Light Emission and Conductance Fluctuations in Electrically Driven and Plasmonically Enhanced Molecular Junctions
arXiv:2307.06876 · doi:10.1021/acsphotonics.4c00291
Abstract
Electrically connected and plasmonically enhanced molecular junctions combine the optical functionalities of high field confinement and enhancement (cavity function), and of high radiative efficiency (antenna function) with the electrical functionalities of molecular transport. Such combined optical and electrical probes have proven useful for the fundamental understanding of metal-molecule contacts and contribute to the development of nanoscale optoelectronic devices including ultrafast electronics and nanosensors. Here, we employ a self-assembled metal-molecule-metal junction with a nanoparticle bridge to investigate correlated fluctuations in conductance and tunneling-induced light emission at room temperature. Despite the presence of hundreds of molecules in the junction, the electrical conductance and light emission are both highly sensitive to atomic-scale fluctuations -- a phenomenology reminiscent of picocavities observed in Raman scattering and of luminescence blinking from photo-excited plasmonic junctions. Discrete steps in conductance associated with fluctuating emission intensities through the multiple plasmonic modes of the junction are consistent with a finite number of randomly localized, point-like sources dominating the optoelectronic response. Contrasting with these microscopic fluctuations, the overall plasmonic and electronic functionalities of our devices feature long-term survival at room temperature and under an electrical bias of a few volts, allowing for measurements over several months.
References in corpus (19)
- Electromigrated nanoscale gaps for surface-enhanced Raman spectroscopy
- Electrically-driven optical antennas
- Continuous-Wave Frequency Upconversion with a Molecular Optomechanical Nanocavity
- Spontaneous hot-electron light emission from electron-fed optical antennas
- Tilt-angle landscapes and temperature dependence of the conductance in biphenyl-dithiol single-molecule junctions
- Conduction mechanisms in biphenyl-dithiol single-molecule junctions
- Optical Probe of Quantum Shot Noise Reduction at a Single-Atom Contact
- Optical antennas driven by quantum tunneling: a key issues review
- Theory of light emission from quantum noise in plasmonic contacts: above-threshold emission from higher-order electron-plasmon scattering
- Electrically Driven Hot-Carrier Generation and Above-threshold Light Emission in Plasmonic Tunnel Junctions
- Over-Bias Light Emission due to Higher Order Quantum Noise of a Tunnel Junction
- Intrinsic Luminescence Blinking from Plasmonic Nanojunctions
- Quantum Coherent Multielectron Processes in an Atomic Scale Contact
- Tuning light emission crossovers in atomic-scale aluminum plasmonic tunnel junctions
- Atomic-scale structural fluctuations of a plasmonic cavity
- Inelastic Light Scattering in the Vicinity of a Single-Atom Quantum Point Contact in a Plasmonic Picocavity
- Structural Order of the Molecular Adlayer Impacts the Stability of Nanoparticle-on-Mirror Plasmonic Cavities
- Infrared light emission from atomic point contacts
- Quantifying efficiency of remote excitation for surface enhanced Raman spectroscopy in molecular junctions