Tuesday, October 27, 2020

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

 

Sergey S. Zhukov, Vasileios Balos, Gabriela Hoffman, Shamim Alom, Mikhail Belyanchikov, Mehmet Nebioglu, Seulki Roh, Artem Pronin, George R. Bacanu, Pavel Abramov, Martin Wolf, Martin Dressel, Malcolm H. Levitt, Richard J. Whitby, Boris Gorshunov,  Mohsen Sajadi 

https://www.nature.com/articles/s41598-020-74972-3

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.

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