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Measurement of Scattering Nonlinearities from a Single Plasmonic Nanoparticle
Published on: January 3, 2016
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Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets.
Tuomas P Rossi1, Susi Lehtola1, Arto Sakko1
1COMP Centre of Excellence, Department of Applied Physics, Aalto University School of Science, P.O. Box 11100, FI-00076 Aalto, Finland.
The Journal of Chemical Physics
|March 10, 2015
Summary
We developed a new method for accurate first-principles nanoplasmonics simulations. This approach improves computational efficiency for simulating metal nanoparticles like gold and silver, advancing the field of computational materials science.
Area of Science:
- Computational physics and chemistry
- Materials science
- Quantum chemistry
Background:
- First-principles nanoplasmonics simulations are computationally demanding, especially for noble metals like copper, silver, and gold.
- The presence of semi-core d-electrons significantly impacts the plasmonic response of these metals, necessitating accurate theoretical treatment.
- Existing methods often face challenges in balancing accuracy and computational cost for complex nanostructures.
Purpose of the Study:
- To present a novel approach for generating local numerical basis sets with controllable accuracy for first-principles nanoplasmonics simulations.
- To address the computational challenges associated with simulating the plasmonic properties of experimentally relevant metal nanoparticles.
- To enable more efficient and accurate theoretical investigations of nanoplasmonic phenomena.
Main Methods:
- Augmenting numerical atomic orbital basis sets with truncated Gaussian-type orbitals (GTOS).
- Employing a completeness-optimization scheme applied to photoabsorption spectra of metal atom dimers.
- Developing local basis sets that systematically improve accuracy towards the complete basis set limit.
Main Results:
- Demonstrated the generation of local numerical basis sets with systematically improving accuracy for copper, silver, and gold nanoparticles.
- Validated the transferability of the developed basis sets to larger nanoparticles, nanoalloys, and various exchange-correlation functionals.
- Achieved basis sets that approach the accuracy of the complete basis set limit.
Conclusions:
- The proposed local basis set approach offers a pathway to achieve controllable accuracy in first-principles nanoplasmonics simulations.
- This method enhances the computational feasibility of studying complex nanometal systems.
- The work facilitates broader applications of accurate first-principles simulations in nanoplasmonics and related fields.
