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Rotational coherence of encapsulated ortho and para water in fullerene-C60 revealed by time-domain terahertz spectroscopy

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Balos,  Vasileios
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Sajadi,  Mohsen
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Chemistry, University of Paderborn;

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Citation

Zhukov, S. S., Balos, V., Hoffman, G., Alom, S., Belyanchikov, M., Nebioglu, M., et al. (2020). Rotational coherence of encapsulated ortho and para water in fullerene-C60 revealed by time-domain terahertz spectroscopy. Scientific Reports, 10(1): 18329. doi:10.1038/s41598-020-74972-3.


Cite as: https://hdl.handle.net/21.11116/0000-0008-0FF9-0
Abstract
We resolve the real-time coherent rotational motion of isolated water molecules encapsulated in fullerene-C60 cages by time-domain terahertz (THz) spectroscopy. We employ single-cycle THz pulses to excite the low-frequency rotational motion of water and measure the subsequent coherent emission of electromagnetic waves by water molecules. At temperatures below ~ 100 K, C60 lattice vibrational damping is mitigated and the quantum dynamics of confined water are resolved with a markedly long rotational coherence, extended beyond 10 ps. The observed rotational transitions agree well with low-frequency rotational dynamics of single water molecules in the gas phase. However, some additional spectral features with their major contribution at ~2.26 THz are also observed which may indicate interaction between water rotation and the C60 lattice phonons. We also resolve the real-time change of the emission pattern of water after a sudden cooling to 4 K, signifying the conversion of ortho-water to para-water over the course of 10s hours. The observed long coherent rotational dynamics of isolated water molecules confined in C60 makes this system an attractive candidate for future quantum technology.