Document Type

Article

Publication Date

1-21-2015

Abstract

By sorting through hundreds of globally stable Si12C12 isomers using a potential surface search and using simulated annealing, we have identified low-energy structures. Unlike isomers knit together by Si–C bonds, the lowest energy isomers have segregated carbon and silicon regions that maximize stronger C–C bonding. Positing that charge separation between the carbon and silicon regions would produce interesting optical absorption in these cluster molecules, we used time-dependent density functional theory to compare the calculated optical properties of four isomers representing structural classes having different types of silicon and carbon segregation regions. Absorptions involving charge transfer between segregated carbon and silicon regions produce lower excitation energies than do structures having alternating Si–C bonding for which frontier orbital charge transfer is exclusively from separated carbon atoms to silicon atoms. The most stable Si12C12 isomer at temperatures below 1100 K is unique as regards its high symmetry and large optical oscillator strength in the visible blue. Its high-energy and low-energy visible transitions (1.15 eV and 2.56 eV) are nearly pure one-electron silicon-to-carbon transitions, while an intermediate energy transition (1.28 eV) is a nearly pure carbon-to-silicon one-electron charge transfer.

Comments

© 2015 Authors(s), published under an exclusive license with American Institute of Physics.

AFIT Scholar, as the repository of the Air Force Institute of Technology, furnishes the published Version of Record for this article in accordance with the sharing policy of the publisher, AIP Publishing. A 12-month embargo was observed.

This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Applied Physics Letters 142, 034303 as fully cited below and may be found at DOI: 10.1063/1.4905542

Funding notes: We acknowledge financial support from Molecular Dynamics and Theory Research Program of the Air Force Office of Scientific Research managed by Dr. Michael Berman.

Source Publication

Journal of Chemical Physics

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