Plasmonic systems, such as metal nanoparticles, are widely used in different areas of application, going from biology to photovoltaics. The modeling of the optical response of such systems is of fundamental importance to analyze their behavior and to design new systems with required properties. When the characteristic sizes/distances reach a few nanometers, nonlocal and spill-out effects become relevant and conventional classical electrodynamics models are no more appropriate. Methods based on the Time-Dependent Density Functional Theory (TD-DFT) represent the current reference for the description of quantum effects. However, TD-DFT is based on knowledge of all occupied orbitals, whose calculation is computationally prohibitive to model large plasmonic systems of interest for applications. On the other hand, methods based on the orbital-free (OF) formulation of TD-DFT can scale linearly with the system size. In this Review, OF methods ranging from semiclassical models to the Quantum Hydrodynamic Theory will be derived from the linear response TD-DFT, so that the key approximations and properties of each method can be clearly highlighted. The accuracy of the various approximations will then be validated for the linear optical properties of jellium nanoparticles, the most relevant model system in plasmonics. OF methods can describe the collective excitations in plasmonic systems with great accuracy and without system-tuned parameters. The accuracy of these methods depends only on the accuracy of the (universal) kinetic energy functional of the ground-state electronic density. Current approximations and future development directions will also be indicated.
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14 September 2022
Review Article|
September 08 2022
Orbital-free methods for plasmonics: Linear response
Special Collection:
Advances in Modeling Plasmonic Systems
Fabio Della Sala
Fabio Della Sala
a)
(Conceptualization, Data curation, Supervision, Writing – original draft, Writing – review & editing)
Institute for Microelectronics and Microsystems (CNR-IMM)
, Via Monteroni, Campus Unisalento, 73100 Lecce, Italy
and Center for Biomolecular Nanotechnologies, Istituto Italiano di Tecnologia
, Via Barsanti 14, 73010 Arnesano (LE), Italy
a)Author to whom correspondence should be addressed: fabio.dellasala@unisalento.it
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a)Author to whom correspondence should be addressed: fabio.dellasala@unisalento.it
Note: This paper is part of the JCP Special Topic on Advances in Modeling Plasmonic Systems.
J. Chem. Phys. 157, 104101 (2022)
Article history
Received:
May 26 2022
Accepted:
August 02 2022
Citation
Fabio Della Sala; Orbital-free methods for plasmonics: Linear response. J. Chem. Phys. 14 September 2022; 157 (10): 104101. https://doi.org/10.1063/5.0100797
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