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Dynamical Valence Fluctuation at the Charge−Density−Wave Phase Boundary in Iodide-Bridged Pt Compound [Pt(chxn)₂I]I₂

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Shinya Takaishi,*^† Daisuke Kawakami,^† Masahiro Yamashita,*^† Mari Sasaki,^‡ Takashi Kajiwara,^† Hitoshi Miyasaka,^‡ Ken-ichi Sugiura,^‡ Yusuke Wakabayashi,^§ Hiroshi Sawa,^§ Hiroyuki Matsuzaki, Hideo Kishida, Hiroshi Okamoto, Harutaka Watanabe, Hisaaki Tanaka, Kazuhiro Marumoto, Hiroshi Ito, and Shin-ichi Kuroda;

Contribution from the Department of Chemistry, Graduate School of Science, Tohoku University and CREST (JST), 6-3 Aza-aoba, Aramaki, Sendai 980-8578, Japan, Department of Chemistry, Graduate School of Science, Tokyo Metropolitan University, 1-1 Minamiosawa, Hachioji 192-0397, Japan, Institute of Materials Structure Science, High Energy Accelerator ResearchOrganization, Tsukuba 305-0801, Japan, Department of Advanced Materials Science, Graduate School of Frontier Sciences, The University of Tokyo, Kashiwa 277-8561, Japan, and Department of Applied Physics, Graduate School of Engineering, Nagoya University, Furocho, Chikusa-ku, Nagoya 464-8603, Japan

J. Am. Chem. Soc., 2006, 128 (19), pp 6420–6425

DOI: 10.1021/ja060193b

Publication Date (Web): April 22, 2006

In papers with more than one author, the asterisk indicates the name of the author to whom inquiries about the paper should be addressed.

†

Tohoku University.

‡

Tokyo Metropolitan University.

Institute of Materials Structure Science.

The University of Tokyo.

Nagoya University.

, takaishi@agnus.chem.tohoku.ac.jp, ; , yamasita@agnus.chem.tohoku.ac.jp

Abstract

We synthesized a novel iodo-bridged linear chain platinum compound, having the quasi-two-dimensional charge−density−wave (CDW) ground state and the smallest band gap. In this compound, we discovered an anomalous valence state in the boundary region at which the CDW phase alternates in the crystal by means of ESR, X-ray diffuse scattering, STM, and electrical resistivity. This anomalous state can be explained by the fast fluctuation between Pt^IV−I···Pt^II and Pt^II···I−Pt^IV in the double well potential. This is the first observation of the dynamical fluctuation of the CDW phase among the quasi one-dimensional halogen-bridged complexes.

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Published In Issue May 17, 2006
Received January 10, 2006

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Article

Dynamical Valence Fluctuation at the Charge−Density−Wave Phase Boundary in Iodide-Bridged Pt Compound [Pt(chxn)₂I]I₂