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Phys. Rev. Lett. 99, 033001 (2007) [4 pages]

Relationship between Third-Order Nonlinear Optical Properties and Magnetic Interactions in Open-Shell Systems: A New Paradigm for Nonlinear Optics

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Masayoshi Nakano1,*, Ryohei Kishi1, Suguru Ohta1, Hideaki Takahashi1, Takashi Kubo2, Kenji Kamada3, Koji Ohta3, Edith Botek4, and Benoit Champagne4
1Department of Materials Engineering Science, Graduate School of Engineering Science, Osaka University, Toyonaka, Osaka 560-8531, Japan
2Department of Chemistry, Graduate School of Science, Osaka University, Toyonaka, Osaka 560-0043, Japan
3Photonics Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), Ikeda, Osaka 563-8577, Japan
4Laboratoire de Chimie Théorique Appliquée, Facultés Universitaires Notre-Dame de la Paix (FUNDP), rue de Bruxelles, 61, 5000 Namur, Belgium

Received 12 January 2007; published 20 July 2007

Although most third-order nonlinear optical (NLO) materials are closed-shell singlet systems, this Letter theoretically shows that the third-order NLO properties are drastically enhanced in symmetric open-shell diradical systems with intermediate diradical character and further reveals that this enhancement is associated with the ferromagnetic and antiferromagnetic interactions. This new paradigm opens up a promising area for designing new third-order NLO materials.

© 2007 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.99.033001
DOI:
10.1103/PhysRevLett.99.033001
PACS:
33.15.Kr, 31.10.+z, 31.15.Rh

*Corresponding author.

mnaka@cheng.es.osaka-u.ac.jp

 
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