Confirming a Predicted Selection Rule in Inelastic Neutron Scattering Spectroscopy: The Quantum Translator-Rotator<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">H</mml:mi><mml:mn>2</mml:mn></mml:msub></mml:math>Entrapped Inside<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mi mathvariant="normal">C</mml:mi><mml:mn>60</mml:mn></mml:msub></mml:math>

Xu, Mengjia; Jiménez‐Ruiz, Mónica; Johnson, Mark R.; Rols, S.; Ye, Shufeng; Carravetta, Marina; Denning, Mark S.; Lei, Xuegong; Bačić, Zlatko; Horsewill, A.J.

doi:10.1103/physrevlett.113.123001

Cited by 28 publications

(12 citation statements)

References 23 publications

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“…For example, several nanoconfined molecules exhibit new set of states, as a result of strong couplings between rotational and translational motions, and new selection rules have been applied to identify observed spectral peaks with respect to those of an isolated molecule. 27,31 Although, much has been learned about characterizing quantum confinement of molecular nuclear motion, several aspects of these features are still not fully understood. This is the case of the endohedral water fullerene (H 2 O@C 60 ) complex, which has been recently synthesized, 25 and then characterized spectroscopically by INS, FIR and NMR techniques.…”

Section: Introductionmentioning

confidence: 99%

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀

Valdés

Carrillo‐Bohórquez

Prosmiti

2018

J. Chem. Theory Comput.

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We implemented a systematic procedure for treating the quantal rotations by including all translational and vibrational degrees of freedom for any triatomic bent molecule in any embedded or confined environment, within the MCTDH framework.Fully coupled quantum treatments were employed to investigate unconventional properties in nanoconfined molecular systems. In this way, we facilitate a complete theoretical analysis of the underlying dynamics, that enables to compute the energy levels and the nuclear spin isomers of a single water molecule trapped in a C 60 fullerene cage.The key point lies on the full 9D description of both nuclear and electronic degrees of freedom, as well as a reliable representation of the guest-host interaction. The presence of occluded impurities or inhomogeneities due to noncovalent interactions in the inter-fullerene environment could modify aspects of the potential, causing significant * To whom correspondence should be addressed coupling between otherwise uncoupled modes. Using specific n-mode model potentials, we obtained splitting patterns, that confirm the effects of symmetry breaking observed by experiments in the ground ortho-H 2 O state. Further, our investigation reveals that the first rotationally excited states of the encapsulated ortho-and para-H 2 O have also raised their three-fold degeneracy. In view of the complexity of the problem our results highlight the importance of accurate and computational demanding approaches for building up predictive models for such nanoconfined molecules.

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Section: Introductionmentioning

confidence: 99%

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀

Valdés

Carrillo‐Bohórquez

Prosmiti

2018

J. Chem. Theory Comput.

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“…In the 3 He case, an NMR signal of He 3 was observed [62]. Another practical method for detecting such complexes is the rotational-vibrational spectroscopy, which allows some nonstandard peculiarities in the spectra to be revealed [63]. In 1997, Saunders et al experimentally observed He 2 @C 60 [64] (see also works [65,66]); and, later, Ng @C 60 with = 2 [67][68][69][70].…”

Section: Aristotlementioning

confidence: 99%

On the Problem of He–He Bond in the Endohedral Fullerene He2@C60

2018

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For more than twenty years, the endohedral fullerene cavity is attracting a permanent attention of experimenters and theorists, computational chemists and physicists, who apply their efforts to simulate encapsulated atoms and molecules in the fullerene cavity on computers and analyze the arising phenomena of atomic bonding. In this work, recent developments concerning the endohedral fullerene He2@C60, in particular, its experimental observation and relevant computational works, are reviewed. On the one hand, the dihelium He2 embedded into the C60 cavity is observed experimentally. On the other hand, the computer simulation shows that each of the He atoms is characterized by an insignificant charge transfer to C60, so that the He dimer exists as a partially charged (He + )2 entity. The key issue of the work concerns the existence of a bond between those two helium atoms. Since the bond is created between two particles, we assert that it suffices to define the bond on the basis of the molecular Löwdin's postulate and use it to study the He dimer in the C60 cavity in terms of the He-He potential energy well. It was analytically demonstrated that this well can contain at least one bound (ground) state. Therefore, according to Löwdin's postulate, which is naturally anticipated in quantum theory, the conclusion is drawn that the (He + )2 entity is a diatomic molecule, in which two heliums are bound with each other. On the basis of those arguments, the concept of endohedral fullerene stability is proposed to be extended. K e y w o r d s: fullerene, endohedral fullerene, He@C60, He2@C60, bond, molecule, Löwdin's postulate.

