Theoretical study on open-shell nonlinear optical molecular systems and a development of a novel computational scheme of exciton dynamics

Masayoshi Nakano, Ryohei Kishi, Hitoshi Fukui, Takuya Minami, Hiroshi Nagai, Kyohei Yoneda, Sean Bonness, Hideaki Takahashi

Research output: Contribution to journalArticlepeer-review

1 Citation (Scopus)

Abstract

This contribution firstly elucidates a structureproperty relationship in third-order nonlinear optical molecular systems with singlet diradical characters. It turns out that the second hyperpolarizabilities (γ) of the singlet open-shell molecules with intermediate diradical characters are significantly enhanced as compared with those of closed-shell and pure diradical molecules. The hybrid density functional theory method, i.e. UBHandHLYP, is applied to the calculations of γ of dimer models composed of singlet diradical diphenalenyl molecules, which show a remarkable enhancement of γ per monomer as decreasing the intermolecular distance. The second contribution is concerned with a development of ab initio molecular orbital configuration-interaction-based quantum master equation (QME) approach. This is found to provide both coherent processes, e.g. dynamic polarization and exciton (electronhole pair) recurrence motion, and incoherent processes, e.g. exciton migration, in molecular systems. Using this approach, the electron/hole dynamics for dynamic polarizabilities α(ω) are examined for several π-conjugated linear chain systems, and the structural dependences of α(ω) are elucidated.

Original languageEnglish
Pages (from-to)123-129
Number of pages7
JournalInternational Journal of Nanoscience
Volume8
Issue number1-2
DOIs
Publication statusPublished - 2009
Externally publishedYes

Keywords

  • Diradical
  • Exciton dynamics
  • Hyperpolarizability
  • Nonlinear optics
  • Open-shell
  • Polarization

ASJC Scopus subject areas

  • Biotechnology
  • Bioengineering
  • Materials Science(all)
  • Condensed Matter Physics
  • Computer Science Applications
  • Electrical and Electronic Engineering

Fingerprint Dive into the research topics of 'Theoretical study on open-shell nonlinear optical molecular systems and a development of a novel computational scheme of exciton dynamics'. Together they form a unique fingerprint.

Cite this