Vibrational contribution to static and dynamic (Hyper)polarizabilities of zigzag BN nanotubes calculated by the finite field nuclear relaxation method

Authors

  • Matteo Ferrabone,

    1. Dipartimento di Chimica IFM, Università di Torino and NIS-Nanostructured Interfaces and Surfaces - Centre of Excellence, Via P. Giuria 7, 10125 Torino, Italy
    Search for more papers by this author
  • Bernard Kirtman,

    1. Department of Chemistry and Biochemistry, University of California, Santa Barbara, California 93106
    Search for more papers by this author
  • Valentina Lacivita,

    1. Dipartimento di Chimica IFM, Università di Torino and NIS-Nanostructured Interfaces and Surfaces - Centre of Excellence, Via P. Giuria 7, 10125 Torino, Italy
    Search for more papers by this author
  • Michel Rérat,

    Corresponding author
    1. Equipe de Chimie Physique, IPREM UMR5254, Université de Pau et des Pays de l'Adour, 64000 Pau, France
    • Equipe de Chimie Physique, IPREM UMR5254, Université de Pau et des Pays de l'Adour, 64000 Pau, France
    Search for more papers by this author
  • Roberto Orlando,

    1. Dipartimento di Scienze e Tecnologie Avanzate, Università del Piemonte Orientale, Viale T. Michel 11, 15121 Alessandria, Italy
    Search for more papers by this author
  • Roberto Dovesi

    1. Dipartimento di Chimica IFM, Università di Torino and NIS-Nanostructured Interfaces and Surfaces - Centre of Excellence, Via P. Giuria 7, 10125 Torino, Italy
    Search for more papers by this author

Abstract

The vibrational contribution to static and dynamic (hyper)polarizabilities for the zigzag (n,0) family of BN nanotubes, with n ranging from (6,0) to (36,0), has been obtained. Calculations were done by the finite field nuclear relaxation (FF-NR) method for periodic systems, newly implemented in the CRYSTAL code, using the Coupled Perturbed Kohn-Sham (CPKS) scheme at the B3LYP/6-31G* level for the required electronic properties. Both transverse and transverse-longitudinal tensor components are determined by applying finite, i.e. static, fields in the transverse direction. The magnitude of the vibrational term increases with the radius of the nanotube as determined by the increase in the field-induced geometric deformation. The resulting vibrational (hyper)polarizability varies from being dominant to negligible, when compared with the corresponding static electronic contribution. This depends upon the radius, as well as the property and the component, in a systematic manner. The extension to longitudinal components, not yet available, will be implemented next. © 2011 Wiley Periodicals, Inc. Int J Quantum Chem, 2012

Ancillary