How To Identify Plasmons from the Optical Response of Nanostructures
arXiv:1709.06754 · doi:10.1021/acsnano.7b03421
Abstract
A promising trend in plasmonics involves shrinking the size of plasmon-supporting structures down to a few nanometers, thus enabling control over light-matter interaction at extreme-subwavelength scales. In this limit, quantum mechanical effects, such as nonlocal screening and size quantization, strongly affect the plasmonic response, rendering it substantially different from classical predictions. For very small clusters and molecules, collective plasmonic modes are hard to distinguish from other excitations such as single-electron transitions. Using rigorous quantum mechanical computational techniques for a wide variety of physical systems, we describe how an optical resonance of a nanostructure can be classified as either plasmonic or nonplasmonic. More precisely, we define a universal metric for such classification, the generalized plasmonicity index (GPI), which can be straightforwardly implemented in any computational electronic-structure method or classical electromagnetic approach to discriminate plasmons from single-particle excitations and photonic modes. Using the GPI, we investigate the plasmonicity of optical resonances in a wide range of systems including: the emergence of plasmonic behavior in small jellium spheres as the size and the number of electrons increase; atomic-scale metallic clusters as a function of the number of atoms; and nanostructured graphene as a function of size and doping down to the molecular plasmons in polycyclic aromatic hydrocarbons. Our study provides a rigorous foundation for the further development of ultrasmall nanostructures based on molecular plasmonics
arXiv commentThis is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes. Link to th original article: http://pubs.acs.org/doi/abs/10.1021/acsnano.7b03421
References in corpus (12)
- Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
- Graphene Plasmonics: Challenges and Opportunities
- Localized surface plasmon resonance in silver nanoparticles: Atomistic first-principles time-dependent density-functional theory calculations
- Extraordinary nonlinear plasmonics in graphene nanoislands
- Tunable plasmons in atomically thin gold nanodisks
- Plasmons do not go that quantum
- turboTDDFT 2.0 - Hybrid functionals and new algorithms within time-dependent density-functional perturbation theory
- Excitons in Silicon Nanocrystalites: The Nature of Luminescence
- Plasmons Driven by Single Electrons in Graphene Nanoislands
- Which resonances in small metallic nanoparticles are plasmonic?
- Quantum Plasmonic Nanoantennas
- Quantum plasmonics: An energy perspective to quantify nonclassical effects
Cited by in corpus (11)
- Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
- Macroscopic QED for quantum nanophotonics: Emitter-centered modes as a minimal basis for multi-emitter problems
- Electrically Driven Hot-Carrier Generation and Above-threshold Light Emission in Plasmonic Tunnel Junctions
- Quantum spill out in few-nanometer metal gaps: Effect on gap plasmons and reflectance from ultrasharp groove arrays
- Quantifying the Plasmonic Character of Optical Excitations in a Molecular J-Aggregate
- Quantum spill-out in nanometer-thin gold slabs: Effect on plasmon mode index and plasmonic absorption
- Comprehensive Microscopic Theory for Coupling of Longitudinal--Transverse Fields and Individual--Collective Excitations
- From single-particle-like to interaction-mediated plasmonic resonances in graphene nanoantennas
- Coulomb effects on the photo-excited quantum dynamics of electrons in a plasmonic nanosphere
- Investigation of plasmonic evolution of atomically size-selected Au clusters by electron energy loss spectrum--from solid state to molecular scale
- Plasmon excitations in mixed metallic nanoarrays