NMR Lineshapes and Scalar Relaxation of the Water‐Endofullerene H217O@C60

Elliott, Stuart J.; Bengs, Christian; Kouřil, Karel; Meier, Benno; Alom, Shamim; Whitby, Richard J.; Levitt, Malcolm H.

doi:10.1002/cphc.201701330

Cited by 19 publications

(16 citation statements)

References 34 publications

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“…Scalar relaxation induced by the quadrupolar relaxation of the 17 O nucleus leads to a spectrum that is symmetric but exhibits different linewidths depending on the 17 O spin quantum number. [55] To facilitate rapid dissolution, H 2 17 O@C 60 is predissolved in orthodichlorobenzene. This sample is kept at 4.2 K overnight to enrich the amount of parawater.…”

Section: Methyl Groupsmentioning

confidence: 99%

Quantum‐rotor‐induced polarization

Meier

2018

Magnetic Reson in Chemistry

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Quantum-rotor-induced polarization is closely related to para-hydrogen-induced polarization. In both cases, the hyperpolarized spin order derives from rotational interaction and the Pauli principle by which the symmetry of the rotational ground state dictates the symmetry of the associated nuclear spin state. In quantum-rotor-induced polarization, there may be several spin states associated with the rotational ground state, and the hyperpolarization is typically generated by hetero-nuclear cross-relaxation. This review discusses preconditions for quantum-rotor-induced polarization for both the 1-dimensional methyl rotor and the asymmetric rotor H O@C , that is, a single water molecule encapsulated in fullerene C . Experimental results are presented for both rotors.

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Section: Methyl Groupsmentioning

confidence: 99%

Quantum‐rotor‐induced polarization

Meier

2018

Magnetic Reson in Chemistry

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“…The high symmetry of the cage allows water to rotate freely, with no perceptible hindering potential. This conclusion has been corroborated by nuclear magnetic resonance 29 , molecular dynamics (MD) simulations 30 and multidimensional quantum calculations of the energy level structure of the encapsulated molecule 31 , 32 . Dielectric measurements of H 2 O@C 60 indicate that the electric dipole moment of water is strongly screened by the cage, leading to a ~fourfold reduction in the effective dipole moment 25 , in good agreement with quantum chemistry calculations 32 .…”

Section: Introductionmentioning

confidence: 68%

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

Zhukov

Balos

Hoffman

et al. 2020

Sci Rep

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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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“…Since then, a number of studies focusing on novel properties of C 60 and its interactions with other species have been carried out. (Ruoff et al, 1993;Diederich and Gómez-López, 1999;Bakry et al, 2007;Mignolet et al, 2013;Wang et al, 2014;Elliott et al, 2018;Kouřil et al, 2018) Some investigations concentrated on medical applications, hydrogen storage, and various endofullerene. (Wang et al, 2013;Srivastava et al, 2016;Srivastava et al, 2017;Elliott et al, 2018;Kouřil et al, 2018).…”

Section: Introductionmentioning

confidence: 99%

“…(Ruoff et al, 1993;Diederich and Gómez-López, 1999;Bakry et al, 2007;Mignolet et al, 2013;Wang et al, 2014;Elliott et al, 2018;Kouřil et al, 2018) Some investigations concentrated on medical applications, hydrogen storage, and various endofullerene. (Wang et al, 2013;Srivastava et al, 2016;Srivastava et al, 2017;Elliott et al, 2018;Kouřil et al, 2018). Due to the fullerene's unique cage-like cavity, a procedure called molecular surgery can be performed to entrap an atom or molecule.…”

Section: Introductionmentioning

confidence: 99%

CO2 Activation Within a Superalkali-Doped Fullerene

2021

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With the aim of finding a suitable synthesizable superalkali species, using the B3LYP/6-31G* density functional level of theory we provide results for the interaction between the buckminsterfullerene C60 and the superalkali Li3F2. We show that this endofullerene is stable and provides a closed environment in which the superalkali can exist and interact with CO2. It is worthwhile to mention that the optimized Li3F2 structure inside C60 is not the most stable C2v isomer found for the “free” superalkali but the D3h geometry. The binding energy at 0 K between C60 and Li3F2 (D3h) is computed to be 119 kJ mol−1. Once CO2 is introduced in the endofullerene, it is activated, and the OCO^ angle is bent to 132°. This activation does not follow the previously studied CO2 reduction by an electron transfer process from the superalkali, but it is rather an actual reaction where a F (from Li3F2) atom is bonded to the CO2. From a thermodynamic analysis, both CO2 and the encapsulated [Li3F2⋅CO2] are destabilized in C60 with solvation energies at 0 K of 147 and < −965 kJ mol−1, respectively.

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NMR Lineshapes and Scalar Relaxation of the Water‐Endofullerene H₂¹⁷O@C₆₀

Cited by 19 publications

References 34 publications

Quantum‐rotor‐induced polarization

Quantum‐rotor‐induced polarization

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

CO2 Activation Within a Superalkali-Doped Fullerene

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