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Size-dependent linear and nonlinear optical responses of silicon clusters
1School of Materials Science and Physics, Nanhu Campus, China University of Mining and Technology, No. 1 University Road, Xuzhou 221116, Jiangsu Province, China. quanjiezhong@cumt.edu.cn.
Physical Chemistry Chemical Physics : PCCP
|January 31, 2024
Summary
Silicon clusters show size-dependent optical properties, with lone-pair electrons dominating their behavior. Their nonlinear optical effects surpass those of phosphorus and sulfur clusters, offering insights into atomic-precision materials.
Area of Science:
- Computational Materials Science
- Quantum Chemistry
- Nanotechnology
Background:
- Silicon clusters exhibit unique geometric and electronic structures distinct from crystalline silicon due to quantum confinement.
- Previous research has explored silicon cluster optical properties, but unresolved questions remain regarding size-dependent responses.
Purpose of the Study:
- To investigate the size-dependent linear and nonlinear optical responses of silicon clusters.
- To understand the influence of lone-pair electrons and nuclear binding strength on optical properties.
Main Methods:
- Employed first-principles calculations to analyze silicon clusters.
- Examined orientationally averaged polarizability (αave) and second-order hyperpolarizability (γave) across various cluster sizes.
Main Results:
- Optical responses are dominated by lone-pair electrons in silicon clusters.
- Both αave and γave increase with cluster size but show no clear per-atom trend due to geometry and electron-to-atom ratios.
- αave and γave are highly sensitive to the binding strength of lone-pair electrons.
Conclusions:
- Silicon clusters demonstrate superior nonlinear optical effects compared to phosphorus and sulfur clusters.
- The study provides crucial insights into the optical characteristics of atomic-precision silicon clusters.
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