Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets

We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold nanoparticles that are of experimental interest but computat...

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Bibliographic Details
Published in:The Journal of chemical physics 2015-03, Vol.142 (9), p.094114-094114
Main Authors: Rossi, Tuomas P, Lehtola, Susi, Sakko, Arto, Puska, Martti J, Nieminen, Risto M
Format: Article
Language:English
Subjects:
ACCURACY
ATOMS
Completeness
Computer Simulation
COMPUTERIZED SIMULATION
COPPER
Copper - chemistry
DENSITY FUNCTIONAL METHOD
Density functional theory
DIMERS
Electronics
ELECTRONS
First principles
GOLD
Gold - chemistry
INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY
Metal Nanoparticles - chemistry
Models, Chemical
Nanoalloys
NANOPARTICLES
Nanotechnology
OPTIMIZATION
Photoabsorption
PLASMONS
Quantum theory
SILVER
Silver - chemistry
TIME DEPENDENCE
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Summary:We present an approach for generating local numerical basis sets of improving accuracy for first-principles nanoplasmonics simulations within time-dependent density functional theory. The method is demonstrated for copper, silver, and gold nanoparticles that are of experimental interest but computationally demanding due to the semi-core d-electrons that affect their plasmonic response. The basis sets are constructed by augmenting numerical atomic orbital basis sets by truncated Gaussian-type orbitals generated by the completeness-optimization scheme, which is applied to the photoabsorption spectra of homoatomic metal atom dimers. We obtain basis sets of improving accuracy up to the complete basis set limit and demonstrate that the performance of the basis sets transfers to simulations of larger nanoparticles and nanoalloys as well as to calculations with various exchange-correlation functionals. This work promotes the use of the local basis set approach of controllable accuracy in first-principles nanoplasmonics simulations and beyond.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.4913739