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Physisorption of h-2 on fullerenes and the solvation of c-60 by hydrogen clusters at finite temperature: a theoretical assessment

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Calvo, F.
Tekin, A.

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The interaction between hydrogen and carbonaceous nanostructures is of fundamental interest in various areas of physical chemistry. In this contribution we have revisited the physisorption of hydrogen molecules and H-2 clusters on fullerenes, following a first-principles approach in which the interaction is quantitatively evaluated for the C-20 system using high-level electronic structure methods. Relative to coupled cluster data at the level of single, double, and perturbative triple excitations taken as a benchmark, the results for rotationally averaged physisorbed H-2 show a good performance of MP2 variants and symmetry-adapted perturbation theory, but significant deviations and basis set convergence issues are found for dispersion-corrected density functional theory. These electronic structure data are fitted to produce effective coarse-grained potentials for use in larger systems such as C-60-H-2. Using path-integral molecular dynamics, the potentials are also applied to parahydrogen clusters solvated around fullerenes, across the regime where the first solvation shell becomes complete and as a function of increasing temperature. For C-60 our findings indicate a sensible dependence of the critical solvation size on the underlying potential. As the temperature is increased, a competition is found between the surface and radial expansions of the solvation shell, with one molecule popping away at intermediate temperatures but getting reinserted at even higher temperatures.

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American Chemical Society (ACS)

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Chemistry, Chemistry, physical and theoretical, Physics, Atoms, Molecular dynamics

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Journal of Physical Chemistry A

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10.1021/acs.jpca.8b00163

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