge. One such central paradigm is the superatom concept that was developed for metallic and ligand-protected metallic clusters. The periodic electronic and geometric closed shells in clusters result in their properties being based on the stability they gain when they achieve closed shells. This stabilization results in the clusters having a well-defined valence allowing them to be classified as superatoms – thus, extending the periodic table to a third dimension. This perspective focuses on extending the superatomic concept to ligated metal-chalcogen clusters that have recently been synthesized in solutions and form assemblies with counterions that have wide-ranging applications. Here we illustrate that the periodic patterns emerge in the electronic structure of ligated metal-chalcogenide clusters. The stabilization gained by the closing of their electronic shells allows for the prediction of their redox properties. Further investigations reveal how the selection of ligands may control the redox properties of the superatoms. These ligated clusters may serve as chemical dopants for two-dimensional semiconductors to control their transport characteristics. Superatomic molecules of multiple metal-chalcogen superatoms allow for the formation of nano pn junctions ideal for directed transport and photon harvesting. As a result, the perspective outlines future developments, including the synthesis of magnetic superatoms.},
doi = {10.1063/5.0062582},
journal = {Journal of Chemical Physics},
number = 12,
volume = 155,
place = {United States},
year = {Tue Sep 28 00:00:00 EDT 2021},
month = {Tue Sep 28 00:00:00 EDT 2021}
}
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