Plasmon-driven sub-picosecond breathing of metal nanoparticles

Bonafé, Franco P.; Aradi, Bálint; Guan, Mengxue; Douglas-Gallardo, Oscar A.; Lian, Chao; Meng, Sheng; Frauenheim, Thomas; Sánchez, Cristián G.

doi:10.1039/c7nr04536k

Cited by 35 publications

(39 citation statements)

References 40 publications

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“…Finally, a classical description of plasmons is less appropriate in the limit of low plasmon densities, where their quantized character must be captured [23][24][25] . Other groups have employed first-principles realtime time-dependent density-functional theory (TDDFT) to study plasmon 26,27 and hot carrier properties in small metallic nanoparticles 21,[28][29][30] . While this method allows the study of nonlinear properties and scales favorably with the system size, it does not include a quantized treatment of the plasmon.…”

Section: Introductionmentioning

confidence: 99%

Single plasmon hot carrier generation in metallic nanoparticles

2019

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Hot carriers produced from the decay of localized surface plasmons in metallic nanoparticles are intensely studied because of their optoelectronic, photovoltaic and photocatalytic applications. From a classical perspective, plasmons are coherent oscillations of the electrons in the nanoparticle, but their quantized nature comes to the fore in the novel field of quantum plasmonics. In this work, we introduce a quantum-mechanical material-specific approach for describing the decay of single quantized plasmons into hot electrons and holes.We find that hot carrier generation rates differ significantly from semiclassical predictions.We also investigate the decay of excitations without plasmonic character and show that their hot carrier rates are comparable to those from the decay of plasmonic excitations for small nanoparticles. Our study provides a rigorous and general foundation for further development of plasmonic hot carrier studies in the plasmonic regime required for the design of ultrasmall devices. arXiv:1904.03697v1 [cond-mat.mes-hall]

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Section: Introductionmentioning

confidence: 99%

Single plasmon hot carrier generation in metallic nanoparticles

2019

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“…In a similar fashion to that presented inRef 46, the smallest clusters (55 and 147 atoms) present several absorption bands, so the assignment of the dipolar SPR band is rather arbitrary because in this range of size there exist a blurry transition between molecular and plasmonic properties. On the other hand, the simulation of photophysical and photodynamic features of icosahedral silver nanoclusters by means of the theoretical approach here employed, has been extensively described in our previous publications 48,49. The optical absorption spectra of the silver nonoclusters are presented in the right panel ofFigure 1, in this case a pronounced increase of the absorption intensity and a red-shift of the dipolar SPR band peak position can be clearly observed.…”

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confidence: 96%

Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters

et al. 2019

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In the last thirty years, the study of plasmonic properties of noble metal nanostructures has become a very dynamic research area. The design and manipulation of matter in the nanometric scale demand a deep understanding of the underlying physico-chemical processes that operate in this size regimen. Here, a fully atomistic study of the spectroscopic and photodynamic properties of different icosahedral silver and gold nanoclusters have been carried out by using Time-Dependent Density Functional Tight-Binding (TD-DFTB) model. Optical absorption spectra of different icosahedral silver and gold nanoclusters of diameters between 1 and 4 nanometers has been simulated. Furthermore, the energy absorption process have been quantified by means of calculating a fully quantum absorption cross-section using the information contained in the reduced single-electron density matrix. This approach allows us take into account for the quantum confinement effects dominating in this size regime. Likewise, the plasmon-induced hot-carrier generation process under laser illuminations have been explored from a fully dynamical perspective. We have found noticeable differences in the energy absorption mechanisms and the plasmon-induced hot-carrier generation process in both metals which can be explained by their respective electronic structures.These difference can be attributed to the existence of ultra-fast electronic dissipation channels in gold nanoclusters that are absented in silver nanoclusters. To the best of our knowledge, this is the first report that addresses this topic from a real time fully atomistic time-dependent approach.

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“…In the case of silver, an elegant application of DFTB was conducted by Douglas-Gallardo et al who tried to rationalize the impact of two adsorbates, water and 1,4-benzoquinone, on the surface plasmon resonance (SPR) band of silver particles of various sizes [300]. This study was a continuation of a previous work devoted to bare icosahedral silver nanoparticles undergoing strong laser pulses [301]. The characteristic of this SPR band, in particular excitation energy and line width, are key in the application of plasmonic particles.…”

Section: Functionalized Clustersmentioning

confidence: 95%

“…Another promising application of DFTB for large metal NPs concerns plasmonics [300,301,368]. For instance, the sub-picosecond breathing-like radial oscillations following a laser pulse excitation have been evidenced for silver NPs up to 309 atoms [301].…”

Section: Dynamics In Excited Statesmentioning

confidence: 99%

Density-functional tight-binding: basic concepts and applications to molecules and clusters

Spiegelman

Tarrat

Cuny

et al. 2020

Advances in Physics: X

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The scope of this article is to present an overview of the Density Functional based Tight Binding (DFTB) method and its applications. The paper introduces the basics of DFTB and its standard formulation up to second order. It also addresses methodological developments such as third order expansion, inclusion of non-covalent interactions, schemes to solve the self-interaction error, implementation of long-range short-range separation, treatment of excited states via the time-dependent DFTB scheme, inclusion of DFTB in hybrid high-level/low level schemes (DFT/DFTB or DFTB/MM), fragment decomposition of large systems, large scale potential energy landscape exploration with molecular dynamics in ground or excited states, nonadiabatic dynamics. A number of applications are reviewed, focusing on -(i)-the variety of systems that have been studied such as small molecules, large molecules and biomolecules, bare or functionalized clusters, supported or embedded systems, and -(ii)-properties and processes, such as vibrational spectroscopy, collisions, fragmentation, thermodynamics or non-adiabatic dynamics. Finally outlines and perspectives are given. ARTICLE HISTORY

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Plasmon-driven sub-picosecond breathing of metal nanoparticles

Cited by 35 publications

References 40 publications

Single plasmon hot carrier generation in metallic nanoparticles

Single plasmon hot carrier generation in metallic nanoparticles

Plasmon-induced hot-carrier generation differences in gold and silver nanoclusters

Density-functional tight-binding: basic concepts and applications to molecules and clusters

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