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

Authors
  • Zhukov, Sergey S.1
  • Balos, Vasileios2
  • Hoffman, Gabriela3
  • Alom, Shamim3
  • Belyanchikov, Mikhail1
  • Nebioglu, Mehmet4
  • Roh, Seulki4
  • Pronin, Artem4
  • Bacanu, George R.3
  • Abramov, Pavel1
  • Wolf, Martin2
  • Dressel, Martin1, 4
  • Levitt, Malcolm H.3
  • Whitby, Richard J.3
  • Gorshunov, Boris1
  • Sajadi, Mohsen2, 5
  • 1 Moscow Institute of Physics and Technology, Moscow, Russia , Moscow (Russia)
  • 2 Fritz-Haber-Institut der MPG, Berlin, Germany , Berlin (Germany)
  • 3 University of Southampton, Southampton, UK , Southampton (United Kingdom)
  • 4 Universität Stuttgart, Stuttgart, Germany , Stuttgart (Germany)
  • 5 University of Paderborn, Paderborn, Germany , Paderborn (Germany)
Type
Published Article
Journal
Scientific Reports
Publisher
Springer Nature
Publication Date
Oct 27, 2020
Volume
10
Issue
1
Identifiers
DOI: 10.1038/s41598-020-74972-3
Source
Springer Nature
License
Green

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.

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