Thermal degradation of optical resonances in plasmonic nanoparticles

Sørensen, Lasse Kragh; Khrennikov, Daniil E.; Gerasimov, V. S.; Ershov, A. E.; Vysotin, M. A.; Monti, Susanna; Zakomirnyi, Vadim I.; Polyutov, Sergey; Ågren, Hans; Karpov, S. V.

doi:10.1039/d1nr06444d

Cited by 6 publications

(16 citation statements)

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“…In such a model, an increase in the thickness of the shell (surface layer) of a particle with a given size and with a lower (compared to a core) dielectric constant (real part) is always accompanied by an increase in the spectral red shift of the surface plasmon resonance. 31…”

Section: Resultsmentioning

confidence: 99%

“…The Extended Discrete Interaction Model (Ex-DIM), [29][30][31] is a discrete structure model parameterized directly from experimental data with respect to the position of the SPR and maximum value of the extinction cross section from a fitted Mie theory. 32 In the Ex-DIM each atom is represented by a Gaussian charge distribution and endowed with a polarizability and relaxation constants which govern the inter-atomic interaction.…”

Section: The Extended Discrete Interaction Modelmentioning

confidence: 99%

“…44 The difference in position and extinction cross section between a perfect face-centered lattice and a structure obtained from molecular dynamics at ambient temperature 293.15 K for spherical structures have been shown to be very small. 31…”

Section: Modelmentioning

confidence: 99%

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Medium dependent optical response in ultra-fine plasmonic nanoparticles

Sørensen

Khrennikov²,

Gerasimov

et al. 2022

Phys. Chem. Chem. Phys.

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Section: Resultsmentioning

confidence: 99%

Section: The Extended Discrete Interaction Modelmentioning

confidence: 99%

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Medium dependent optical response in ultra-fine plasmonic nanoparticles

Sørensen

Khrennikov²,

Gerasimov

et al. 2022

Phys. Chem. Chem. Phys.

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“…In such a model, an increase in the thickness of the shell (surface layer) of a particle of a given size with a lower (compared to a core) dielectric constant is always accompanied by an increase in the spectral red shift of the SPR as was shown in the example of melting of ultrafine nanoparticles with a dominating surface contribution. 35 It is notable that the effect of the lightinduced dipole chaotization within the particle surface layer related to local anisotropy affects the local value of the dielectric constants of the material in this layer. This may underlie the intrinsic concurrent mechanism to the red shifts in ultrafine nanoparticles in contrast to the retardation and increasing the inertial mass effects, prevailing for larger nanoparticles.…”

Section: ■ Discussionmentioning

confidence: 99%

“…21,31−34 The maximum value of the extinction cross section is fitted to the classical results. 35 For all fitting, we assume that the experiments have been performed at room temperature, which we set to 293.15 K.…”

Section: ■ Methodsmentioning

confidence: 99%

Nature of the Anomalous Size Dependence of Resonance Red Shifts in Ultrafine Plasmonic Nanoparticles

et al. 2022

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Plasmonic red shifts of nanoparticles are commonly used in imaging technologies to probe the character of local environments, and the understanding of their dependence on size, shape, and surrounding media has therefore become an important target for research. The red shift of plasmon resonances changes character at about 8−10 nm of size for spherical gold nanoparticles�above this value, the red shift progresses linearly with particle size, while below this size, the red shift changes nonlinearly and more strongly with size. Using an atomistic discrete interaction model, we have studied the special properties of the nanoparticle surface layers and discovered its importance for ultrafine plasmonic nanoparticles and their red shifts. We find that the physical origin for the specific properties inherent to the surface layer of atoms near the nanoparticle boundary is related to the anisotropy of the local environment of atoms in this layer by other atoms. The anisotropy changes the conditions for light-induced nonlocal interactions of neighboring atoms with each other and with the incident radiation compared to the atoms located in the particle core with isotropic nearest surroundings by other atoms. The local anisotropy of the nanoparticle crystal lattice is a geometric factor that increases toward its boundary and that is the most fundamental factor underlying the physical differences between the nanoparticle surface layer and the core material. It is shown that the inflexion point at 8−10 nm is due to a change in the dominant physical origin of the red shift�from chaotization of atomically light-induced dipoles within the surface layer in the case of ultrafine nanoparticles to retardation effects for large nanoparticles in which the relative volume of the surface layer decreases rapidly to a negligible value with increasing nanoparticle size. The patterns revealed are the basis for predicting the manifestation of surface layer effects in ultrafine plasmonic nanoparticles of different shapes and composed of different plasmonic materials.

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