Ab initio calculations of first hyperpolarizabilities for donor-acceptor azobenzenes and their dimers

Y. Okuno, Shiyoshi Yokoyama, S. Mashiko

Research output: Contribution to journalConference article

2 Citations (Scopus)

Abstract

To understand the large nonlinear optical activities of azobenzene dendrons, which are dendritic macromolecules comprising donor-acceptor azobenzenes as branching units, we carried out ab initio calculations for azobenzene monomers, i.e., 4-dimethylamino-4′-carboxyazobenzene and 4-dimethylamino-2′-nitro-4′-carboxyazobenzene, and their dimers. We determined the stable structures and calculated the first hyperpolarizabilities, using the coupled-perturbed Hartree-Fock method. We found that two azobenzenes in the stable structure of each of the dimers have correlated orientations that produce a large overall dipole. The hyperpolarizabilities for the dimers were larger than those for the corresponding monomers. From these findings, we conclude that the poling of branching units by the interaction between azobenzene moieties within the azobenzene dendrons results in cone-shape structures that cause the large nonlinear optical activities.

Original languageEnglish
Pages (from-to)83-90
Number of pages8
JournalMolecular Crystals and Liquid Crystals Science and Technology Section B: Nonlinear Optics
Volume26
Issue number1-3
Publication statusPublished - Dec 1 2000
Externally publishedYes
EventInternational Workshop on Molecular Design of Photonic Materials - Takarazuka, Japan
Duration: Dec 9 1999Dec 10 1999

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Azobenzene
Dimers
optical activity
dimers
monomers
Dendrimers
macromolecules
cones
Monomers
dipoles
causes
Macromolecules
azobenzene
Cones
interactions

All Science Journal Classification (ASJC) codes

  • Control and Systems Engineering
  • Condensed Matter Physics

Cite this

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title = "Ab initio calculations of first hyperpolarizabilities for donor-acceptor azobenzenes and their dimers",
abstract = "To understand the large nonlinear optical activities of azobenzene dendrons, which are dendritic macromolecules comprising donor-acceptor azobenzenes as branching units, we carried out ab initio calculations for azobenzene monomers, i.e., 4-dimethylamino-4′-carboxyazobenzene and 4-dimethylamino-2′-nitro-4′-carboxyazobenzene, and their dimers. We determined the stable structures and calculated the first hyperpolarizabilities, using the coupled-perturbed Hartree-Fock method. We found that two azobenzenes in the stable structure of each of the dimers have correlated orientations that produce a large overall dipole. The hyperpolarizabilities for the dimers were larger than those for the corresponding monomers. From these findings, we conclude that the poling of branching units by the interaction between azobenzene moieties within the azobenzene dendrons results in cone-shape structures that cause the large nonlinear optical activities.",
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TY - JOUR

T1 - Ab initio calculations of first hyperpolarizabilities for donor-acceptor azobenzenes and their dimers

AU - Okuno, Y.

AU - Yokoyama, Shiyoshi

AU - Mashiko, S.

PY - 2000/12/1

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N2 - To understand the large nonlinear optical activities of azobenzene dendrons, which are dendritic macromolecules comprising donor-acceptor azobenzenes as branching units, we carried out ab initio calculations for azobenzene monomers, i.e., 4-dimethylamino-4′-carboxyazobenzene and 4-dimethylamino-2′-nitro-4′-carboxyazobenzene, and their dimers. We determined the stable structures and calculated the first hyperpolarizabilities, using the coupled-perturbed Hartree-Fock method. We found that two azobenzenes in the stable structure of each of the dimers have correlated orientations that produce a large overall dipole. The hyperpolarizabilities for the dimers were larger than those for the corresponding monomers. From these findings, we conclude that the poling of branching units by the interaction between azobenzene moieties within the azobenzene dendrons results in cone-shape structures that cause the large nonlinear optical activities.

AB - To understand the large nonlinear optical activities of azobenzene dendrons, which are dendritic macromolecules comprising donor-acceptor azobenzenes as branching units, we carried out ab initio calculations for azobenzene monomers, i.e., 4-dimethylamino-4′-carboxyazobenzene and 4-dimethylamino-2′-nitro-4′-carboxyazobenzene, and their dimers. We determined the stable structures and calculated the first hyperpolarizabilities, using the coupled-perturbed Hartree-Fock method. We found that two azobenzenes in the stable structure of each of the dimers have correlated orientations that produce a large overall dipole. The hyperpolarizabilities for the dimers were larger than those for the corresponding monomers. From these findings, we conclude that the poling of branching units by the interaction between azobenzene moieties within the azobenzene dendrons results in cone-shape structures that cause the large nonlinear optical activities.

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