Molecular motion in methylammonium hexahalotellurates(IV) as studied by means of the pulsed nuclear magnetic resonance.
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概要
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Molecular motion in solid (CH<SUB>3</SUB>NH<SUB>3</SUB>)<SUB>2</SUB>TeX<SUB>6</SUB> (X=Cl, Br, and I) was studied by measuring the spin-lattice relaxation time, <I>T</I><SUB>1</SUB>, of <SUP>1</SUP>H and <SUP>35</SUP>Cl nuclei in several crystalline phases appearing below room temperature. A deep minimum of the proton <I>T</I><SUB>1</SUB> was observed in the low-temperature phase of all the compounds, indicating that the methylammonium ion performs a rapid reorientation as a whole about its three-fold axis. The activation energies, <I>E</I><SUB>a</SUB>, for the motion of cations are determined to be 7.0, 3.7, and 2.7 kJ/mol for X=Cl, Br, and I respectively. In (CH<SUB>3</SUB>NH<SUB>3</SUB>)<SUB>2</SUB>TeI<SUB>6</SUB>, which has the lowest <I>E</I><SUB>a</SUB> value, the relaxation process associated with the tunneling of the cation is apparent at low temperatures. For all the complexes studied, a shallow <I>T</I><SUB>1</SUB> minimum ascribable to the independent rotation of the CH<SUB>3</SUB> and NH<SUB>3</SUB> groups in the cation was observed on the high-temperature side of each deep <I>T</I><SUB>1</SUB> minimum. The <SUP>35</SUP>Cl <I>T</I><SUB>1</SUB> of (CH<SUB>3</SUB>NH<SUB>3</SUB>)<SUB>2</SUB>TeCl<SUB>6</SUB> exhibited a distinct minimum at the lower phase-transition point at 139 K and a discontinuity at the higher one near 230 K. The hindered rotation of the [TeCl<SUB>6</SUB>]<SUP>2−</SUP> octahedron occurs in the room-temperature phase, with an <I>E</I><SUB>a</SUB> value of 48 kJ/mol.
- 公益社団法人 日本化学会の論文
著者
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Ikeda Ryuichi
Department Of Chemistry Faculty Of Engineering Gifu University
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Furukawa Yoshihiro
The Institute of Scientific and Industrial Research, Osaka University
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Kiriyama Hideko
The Institute of Scientific and Industrial Research, Osaka University
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