Anomalous Temperature Dependence of $\mathbf{g}$-Tensor in Organic Conductor, (TMTTF)2X ($\text{X}=\text{Br}$, PF6, and SbF6)
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概要
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The magnetic properties of organic conductor (TMTTF)2X ($\text{X}=\text{Br}$, PF6, and SbF6), where TMTTF is tetramethyltetrathiafulvalene, were examined by electron spin resonance (ESR) spectroscopy, X-ray diffraction (XRD) of the single crystals, and quantum–chemical calculation of the $\mathbf{g}$-tensor. In the case of salts with bulky counter anions such as the PF6 and SbF6, an anomalous temperature dependence of the $\mathbf{g}$-tensor was observed in the temperature range from 20 to 296 K. This anomalous behavior of the $\mathbf{g}$-tensor signifies the rotation of the principal axes as well as the shift of the principal values. The $\mathbf{g}$-tensor of the Br salt is, however, temperature independent. No remarkable change in the intra-molecular structure as a function of temperature was observed for all salts. On the other hand, the distance between TMTTF and counter-anion molecules obviously decreases as the temperature decreases for the PF6 and SbF6 salts, while thermal contraction is not remarkable for the Br salt. In order to clarify the origin of the anomalous behavior of the $\mathbf{g}$-tensor, we investigated the possibility of deformation of the wave-function by the counter-anion potentials using a quantum–chemical calculation for the actual crystal structures measured at low-temperatures. In this paper, we describe the first direct observation of the deformation of the frontier orbital by the counter anion potential for organic conductors. The intra-molecular spin-distribution as a function of temperature is also discussed from the microscopic point of view.
- 2009-10-15
著者
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HARA Toshifumi
Institute for Molecular Science
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FURUKAWA Ko
Institute for Molecular Science
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Nakamura Toshikazu
Institute For Molecular Science
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Nakamura Toshikazu
Institute for Molecular Science, Okazaki, Aichi 444-8585
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