Abstract
A phase transition in an organic charge-transfer complex, which originates from the neutral-ionic valence instability, can be tuned toward zero kelvin with use of external pressure or chemical modification as a control parameter. The phase diagram and observed dielectric behaviors are typical of quantum paraelectricity, yet this zero-kelvin transition point namely, the quantum critical point, accompanies large quantum fluctuation of the molecular charge, as demonstrated by the molecular vibrational mode spectra. The result indicates that the π-electron transfer between donor and acceptor molecules is coupled with the zero-point lattice dynamics around the quantum critical point.
References
30
Referenced
181
-
J. S. Miller Ed. Extended Linear Chain Compounds (Plenum Press New York 1982) vols. 1 to 3.
(
10.1007/978-1-4613-3249-7
) -
T. Ishiguro K. Yamaji G. Saito Eds. Organic Superconductors (Springer-Verlag Berlin ed. 2 1998).
(
10.1007/978-3-642-58262-2
) -
E. Coronado P. Delhaes D. Gatteschi J. S. Miller Eds. Molecular Magnetism: From Molecular Assemblies to the Devices vol. E321 NATO ASI Series (Kluwer Academic Dordrecht Netherlands 1996).
(
10.1007/978-94-017-2319-0
) -
K. Nasu Ed. Relaxations of Excited States and Photo-Induced Phase Transitions (Springer-Verlag Berlin 1997).
(
10.1007/978-3-642-60702-8
) -
Torrance J. B., Vazquez J. E., Mayerle J. J., Lee V. Y., Phys. Rev. Lett. 46, 253 (1981).
(
10.1103/PhysRevLett.46.253
) / Phys. Rev. Lett. by Torrance J. B. (1981) -
Tokura Y., et al., Phys. Rev. Lett. 63, 2405 (1989).
(
10.1103/PhysRevLett.63.2405
) / et al., Phys. Rev. Lett. by Tokura Y. (1989) -
Lemée-Cailleau M. H., et al., Phys. Rev. Lett. 79, 1690 (1997).
(
10.1103/PhysRevLett.79.1690
) / et al., Phys. Rev. Lett. by Lemée-Cailleau M. H. (1997) -
Luty T., et al., Europhys. Lett. 59, 619 (2002).
(
10.1209/epl/i2002-00149-4
) / et al., Europhys. Lett. by Luty T. (2002) -
Mathur N. D., et al., Nature 394, 39 (1998).
(
10.1038/27838
) / et al., Nature by Mathur N. D. (1998) 10.1038/35101507
10.1126/science.1063539
-
Aoki S., Nakayama T., Miura A., Phys. Rev. B 48, 626 (1993).
(
10.1103/PhysRevB.48.626
) / Phys. Rev. B by Aoki S. (1993) -
Horiuchi S., Okimoto Y., Kumai R., Tokura Y., J. Am. Chem. Soc. 123, 665 (2001).
(
10.1021/ja0016654
) / J. Am. Chem. Soc. by Horiuchi S. (2001) -
Müller K. A., Burkard H., Phys. Rev. B 19, 3593 (1979).
(
10.1103/PhysRevB.19.3593
) / Phys. Rev. B by Müller K. A. (1979) -
Samara G. A., Phys. Rev. Lett. 27, 103 (1971).
(
10.1103/PhysRevLett.27.103
) / Phys. Rev. Lett. by Samara G. A. (1971) -
Barrett J. H., Phys. Rev. 86, 118 (1952).
(
10.1103/PhysRev.86.118
) / Phys. Rev. by Barrett J. H. (1952) - S. Horiuchi Y. Okimoto R. Kumai Y. Tokura data not shown.
-
Aoki S., Nakayama T., Miura A., Synth. Met. 70, 1243 (1995).
(
10.1016/0379-6779(94)02838-P
) / Synth. Met. by Aoki S. (1995) -
Mitani T., et al., Phys. Rev. B 35, 427 (1987).
