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

Masayoshi Nakano, Ryohei Kishi, Suguru Ohta, Hideaki Takahashi, Takashi Kubo, Kenji Kamada, Koji Ohta, Edith Botek, and Benoit Champagne

Phys. Rev. Lett. 99, 033001 – Published 20 July 2007

Abstract

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.

Received 12 January 2007

DOI:https://doi.org/10.1103/PhysRevLett.99.033001

Authors & Affiliations

Masayoshi Nakano^1,*, 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

^*Corresponding author. mnaka@cheng.es.osaka-u.ac.jp

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Issue

Vol. 99, Iss. 3 — 20 July 2007

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