Localized surface plasmons (LSPs) in metal nanostructures have attracted much attentionfor their role in generating non-equilibrium hot carriers (HCs) for photochemistry 1-3 , photodetection 4,5 and photoluminescence 6 . In addition to optical excitation, LSPs and HC dynamics can be driven electrically via inelastic tunneling. LSP-mediated light emission in tunnel junctions 7-13 commonly features photon energies below the threshold set by the applied voltage bias. Recent work [14][15][16][17][18] has reported photon energies significantly above that threshold, while the underlying physical origin remains elusive. Proposed mechanisms include higher-order electron-plasmon and electron-electron interactions 15,17-20 , and blackbody radiation of hot electrons 16,21 . We report measurements of light emission in tunnel junctions of different plasmonic materials and reveal that HCs generated by nonradiative decay of electrically excited plasmons play a key role in above-threshold light emission. We observed the crossover from above-to below-threshold light emission regime by controlling the tunneling current. There is a giant material dependence of the photon yield, as much as four orders of magnitude, much greater than the plasmon-enhanced radiative efficiency of the tunneling gap. The spectral features of light emission are consistent with a proposed mechanism that incorporates the plasmonic field enhancement and a non-equilibrium HC distribution parametrized by a bias-dependent Boltzmann factor. The effective temperatures of HCs are found to correlate with the bias voltage, rather than the dissipated electrical power. Electrically driven HC generation (above 2000 K under modest voltage) and plasmon-enhanced light emission could open new strategies for chemistry, optoelectronics and quantum optics.Electrically driven light emission from tunnel junctions is of great interest for a variety of technologies requiring efficient optoelectronic integration and conversion at the nanoscale, such

Atomic-sized plasmonic tunnel junctions are of fundamental interest, with great promise as the smallest on-chip light sources in various optoelectronic applications. Several mechanisms of light emission in electrically driven plasmonic tunnel junctions have been proposed, from single-electron or higher-order multielectron inelastic tunneling to recombination from a steady-state population of hot carriers. By progressively altering the tunneling conductance of an aluminum junction, we tune the dominant light emission mechanism through these possibilities for the first time, finding quantitative agreement with theory in each regime. Improved plasmonic resonances in the energy range of interest increase photon yields by 2 orders of magnitude. These results demonstrate that the dominant emission mechanism is set by a combination of tunneling rate, hot carrier relaxation time scales, and junction plasmonic properties.

The electronic Seebeck response in a conductor involves the energy-dependent mean free path of the charge carriers and is affected by crystal structure, scattering from boundaries and defects, and strain. Previous photothermoelectric (PTE) studies have suggested that the thermoelectric properties of polycrystalline metal nanowires are related to grain structure, although direct evidence linking crystal microstructure to the PTE response is difficult to elucidate. Here, we show that room temperature scanning PTE measurements are sensitive probes that can detect subtle changes in the local Seebeck coefficient of gold tied to the underlying defects and strain that mediate crystal deformation. This connection is revealed through a combination of scanning PTE and electron microscopy measurements of single-crystal and bicrystal gold microscale devices. Unexpectedly, the photovoltage maps strongly correlate with gradually varying crystallographic misorientations detected by electron backscatter diffraction. The effects of individual grain boundaries and differing grain orientations on the PTE signal are minimal. This scanning PTE technique shows promise for identifying minor structural distortions in nanoscale materials and devices.

Plasmonic-based photodetectors are receiving increased attention because simple structural changes can make the photodetectors spectrally sensitive. In this study, asymmetric gold nanostructures are used as simple structures for photodetection via the photothermoelectric response. These single metal photodetectors use localized optical absorption from plasmon resonances of gold nanowires at desired wavelengths to generate temperature gradients. Combined with a geometry-dependent Seebeck coefficient, the result is a net electrical signal when the whole geometry is illuminated, with spectral sensitivity and polarization dependence from the plasmon resonances. We show experimental results and simulations of single-wavelength photodetectors at two wavelengths in the near IR range: 785 and 1060 nm. Based on simulation results and a model for the geometry-dependent Seebeck response, we demonstrate a photodetector structure that generates polarization-sensitive responses of opposite signs for the two wavelengths. The experimental photothermoelectric results are combined with simulations to infer the geometry dependence of the Seebeck response. These results can be used to increase the responsivity of these photodetectors further.

Tunneling metal–insulator–metal (MIM) junctions can exhibit an open-circuit photovoltage (OCPV) response under illumination that may be useful for photodetection. One mechanism for photovoltage generation is hot carrier tunneling, in which photoexcited carriers generate a net photocurrent that must be balanced by a drift current in the open-circuit configuration. We present experiments in electromigrated planar MIM structures, designed with asymmetric plasmonic properties using Au and Pt electrodes. Decay of optically excited local plasmonic modes preferentially creates hot carriers on the Au side of the junction, leading to a clear preferred directionality of the hot electron photocurrent and hence a preferred polarity of the resulting OCPV. In contrast, in an ensemble of symmetric devices constructed from only Au, polarity of the OCPV has no preferred direction.