Imaging of THz Photonic Modes by Scattering Scanning Near-Field Optical Microscopy.

We investigated the near-field distribution associated to the photonic mode of terahertz photonic micro-resonators by scattering scanning near-field optical microscopy. Probing individual THz micro-resonators concentrating electric fields is important for high-sensitivity chemical and biochemical sensing and fundamental light-matter interactions studies at the nanoscale. We imaged both electric field concentration predicted by numerical simulations and unexpected patterns that deviate from intuitive assumptions. We propose a scenario based on the combination of the near-field with the far-field pattern of the probe/resonator ensemble that is in excellent agreement with the experimental data and propose an image analysis procedure to recover the near-field of such structures.

On the influence of water on THz vibrational spectral features of molecular crystals.

The nanoscale structure of molecular assemblies plays a major role in many (µ)-biological mechanisms. Molecular crystals are one of the most simple of these assemblies and are widely used in a variety of applications from pharmaceuticals and agrochemicals, to nutraceuticals and cosmetics. The collective vibrations in such molecular crystals can be probed using terahertz spectroscopy, providing unique characteristic spectral fingerprints. However, the association of the spectral features to the crystal conformation, crystal phase and its environment is a difficult task. We present a combined computational-experimental study on the incorporation of water in lactose molecular crystals, and show how simulations can be used to associate spectral features in the THz region to crystal conformations and phases. Using periodic DFT simulations of lactose molecular crystals, the role of water in the observed lactose THz spectrum is clarified, presenting both direct and indirect contributions. A specific experimental setup is built to allow the controlled heating and corresponding dehydration of the sample, providing the monitoring of the crystal phase transformation dynamics. Besides the observation that lactose phases and phase transformation appear to be more complex than previously thought - including several crystal forms in a single phase and a non-negligible water content in the so-called anhydrous phase - we draw two main conclusions from this study. Firstly, THz modes are spread over more than one molecule and require periodic computation rather than a gas-phase one. Secondly, hydration water does not only play a perturbative role but also participates in the facilitation of the THz vibrations.