Hot-Electron Intraband Luminescence from Single Hot Spots in Noble-Metal Nanoparticle Films

Haug, Tobias; Klemm, Philippe; Bange, Sebastian; Lupton, John M.

doi:10.1103/physrevlett.115.067403

Cited by 100 publications

(197 citation statements)

References 26 publications

(40 reference statements)

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“…More interestingly, the straight line can be extrapolated to the origin of the coordinate (see , Supporting Information). This is the unique feature of hot‐electron intraband luminescence observed previously in plasmonic hot spots and semiconductor NSs . This result indicates clearly that the broadband luminescence observed for the Ga NSs placed on the thin Ag film in the high excitation irradiance regime belongs to hot‐electron intraband luminescence, similar to blackbody radiation .…”

Section: Resultssupporting

confidence: 79%

Liquid Gallium Nanospheres Emitting White Light

Xiang

Chen

Jiang

et al. 2019

Laser & Photonics Reviews

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Gallium (Ga) is not only a metal possessing surface plasmon resonance in the ultraviolet region but also a phase‐change material with very low melting point. Spherical Ga nanoparticles composed of liquid Ga cores and solid Ga2O3 shells, which exhibit surface plasmonic resonances spanning the ultraviolet to near‐infrared spectral region, are fabricated by using femtosecond laser ablation. Under the excitation of femtosecond laser light, only second harmonic generation is observed in the Ga nanospheres placed on a glass substrate. In sharp contrast, white light emission can be generated in such Ga nanospheres when they are placed on a thin silver film. It is revealed numerically and confirmed experimentally that a Fano resonance originating from the interference between the mirror‐image‐induced magnetic dipole mode and the gap plasmon mode is formed in the backward scattering spectra of the Ga nanospheres. Efficient white light emission can be achieved by resonantly exciting either the magnetic dipole resonance or the Fano resonance. Based on spectral analysis, the white light emission is identified as the hot‐electron intraband luminescence. The fabricated core–shell Ga nanospheres provide an ideal platform on which the optical properties and practical applications of liquid Ga nanoparticles can be systematically investigated.

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Section: Resultssupporting

confidence: 79%

Liquid Gallium Nanospheres Emitting White Light

Xiang

Chen

Jiang

et al. 2019

Laser & Photonics Reviews

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“…Its power dependence is close to quadratic (1.98 ± 0.06) for the spectrally integrated signal as shown in Fig. 1c (black), and exhibits a frequency-dependent power law exponent due to varying spectral shape (see Supplement) in agreement with previous studies [24,25].…”

Section: Fig 1bsupporting

confidence: 90%

Enhanced Third-Order Optical Nonlinearity Driven by Surface-Plasmon Field Gradients

et al. 2018

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Efficient nonlinear optical frequency mixing in small volumes is key for future on-chip photonic devices. However, the generally low conversion efficiency severely limits miniaturization to nanoscale dimensions. Here we demonstrate that gradient-field effects can provide for an efficient, conventionally dipole-forbidden nonlinear response. We show that a longitudinal nonlinear source current can dominate the third-order optical nonlinearity of the free electron response in gold in the technologically important near-IR frequency range where the nonlinearities due to other mechanisms are particularly small. Using adiabatic nanofocusing to spatially confine the excitation fields, from measurements of the 2ω_{1}-ω_{2} four-wave mixing response as a function of detuning ω_{1}-ω_{2}, we find up to 10^{-5} conversion efficiency with a gradient-field contribution to χ_{Au}^{(3)} of up to 10^{-19} m^{2}/V^{2}. The results are in good agreement with the theory based on plasma hydrodynamics and underlying electron dynamics. The associated increase in the nonlinear conversion efficiency with a decreasing sample size, which can even overcompensate the volume decrease, offers a new approach for enhanced nonlinear nano-optics. This will enable more efficient nonlinear optical devices and the extension of coherent multidimensional spectroscopies to the nanoscale.

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“…Hence, it can be very useful to study the dynamics of hot electrons. In metals, this should be useful to analyze luminescence induced by absorption of short pulses [77]. In semiconductors, the possibility of increasing the efficiency of PV cells using hot electrons has motivated many studies of ultrafast dynamics using photoluminescence [78].…”

Section: Discussionmentioning

confidence: 99%

Light Emission by Nonequilibrium Bodies: Local Kirchhoff Law

et al. 2018

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The goal of this paper is to introduce a local form of Kirchhoff law to model light emission by nonequilibrium bodies. While absorption by a finite-size body is usually described using the absorption cross section, we introduce a local absorption rate per unit volume and also a local thermal emission rate per unit volume. Their equality is a local form of Kirchhoff law. We revisit the derivation of this equality and extend it to situations with subsystems in local thermodynamic equilibrium but not in equilibrium between them, such as hot electrons in a metal or electrons with different Fermi levels in the conduction band and in the valence band of a semiconductor. This form of Kirchhoff law can be used to model (i) thermal emission by nonisothermal finite-size bodies, (ii) thermal emission by bodies with carriers at different temperatures, and (iii) spontaneous emission by semiconductors under optical (photoluminescence) or electrical pumping (electroluminescence). Finally, we show that the reciprocity relation connecting light-emitting diodes and photovoltaic cells derived by Rau is a particular case of the local Kirchhoff law.

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Hot-Electron Intraband Luminescence from Single Hot Spots in Noble-Metal Nanoparticle Films

Cited by 100 publications

References 26 publications

Liquid Gallium Nanospheres Emitting White Light

Liquid Gallium Nanospheres Emitting White Light

Enhanced Third-Order Optical Nonlinearity Driven by Surface-Plasmon Field Gradients

Light Emission by Nonequilibrium Bodies: Local Kirchhoff Law

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