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

Abstract

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.

Authors:
; ;  [1];  [1];  [2];  [1];  [3]
  1. COMP Centre of Excellence, Department of Applied Physics, Aalto University School of Science, P.O. Box 11100, FI-00076 Aalto (Finland)
  2. (United States)
  3. (Finland)
Publication Date:
OSTI Identifier:
22416210
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 9; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ACCURACY; ATOMS; COMPUTERIZED SIMULATION; COPPER; DENSITY FUNCTIONAL METHOD; DIMERS; ELECTRONS; GOLD; NANOPARTICLES; OPTIMIZATION; PERFORMANCE; PLASMONS; SILVER; TIME DEPENDENCE

Citation Formats

Rossi, Tuomas P., E-mail: tuomas.rossi@alumni.aalto.fi, Sakko, Arto, Puska, Martti J., Lehtola, Susi, E-mail: susi.lehtola@alumni.helsinki.fi, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, Nieminen, Risto M., and Dean’s Office, Aalto University School of Science, P.O. Box 11000, FI-00076 Aalto. Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets. United States: N. p., 2015. Web. doi:10.1063/1.4913739.
Rossi, Tuomas P., E-mail: tuomas.rossi@alumni.aalto.fi, Sakko, Arto, Puska, Martti J., Lehtola, Susi, E-mail: susi.lehtola@alumni.helsinki.fi, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, Nieminen, Risto M., & Dean’s Office, Aalto University School of Science, P.O. Box 11000, FI-00076 Aalto. Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets. United States. doi:10.1063/1.4913739.
Rossi, Tuomas P., E-mail: tuomas.rossi@alumni.aalto.fi, Sakko, Arto, Puska, Martti J., Lehtola, Susi, E-mail: susi.lehtola@alumni.helsinki.fi, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, Nieminen, Risto M., and Dean’s Office, Aalto University School of Science, P.O. Box 11000, FI-00076 Aalto. Sat . "Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets". United States. doi:10.1063/1.4913739.
@article{osti_22416210,
title = {Nanoplasmonics simulations at the basis set limit through completeness-optimized, local numerical basis sets},
author = {Rossi, Tuomas P., E-mail: tuomas.rossi@alumni.aalto.fi and Sakko, Arto and Puska, Martti J. and Lehtola, Susi, E-mail: susi.lehtola@alumni.helsinki.fi and Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 and Nieminen, Risto M. and Dean’s Office, Aalto University School of Science, P.O. Box 11000, FI-00076 Aalto},
abstractNote = {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.},
doi = {10.1063/1.4913739},
journal = {Journal of Chemical Physics},
number = 9,
volume = 142,
place = {United States},
year = {Sat Mar 07 00:00:00 EST 2015},
month = {Sat Mar 07 00:00:00 EST 2015}
}