- Letter
- Open Access
Spectroscopic signature of sublattice polarization in the lattice dynamics of an antiferroelectric crystal
Phys. Rev. Research 5, L012036 – Published 16 March, 2023
DOI: https://doi.org/10.1103/PhysRevResearch.5.L012036
Abstract
Spectroscopic measurements of the far-infrared phonon dynamics for a model antiferroelectric crystal are performed at low temperature. In agreement with the phenomenological expectations for a displacive antiferroelectric transition, a polar soft mode associated to a close-lying polar phase of the otherwise centrosymmetric structure is observed. Incomplete softening of the polar soft mode due to the antiferroelectric transition quantifies the energy barrier between the neighboring states. The dynamics are modeled with a biquadratic Landau potential incorporating a symmetry constraining effective interaction between displaced ions. A signature of sublattice polarization is observed in a scaling of the effective antipolar interaction in the antiferroelectric phase.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (37)
- C. Kittel, Theory of antiferroelectric crystals, Phys. Rev. 82, 729 (1951).
- L. E. Cross, Antiferroelectric-ferroelectric switching in a simple “Kittel” antiferroelectric, J. Phys. Soc. Jpn. 23, 77 (1967).
- K. Okada, Phenomenological theory of antiferroelectric transition. I. second-order transition, J. Phys. Soc. Jpn. 27, 420 (1969).
- A. P. Levanyuk and D. G. Sannikov, Anomalies in dielectric properties in phase transitions, Zh. Eksp. Teor. Fiz. 55, 256 (1968) [Sov. Phys.–JETP 28, 134 (1969)].
- L. D. Landau and E. M. Lifshitz, Electrodynamics of Continuous Media, 2nd edition (Pergamon, Oxford, 1984).
- H. T. Stokes and D. M. Hatch, Model for the ordered phases in KCN and NaCN, Phys. Rev. B 30, 3845 (1984).
- H. Takezoe, E. Gorecka, and M. Čepič, Antiferroelectric liquid crystals: Interplay of simplicity and complexity, Rev. Mod. Phys. 82, 897 (2010).
- P. Tolédano and M. Guennou, Theory of antiferroelectric phase transitions, Phys. Rev. B 94, 014107 (2016).
- T. Fukami, S. Akahoshi, K. Hukuda, and T. Yagi, Refinement of the crystal structure of above and below antiferroelectric phase transition temperature, J. Phys. Soc. Jpn. 56, 2223 (1987).
- S. Horiuchi, R. Kumai, and S. Ishibashi, Strong polarization switching with low-energy loss in hydrogen-bonded organic antiferroelectrics, Chem. Sci. 9, 425 (2018).
- A. K. Tagantsev, K. Vaideeswaran, S. B. Vakhrushev, A. V. Filimonov, R. G. Burkovsky, A. Shaganov, D. Andronikova, A. I. Rudskoy, A. Q. R. Baron, H. Uchiyama, D. Chernyshov, A. Bosak, Z. Ujma, K. Roleder, A. Majchrowski, J.-H. Ko, and N. Setter, The origin of antiferroelectricity in , Nat. Commun. 4, 2229 (2013).
- J. Hlinka, T. Ostapchuk, E. Buixaderas, C. Kadlec, P. Kuzel, I. Gregora, J. Kroupa, M. Savinov, A. Klic, J. Drahokoupil, I. Etxebarria, and J. Dec, Multiple Soft-Mode Vibrations of Lead Zirconate, Phys. Rev. Lett. 112, 197601 (2014).
- J. Íñiguez, M. Stengel, S. Prosandeev, and L. Bellaiche, First-principles study of the multimode antiferroelectric transition in , Phys. Rev. B 90, 220103(R) (2014).
- E. Constable, S. Raymond, S. Petit, E. Ressouche, F. Bourdarot, J. Debray, M. Josse, O. Fabelo, H. Berger, S. deBrion, and V. Simonet, Magnetic and dielectric order in the kagomelike francisite , Phys. Rev. B 96, 014413 (2017).
- C. Milesi-Brault, C. Toulouse, E. Constable, H. Aramberri, V. Simonet, S. de Brion, H. Berger, L. Paolasini, A. Bosak, J. Íñiguez, and M. Guennou, Archetypal soft-mode-driven antipolar transition in francisite , Phys. Rev. Lett. 124, 097603 (2020).
