Quantum mechanical effects in plasmonic structures with subnanometre gaps

Zhu, Wenqi; Esteban, Rubén; Borisov, Andrei G.; Baumberg, Jeremy J.; Nordlander, Peter; Lezec, Henri J.; Aizpurua, Javier; Crozier, Kenneth B.

doi:10.1038/ncomms11495

Cited by 691 publications

(685 citation statements)

References 134 publications

(264 reference statements)

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“…Additionally, we experimentally determined the adsorption site area of malachite green to be approximately 2.19 nm 2 , where the average moleculemolecule distance is 1.14 nm. Although these molecules are potentially within the strong coupling regime, 69 we believe the overall spectra are dominated by the plasmon/molecule coupling as evidenced by our good agreement with experiment. For smaller NP's (i.e., < 50 nm), higher site densities, or molecules with higher oscillator strengths, we suspect that the molecule/molecule interaction will play a more important role in the coupling.…”

Section: Parametrizing Monolayer Of Quantum Moleculessupporting

confidence: 72%

Capturing Plasmon–Molecule Dynamics in Dye Monolayers on Metal Nanoparticles Using Classical Electrodynamics with Quantum Embedding

Smith¹,

Karam

Haber³

et al. 2017

J. Phys. Chem. C

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A multi-scale hybrid quantum/classical approach using classical electrodynamics and a collection of discrete three-level quantum systems is used to simulate the coupled dynamics and spectra of a malachite green monolayer adsorbed to the surface of a spherical gold nanoparticle (NP). This method utilizes finite difference time domain (FDTD) to describe the plasmonic response of the NP within the main FDTD framework and a three-level quantum description for the molecule via a Maxwell/Liouville framework.To avoid spurious self-excitation, each quantum molecule has its own auxiliary FDTD subregion embedded within the main FDTD grid. The molecular parameters are determined by fitting the experimental extinction spectra to Lorentzians, yielding the energies, transition dipole moments, and the dephasing lifetimes. This approach can be potentially applied to modeling thousands of molecules on the surface of a plasmonic NP. In this paper, however, we first present results for two molecules with scaled oscillator strengths to reflect the optical response of a full monolayer. There is good agreement with experimental extinction measurements, predicting the plasmon and molecule depletions. Additionally, this model captures the polariton peaks overlapped with a Fano-type resonance profile observed in the experimental extinction measurements. This technique can be generalized to any nanostructure/multi-chromophore system, where the molecules can be treated with essentially any quantum method.

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Section: Parametrizing Monolayer Of Quantum Moleculessupporting

confidence: 72%

Capturing Plasmon–Molecule Dynamics in Dye Monolayers on Metal Nanoparticles Using Classical Electrodynamics with Quantum Embedding

Smith¹,

Karam

Haber³

et al. 2017

J. Phys. Chem. C

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“…It has recently been reported that the localized plasmons in multiple metal nanostructures reveal interesting phenomena, such as a red-shift of the surface plasmon frequency, large enhancement of the local electric fields, the nonlocal quantum effects and the quantum tunneling effects between the metal nanostructures [5][6][7][8][9][10][11][12].…”

Section: Introductionmentioning

confidence: 99%

Differential Equations for Localized Plasmons in the Random Phase Approximation

Ichikawa

2017

e-J. Surf. Sci. Nanotech.

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Differential equations are derived for localized bulk and surface plasmons in metal nanostructures in the random phase approximation (RPA) at the high frequency condition. A differential equation for the scalar potential in the RPA gives a position-dependent Drude-like dielectric function. Using the dielectric function, a differential equation for the vector potential is derived in the Lorentz gauge. A corrected RPA differential equation for the scalar potential is then derived by using the differential equation for the vector potential and the Lorentz condition. The vector potential contribution to the electric field in the Lorentz gauge is found negligible compared with the scalar potential one in metal nanostructures. This indicates that the scalar potential plays important roles in analyzing the localized plasmons in metal nanostructures as reported previously. The corrected RPA differential equations are found equivalent to the Maxwell equations using the position-dependent Drude-like dielectric function.

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“…At the distances between metal particles smaller than few nanometers, the nonlocal response of metals [31] and electron tunnelling effect [36] between the particles become important. Thus, it is expected that, at the distances between emitter and metal surface of 0.5-2 nm, the nonlocality in the metal response is also sensitive.…”

Section: Resultsmentioning

confidence: 99%

Fluorescence of molecules placed near a spherical particle: Rabi splitting

Dvoynenko¹

2017

Semicond. Phys. Quantum Electron. Optoelectron.

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Abstract. Theoretical study of spontaneously emitted spectra of point-like source placed near spherical Ag particle was performed. It was shown that near-field electromagnetic interaction between a point-like emitter and spherical Ag particle leads to strong coupling between them at very small emitter-metal surface distances. It was shown that values of Rabi splitting are quantitatively close to that of emitter-flat substrate interaction.

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Quantum mechanical effects in plasmonic structures with subnanometre gaps

Cited by 691 publications

References 134 publications

Capturing Plasmon–Molecule Dynamics in Dye Monolayers on Metal Nanoparticles Using Classical Electrodynamics with Quantum Embedding

Capturing Plasmon–Molecule Dynamics in Dye Monolayers on Metal Nanoparticles Using Classical Electrodynamics with Quantum Embedding

Differential Equations for Localized Plasmons in the Random Phase Approximation

Fluorescence of molecules placed near a spherical particle: Rabi splitting

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