(
10.1103/PhysRevB.35.427
) / et al., Phys. Rev. B by Mitani T. (1987) -
Nagaosa N., J. Phys. Soc. Jpn. 55, 2754 (1986).
(
10.1143/JPSJ.55.2754
) / J. Phys. Soc. Jpn. by Nagaosa N. (1986) - Concerning the low- T phase of DMTTF-QCl 4 crystal E. Collet et al. (27) recently reported the doubling of one interchain axis of the triclinic unit cell which originally contains only one DA pair. Furthermore their structural analysis showed a layered ferrielectric ordering of antiparallel DA dimer by assuming that two (nonequivalent) N and I layers alternate along this doubled axis (noncentrosymmetric space group P 1). However both infrared and Raman spectroscopy (Fig. 4) have provided evidence in support of the homogeneous ρ without the mode splitting that would be expected for the modulated molecular environment and/or ionicity in the presence of nonequivalent DA stacks. In accord with these spectroscopic results our latest structural analysis by synchrotron x-ray diffraction (λ = 0.699 Å) on our DMTTF-QCl 4 specimen at 14 K (< T c ) successfully demonstrated that two equivalent DA dimers in a centrosymmetic supercell (space group P 1̅) construct a layer-type antiferroelectric order (28). { R = 0.063 R w = 0.066 based on 1387 observed reflections [ I > 3σ( I )] and 237 variable parameters.}
-
Schneider T., Beck H., Stoll E., Phys. Rev. B13, 1123 (1976).
(
10.1103/PhysRevB.13.1123
) / Phys. Rev. by Schneider T. (1976) -
Nogami Y., et al., Synth. Met. 70, 1219 (1995).
(
10.1016/0379-6779(94)02826-K
) / et al., Synth. Met. by Nogami Y. (1995) -
Girlando A., Zanon I., Bozio R., Pecile C., J. Chem. Phys. 68, 22 (1978).
(
10.1063/1.435487
) / J. Chem. Phys. by Girlando A. (1978) -
Horiuchi S., Okimoto Y., Kumai R., Tokura Y., J. Phys. Soc. Jpn. 69, 1302 (2002).
(
10.1143/JPSJ.69.1302
) / J. Phys. Soc. Jpn. by Horiuchi S. (2002) -
Okimoto Y., et al., Phys. Rev. Lett. 87, 187401 (2001).
(
10.1103/PhysRevLett.87.187401
) / et al., Phys. Rev. Lett. by Okimoto Y. (2001) -
Collet E., et al., Phys. Rev. B 63, 054105 (2001).
(
10.1103/PhysRevB.63.054105
) / et al., Phys. Rev. B by Collet E. (2001) - Supplementary material is available on Science Online.
-
Girlando A., Bozio R., Pecile C., Torrance J. B., Phys. Rev. B26, 2306 (1982).
(
10.1103/PhysRevB.26.2306
) / Phys. Rev. by Girlando A. (1982) - We thank H. Okamoto N. Nagaosa S. Miyasaka N. Takeshita Y. Ogawa and H. Sawa for enlightening discussions.
Dates
Type | When |
---|---|
Created | 22 years, 7 months ago (Jan. 9, 2003, 8:23 p.m.) |
Deposited | 1 year, 7 months ago (Jan. 9, 2024, 11:34 p.m.) |
Indexed | 3 weeks, 5 days ago (Aug. 2, 2025, 12:31 a.m.) |
Issued | 22 years, 7 months ago (Jan. 10, 2003) |
Published | 22 years, 7 months ago (Jan. 10, 2003) |
Published Print | 22 years, 7 months ago (Jan. 10, 2003) |
@article{Horiuchi_2003, title={Quantum Phase Transition in Organic Charge-Transfer Complexes}, volume={299}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1076129}, DOI={10.1126/science.1076129}, number={5604}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Horiuchi, Sachio and Okimoto, Yoichi and Kumai, Reiji and Tokura, Yoshinori}, year={2003}, month=jan, pages={229–232} }