- D. A. Prishchenko, A. A. Tsirlin, V. Tsurkan, A. Loidl, A. Jesche, and V. G. Mazurenko, Antiferroelectric instability in the kagome francisites (X = Cl,Br), Phys. Rev. B 95, 064102 (2017).
- W. Cochran, Crystal stability and the theory of ferroelectricity, Adv. Phys. 9, 387 (1960).
- W. Cochran, Crystal stability and the theory of ferroelectricity part II. Piezoelectric crystals, Adv. Phys. 10, 401 (1961).
- K. H. Miller, P. W. Stephens, C. Martin, E. Constable, R. A. Lewis, H. Berger, G. L. Carr, and D. B. Tanner, Infrared phonon anomaly and magnetic excitations in single-crystal , Phys. Rev. B 86, 174104 (2012).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/PhysRevResearch.5.L012036 for experimental details, supporting measurements, and eigen mode derivation of the AFE model.
- C. Geuzaine and J. F. Remacle, Gmsh: A 3-d finite element mesh generator with built-in pre- and post-processing facilities, Int. J. Numer. Methods Eng. 79, 1309 (2009).
- F. Hecht, New development in freefem+, J. Numer. Math. 20, 251 (2012).
- P. J. Frey, Medit : An interactive mesh visualization software, INRIA Tech. Rep. 0253 (2001).
- E. Barsoukov and J. R. Macdonald, Impedance Spectroscopy (Wiley, Hoboken, NJ, 2005).
- E. Constable and R. A. Lewis, Optical parameters of ZnTe determined using continuous-wave terahertz radiation, J. Appl. Phys. 112, 063104 (2012).
- A. A. Volkov, G. V. Kozlov, E. B. Kryukova, and J. Petzelt, Low-temperature transformations of the relaxational soft modes in crystals of the rochelle salt family, Zh. Eksp. Teor. Fiz. 90, 192 (1986) [Sov. Phys.–JETP 63, 110 (1986)].
- T. Ostapchuk, J. Petzelt, V. Zelezny, S. Kamba, V. Bovtun, V. Porokhonskyy, A. Pashkin, P. Kuzel, M. D. Glinchuk, I. P. Bykov, B. Gorshunov, and M. Dressel, Polar phonons and central mode in antiferroelectric ceramics, J. Phys.: Condens. Matter 13, 2677 (2001).
- E. Buixaderas, S. Kamba, and J. Petzelt, Lattice dynamics and central-mode phenomena in the dielectric response of ferroelectrics and related materials, Ferroelectrics 308, 131 (2004).
- G. Shirane, E. Sawaguchi, and Y. Takagi, Dielectric properties of lead zirconate, Phys. Rev. 84, 476 (1951).
- W. Cochran, Crystal Stability and the Theory of Ferroelectricity, Phys. Rev. Lett. 3, 412 (1959).
- R. D. King-Smith and D. Vanderbilt, Theory of polarization of crystalline solids, Phys. Rev. B 47, 1651 (1993).
- D. Vanderbilt and R. D. King-Smith, Electric polarization as a bulk quantity and its relation to surface charge, Phys. Rev. B 48, 4442 (1993).
- R. Resta, Macroscopic polarization in crystalline dielectrics: The geometric phase approach, Rev. Mod. Phys. 66, 899 (1994).
- W. A. Benalcazar, B. A. Bernevig, and T. L. Hughes, Electric multipole moments, topological multipole moment pumping, and chiral hinge states in crystalline insulators, Phys. Rev. B 96, 245115 (2017).
- H. v. Einsiedel and S. S. Rosenblum, Electric quadrupole interaction in the phase transition region of antiferroelectric , J. Phys. C: Solid State Phys. 6, L292 (1973).
- H. V. Einsiedel and S. S. Rosenblum, Temperature dependence of the electric quadrupole interaction in , Phys. Status Solidi B 65, K5 (1974).
- Y. Yeshurun, Y. Schlesinger, and S. Havlin, Temperature dependence of the electric quadrupole interaction in , J. Phys. Chem. Solids 40, 231 (1979).