Hiding in the crowd: Spectral signatures of overcoordinated hydrogen bond environments

• DOI: 10.48550/arxiv.1906.08897
• Publication Date: 2019-01-01
• Authors: Tobias Morawietz; Andrés S. Urbina; Patrick K. Wise; Xiangen Wu; Wanjun Lu; Dor Ben‐Amotz; Thomas E. Markland
• Keywords: Supercooling; Liquid water

Molecules with an excess number of hydrogen-bonding partners play a crucial role in fundamental chemical processes, ranging from the anomalous diffusion supercooled water to transport aqueous proton defects and ordering around hydrophobic solutes. Here we show that overcoordinated hydrogen bond environments can be identified both ambient regimes liquid by combining experimental Raman multivariate curve resolution measurements machine learning accelerated quantum simulations. In particular, find OH groups appearing spectral regions usually associated non-hydrogen-bonded species actually correspond bonds formed environments. We further only these exhibit turnover population as function temperature, which is robust persists under constant pressure density conditions. This work thus provides new tool identify, interpret, elucidate signatures crowded networks.