2022/01/01 by Sergey Mitryukovskiy, Danny E. P. Vanpoucke, Danny Vanpoucke +7 · 25 citations
Chemistry · Engineering · Physics and Astronomy · #Acoustic Wave Resonator Technologies #Chemical physics #Chemistry #Computational chemistry #Crystal (programming language) #Crystallography #Materials science #Molecular Spectroscopy and Structure #Molecular dynamics #Molecular vibration #Molecule #Optoelectronics #Organic chemistry #Phase (matter) #Physics #Spectroscopy #Terahertz radiation #Terahertz technology and applications #physics.chem-ph #physics.optics
paper · pdf · open access · doi:10.1039/d1cp03261e
published in Physical Chemistry Chemical Physics 24(10), 6107-6125 (Royal Society of Chemistry)
openalex publication_date 2022/01/01 · arxiv created 2022/02/22 · arxiv updated 2022/03/23 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/06
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 computationalexperimental 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 thoughtincluding several crystal forms in a single phase and a non-negligible water content in the so-called anhydrous phasewe 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.