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Phys. Rev. Lett. 87, 177401 (2001) [4 pages]

Large Third-Order Optical Nonlinearity of Cu-O Chains Investigated by Third-Harmonic Generation Spectroscopy

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H. Kishida1, M. Ono1, K. Miura1, H. Okamoto1,2,3, M. Izumi4, T. Manako4, M. Kawasaki2,4,5, Y. Taguchi6, Y. Tokura2,4,6, T. Tohyama5, K. Tsutsui5, and S. Maekawa5
1Department of Advanced Materials Science, University of Tokyo, Tokyo 113-0033, Japan
2Correlated Electron Research Center (CERC), National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba, 305-0046 Japan
3Structure and Transformation Group, PRESTO, Tokyo 113-0033, Japan
4Joint Research Center for Atom Technology (JRCAT), Tsukuba 305-0046, Japan
5Institute for Materials Research, Tohoku University, Sendai 980-8577, Japan
6Department of Applied Physics, University of Tokyo, Tokyo 113-8656, Japan

Received 16 January 2001; published 8 October 2001

Spectra of the third-order nonlinear susceptibility χ(3) have been investigated for one-dimensional Mott insulators, Sr2CuO3 and Ca2CuO3, by applying the third-harmonic generation (THG) spectroscopy on their single-crystalline thin films. The three-photon resonance to the lowest charge-transfer (CT) state with odd parity strongly enhances χ(3), which is of the order of 10-9 esu. The two-photon resonant structure unravels the even-CT state, located close to the odd-CT state. Two types of χ(3) spectra obtained from THG and the electroreflectance measurements are explained based on the concept of spin-charge separation.

© 2001 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.87.177401
DOI:
10.1103/PhysRevLett.87.177401
PACS:
78.66.Nk, 42.65.Ky
 
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