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Nanoantennas for light enhance light-matter interaction at the nanoscale making them useful in optical communication, sensing, and spectroscopy. So far nanoantenna engineering has been largely based on rules derived from the radio frequency domain which neglect the inertia of free metal electrons at optical frequencies causing phenomena such as complete field penetration, ohmic losses and plasmon resonances. Here we introduce a general and scalable evolutionary algorithm that accounts for topological constrains of the fabrication method and therefore yields unexpected nanoantenna designs exhibiting strong light localization and enhancement which can directly be "printed" by focused-ion beam milling. The fitness ranking in a hierarchy of such antennas is validated experimentally by two-photon photoluminescence. Analysis of the best antennas' operation principle shows that it deviates fundamentally from that of classical radio wave-inspired designs. Our work sets the stage for a widespread application of evolutionary optimization to a wide range of problems in nano photonics., Comment: 3 figures; please see the supplementary information for additional data

The soft character of organic materials leads to strong coupling between molecular nuclear and electronic dynamics. This coupling opens the way to control charge transport in organic electronic devices by inducing molecular vibrational motions. However, despite encouraging theoretical predictions, experimental realization of such control has remained elusive. Here we demonstrate experimentally that photoconductivity in a model organic optoelectronic device can be controlled by the selective excitation of molecular vibrations. Using an ultrafast infrared laser source to create a coherent superposition of vibrational motions in a pentacene/C60 photoresistor, we observe that excitation of certain modes in the 1500-1700 cm$^{-1}$ region leads to photocurrent enhancement. Excited vibrations affect predominantly trapped carriers. The effect depends on the nature of the vibration and its mode-specific character can be well described by the vibrational modulation of intermolecular electronic couplings. Vibrational control thus presents a new tool for studying electron-phonon coupling and charge dynamics in (bio)molecular materials.

The design of nano-antennas is so far mainly inspired by radio-frequency technology. However, material properties and experimental settings need to be reconsidered at optical frequencies, which entails the need for alternative optimal antenna designs. Here a checkerboard-type, initially random array of gold cubes is subjected to evolutionary optimization. To illustrate the power of the approach we demonstrate that by optimizing the near-field intensity enhancement the evolutionary algorithm finds a new antenna geometry, essentially a split-ring/two-wire antenna hybrid which surpasses by far the performance of a conventional gap antenna by shifting the n=1 split-ring resonance into the optical regime., Comment: Also see Supplementary material, as attached to the main paper