Light-induced electronic non-equilibrium in plasmonic particles

Kornbluth, Mordechai; Nitzan, Abraham; Seideman, Tamar

doi:10.1063/1.4802000

Cited by 51 publications

(75 citation statements)

References 75 publications

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“…1(a) and Fig. 5(a); it is described (via the term ∂f ∂t ex ) using an improved version of the Fermi golden rule type form suggested in [18,19,22,38] which here also incorporates explicitly the absorption lineshape of the nanostructure, see Eq. (A9).…”

Section: Modelmentioning

confidence: 99%

“Hot” electrons in metallic nanostructures—non-thermal carriers or heating?

2019

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Understanding the interplay between illumination and the electron distribution in metallic nanostructures is a crucial step towards developing applications such as plasmonic photocatalysis for green fuels, nanoscale photodetection and more. Elucidating this interplay is challenging, as it requires taking into account all channels of energy flow in the electronic system. Here, we develop such a theory, which is based on a coupled Boltzmann-heat equations and requires only energy conservation and basic thermodynamics, where the electron distribution, and the electron and phonon (lattice) temperatures are determined uniquely. Applying this theory to realistic illuminated nanoparticle systems, we find that the electron and phonon temperatures are similar, thus justifying the (classical) single-temperature models. We show that while the fraction of high-energy “hot” carriers compared to thermalized carriers grows substantially with illumination intensity, it remains extremely small (on the order of 10−8). Importantly, most of the absorbed illumination power goes into heating rather than generating hot carriers, thus rendering plasmonic hot carrier generation extremely inefficient. Our formulation allows for the first time a unique quantitative comparison of theory and measurements of steady-state electron distributions in metallic nanostructures.

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Section: Modelmentioning

confidence: 99%

“Hot” electrons in metallic nanostructures—non-thermal carriers or heating?

2019

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“…In order to model this process using our time dependent framework, we assume the existence of hot electrons in the LQC. We borrow an analytical expression for the distribution from our previous work 55,56 to investigate the transient hot-electron dynamics. The electrons in the RQC follow a pure FDD.…”

Section: G Hot-electron Dynamicsmentioning

confidence: 99%

Emergence of Landauer transport from quantum dynamics: A model Hamiltonian approach

Pal

Ramakrishna

Seideman

2018

The Journal of Chemical Physics

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The Landauer expression for computing current-voltage characteristics in nanoscale devices is efficient but not suited to transient phenomena and a time-dependent current because it is applicable only when the charge carriers transition into a steady flux after an external perturbation. In this article, we construct a very general expression for time-dependent current in an electrode-molecule-electrode arrangement. Utilizing a model Hamiltonian (consisting of the subsystem energy levels and their electronic coupling terms), we propagate the Schrödinger wave function equation to numerically compute the time-dependent population in the individual subsystems. The current in each electrode (defined in terms of the rate of change of the corresponding population) has two components, one due to the charges originating from the same electrode and the other due to the charges initially residing at the other electrode. We derive an analytical expression for the first component and illustrate that it agrees reasonably with its numerical counterpart at early times. Exploiting the unitary evolution of a wavefunction, we construct a more general Landauer style formula and illustrate the emergence of Landauer transport from our simulations without the assumption of time-independent charge flow. Our generalized Landauer formula is valid at all times for models beyond the wide-band limit, non-uniform electrode density of states and for time and energy-dependent electronic coupling between the subsystems. Subsequently, we investigate the ingredients in our model that regulate the onset time scale of this steady state. We compare the performance of our general current expression with the Landauer current for time-dependent electronic coupling. Finally, we comment on the applicability of the Landauer formula to compute hot-electron current arising upon plasmon decoherence.

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“…12) are temperature dependent and the anti-Stokes signal rapidly increases upon temperature. This may particularly occur when some intense and/or pulsed laser excitation generates a high-temperature electron gas [54]; however, the signal has still to be interpreted as inelastic light scattering by free carriers [50]. This can even be useful to determine the free-electron gas temperature that can considerably differ from the lattice temperature (deducible for instance from Raman signatures of lattice vibrations).…”

Section: B Spectral Response For Electronic Scatteringmentioning

confidence: 99%

Plasmon-resonant Raman spectroscopy in metallic nanoparticles: Surface-enhanced scattering by electronic excitations

et al. 2015

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Since the discovery of surface-enhanced Raman scattering (SERS) 40 years ago, the origin of the "background" that is systematically observed in SERS spectra has remained questionable. To deeply analyze this phenomenon, plasmon-resonant Raman scattering was recorded under specific experimental conditions on a panel of composite multilayer samples containing noble metal (Ag and Au) nanoparticles. Stokes, anti-Stokes, and wide, including very low, frequency ranges have been explored. The effects of temperature, size (in the nm range), embedding medium (SiO 2 , Si 3 N 4 , or TiO 2 ) or ligands have been successively analyzed. Both lattice (Lamb modes and bulk phonons) and electron (plasmon mode and electron-hole excitations) dynamics have been investigated. This work confirms that in Ag-based nanoplasmonics composite layers, only Raman scattering by single-particle electronic excitations accounts for the background. This latter appears as an intrinsic phenomenon independently of the presence of molecules on the metallic surface. Its spectral shape is well described by revisiting a model developed in the 1990s for analyzing electron scattering in dirty metals, and used later in superconductors. The g s factor, that determines the effective mean-free path of free carriers, is evaluated, g expt s = 0.33 ± 0.04, in good agreement with a recent evaluation based on time-dependent local density approximation g theor s = 0.32. Confinement and interface roughness effects at the nanometer range thus appear crucial to understand and control SERS enhancement and more generally plasmon-enhanced processes on metallic surfaces.

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Light-induced electronic non-equilibrium in plasmonic particles

Cited by 51 publications

References 75 publications

“Hot” electrons in metallic nanostructures—non-thermal carriers or heating?

“Hot” electrons in metallic nanostructures—non-thermal carriers or heating?

Emergence of Landauer transport from quantum dynamics: A model Hamiltonian approach

Plasmon-resonant Raman spectroscopy in metallic nanoparticles: Surface-enhanced scattering by electronic excitations

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