Plasmonics aims to interface photonics and electronics. Finding optical, near-field analogues of much used electro-technical components is crucial to the success of such a platform. Here we present the plasmonic analogue of a non-reciprocal antenna.
For non-reciprocality in a plasmonic context, the optical excitation and emission resonances of the antenna need to be an orthogonal set. We show that nonlinear excitation of metal nanoantennas creates a sufficient shift between excitation and emission wavelengths that they can be interpreted as decoupled, allowing for independent tuning of excitation and emission properties along different spatial dimensions. This leads, for given excitation wavelength and polarization, to independent optimization of emission intensity, frequency spectrum, polarization and angular spectrum. Non-reciprocal optical antennas of both gold and aluminum are characterized and shown to be useful as e.g. nonlinear signal transducers or nanoscale sources of widely tunable light.
Coherent broadband excitation of plasmons brings ultrafast photonics to the nanoscale. However, to fully leverage this potential for ultrafast nanophotonic applications, the capacity to engineer and control the ultrafast response of a plasmonic syste
m at will is crucial. Here, we develop a framework for systematic control and measurement of ultrafast dynamics of near-field hotspots. We show deterministic design of the coherent response of plasmonic antennas at femtosecond timescales. Exploiting the emerging properties of coupled antenna configurations, we use the calibrated antennas to engineer two sought-after applications of ultrafast plasmonics: a subwavelength resolution phase shaper, and an ultrafast hotspot switch. Moreover, we demonstrate that mixing localized resonances of lossy plasmonic particles is the mechanism behind nanoscale coherent control. This simple, reproducible and scalable approach promises to transform ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid state physics and quantum biology.
Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest
in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assemblies. However, single-molecule techniques to access ultrafast coherences at physiological conditions were not available so far. Here we show by employing femtosecond pulse-shaping techniques that quantum coherences in single organic molecules can be created, probed, and manipulated at ambient conditions even in highly disordered solid environments. We find broadly distributed coherence decay times for different individual molecules giving direct insight into the structural heterogeneity of the local surroundings. Most importantly, we induce Rabi-oscillations and control the coherent superposition state in a single molecule, thus performing a basic femtosecond single-qubit operation at room temperature.