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“…The carbon atom can be inside or outside the cage, and different spectra exist for these different spatial regions. Although this system is a very simple one, it has practical relevance in that the trapping of various atoms and molecules within fullerene cages is currently being investigated with a range of applications in mind, from drug delivery [23][24][25], to nanomaterials design [26], and to a new type of trap for single atom physics experiments [27].…”

Section: Equation Although In 1912mentioning

confidence: 99%

Quantum Bound States in a C–C60 System

Adam

Sofianos

2015

Few-Body Syst

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We investigate the quantum mechanical system of a carbon "test atom" in the proximity of a C60 molecule, both inside and outside the fullerene "cage". Two sets of bound states are found to exist, a deeply bound set inside the cage and another weakly bound set outside it. Tunnelling between these regions is highly unlikely to happen because of the extreme height and width of the potential barrier. However, we predict that a layer of atoms could be adsorbed onto C60 by forming a quantum mechanical bound state, with the adsorbed atoms being concentrated above the "panels" of the buckyball, consistent with "bucky onions" observed experimentally. Until now analysis of such fullerene systems has been via classical mechanics, but a quantum approach reveals new insights. BackgroundSince 1970, when Henson proposed the buckminsterfullerene structure [1], major strides have been made in the field. The compound was first identified by Iijima in 1980 [2] and synthesized in 1985 [3], the latter work resulting in the 1996 Nobel Prize for Chemistry. Fullerenes have attracted wide interest over the past 30 years, for both fundamental and practical reasons, in fields as diverse as geology [4], astronomy [5] and medicine [6]. Very recently the field has diversified yet further, with the synthesis of an all boron fullerene [7].Although it may be surmised that systems containing C60 molecules are too "large" to sustain quantum effects, the observation of Arndt et al. [8], namely the measurement of a quantum interference pattern produced by C60 molecules passing through a diffraction grating, contradicts this. Despite the large number of degrees of freedom (180 for a single C60 molecule) and the associated high probability of decoherence, diffraction was observed. Molecules of the size and complexity of C60 evidently lie in a zone between classical and quantum systems. Although this fact is indeed of fundamental interest, our motivation for undertaking this investigation was to determine whether the Schrödinger equation would yield useful insights into the properties of simple C60 cluster systems. The mechanics of such systems is traditionally analyzed via classical techniques based on the Euler-Lagrange equations (see, for example, Refs. [9][10][11]). The extension to finite temperature and thereby thermodynamical functions is made via the Nosé-Hoover Hamiltonian [12,13].The advantage that a quantum mechanical approach has over corresponding classical techniques is that, for bound states, the condition of normalization imposes tremendous restrictions on the solutions to the Schrödinger Electronic supplementary material The online version of this article (

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Confirming a Predicted Selection Rule in Inelastic Neutron Scattering Spectroscopy: The Quantum Translator-RotatorH2Entrapped InsideC60

Cited by 28 publications

References 23 publications

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀

On the Problem of He–He Bond in the Endohedral Fullerene He2@C60

Quantum Bound States in a C–C60 System

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Confirming a Predicted Selection Rule in Inelastic Neutron Scattering Spectroscopy: The Quantum Translator-RotatorH2Entrapped InsideC60

Cited by 28 publications

References 23 publications

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C60

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C60

On the Problem of He–He Bond in the Endohedral Fullerene He2@C60

Quantum Bound States in a C–C60 System

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Product

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Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀

Fully Coupled Quantum Treatment of Nanoconfined Systems: A Water Molecule inside a Fullerene C₆₀