Path integral Monte Carlo calculations of calcium-doped 4He clusters

• Published in: International journal of quantum chemistry 2014-10, Vol.114 (19), p.1318-1326
• Main Authors: Rodríguez-Cantano, Rocío, González-Lezana, Tomás, Villarreal, Pablo, López-Durán, David, Gianturco, Franco A., Delgado-Barrio, Gerardo
• Format: Article
• Language: English
• Subjects: Chemistry; Helium clusters; path integral Monte Carlo; Physical chemistry; Quantum physics
• ISSN: 0020-7608; 1097-461X
• DOI: 10.1002/qua.24622

The energetics and structures of HeNCa clusters have been studied by means of path integral Monte Carlo calculations. Sizes ranging between N = 10 and 40 helium atoms were considered at T = 1, 1.5, and 2 K. Radial and angular distributions have been analyzed in detail to investigate the geometry of the bound systems. The comparison of the results obtained with two current He–Ca interactions (Kleinekathöfer, Chem. Phys. Lett. 2000, 324, 40, and Lovallo and Klobukowski J. Chem. Phys. 2004, 120, 246) reveals substantial differences regarding the precise location of the Ca impurity with respect to the helium droplet. Whereas the use of the first potential yields a doped cluster in which the Ca atom is solvated inside a helium cage, predictions with the much weaker HeCa potential by Lovallo and Klobukowski correspond to the formation of a dimple at the surface of the outer He atoms to host the Ca atom, a situation which is consistent with the experimental findings for the system. © 2014 Wiley Periodicals, Inc. The precise location of Ca impurities in He droplets is investigated by means of path integral Monte Carlo calculations for clusters with up to 40 He atoms. The structure and energetics of the droplets depends on the He–Ca interaction used. By comparing theoretical results with existing experimental data, this study of He–Ca potentials highlights the importance of a correct description of the impurity‐dopant interaction.