Polar phonon anomalies in single-crystalline TbScO3

Polarized infrared reflectivity spectra of a (1 1 0)-oriented TbScO3 single-crystal plate were measured down to 10 K. The number of observed polar phonons active along the crystallographic c-axis at low temperatures is much higher than predicted by the factor group analysis for the orthorhombic Pbnm- space group. Moreover, the lowest frequency phonons active in E| c as well as in E| polarized spectra exhibit dramatic softening tending to a lattice instability at low temperatures. The dielectric permittivity at microwave frequencies does not show any ferroelectric-like anomaly, but the dielectric loss exhibits a maximum at 100 K. The origin of the discrepancy between the number of predicted and observed polar phonons as well as the tendency toward lattice instability are discussed. Magnetic measurements reveal an antiferromagnetic phase transition near 3 K.

[1]  Michal Malinowski,et al.  Self-organized, rodlike, micrometer-scale microstructure of Tb3Sc2Al3O12-TbScO3:Pr eutectic , 2006 .

[2]  Jürgen Schubert,et al.  A strong ferroelectric ferromagnet created by means of spin-lattice coupling. , 2011, Nature.

[3]  C. Jia,et al.  Structural and optical properties of epitaxial BaTiO3 thin films grown on GdScO3(110). , 2003 .

[4]  G. Jellison,et al.  Dielectric and optical properties of epitaxial rare-earth scandate films and their crystallization behavior , 2006 .

[5]  B. Veličkov,et al.  Crystal chemistry of GdScO3, DyScO3, SmScO3 and NdScO3 , 2007 .

[6]  Volker Kahlenberg,et al.  Redetermination of EuScO3 , 2009, Acta crystallographica. Section E, Structure reports online.

[7]  P. Kužel,et al.  Soft mode behavior in SrTiO3/DyScO3 thin films: Evidence of ferroelectric and antiferrodistortive phase transitions , 2009 .

[8]  P. Dore,et al.  Far infrared properties of the rare-earth scandate DyScO3 , 2010, Journal of physics. Condensed matter : an Institute of Physics journal.

[9]  Darrell G. Schlom,et al.  A Thermodynamic Approach to Selecting Alternative Gate Dielectrics , 2002 .

[10]  A. Tagantsev,et al.  Room-temperature ferroelectricity in strained SrTiO3 , 2004, Nature.

[11]  R. Uecker,et al.  Redetermination of terbium scandate, revealing a defect-type perovskite derivative , 2008, Acta crystallographica. Section E, Structure reports online.

[12]  J. Kreisel,et al.  Raman scattering of perovskite DyScO3 and GdScO3 single crystals , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[13]  U. Gösele,et al.  Impact of misfit dislocations on the polarization instability of epitaxial nanostructured ferroelectric perovskites , 2004, Nature materials.

[14]  D. Vanderbilt,et al.  Si-compatible candidates for high-κ dielectrics with the Pbnm perovskite structure , 2010, 1005.2767.

[15]  S. Trolier-McKinstry,et al.  Thermal expansion of the new perovskite substrates DyScO_3 and GdScO_3 , 2005 .

[16]  V. Nagarajan,et al.  Can interface dislocations degrade ferroelectric properties , 2004 .

[17]  P. Kužel,et al.  Temperature and electric field tuning of the ferroelectric soft mode in a strained SrTiO 3 / DyScO 3 heterostructure , 2009 .

[18]  A. Eremenko,et al.  An electrode-free method of characterizing the microwave dielectric properties of high-permittivity thin films , 2011 .

[19]  Suman Datta,et al.  Gate Oxides Beyond SiO_2 , 2008 .

[20]  V. Gopalan,et al.  Enhancement of Ferroelectricity in Strained BaTiO3 Thin Films , 2004, Science.

[21]  P. Schiffer,et al.  Low temperature magnetism in the perovskite substrate DyScO3 , 2009 .

[22]  P. Kužel,et al.  Electric field tuning of hard polar phonons in strained SrTiO3 films , 2010 .

[23]  R. Uecker,et al.  Properties of rare-earth scandate single crystals (Re = Nd-Dy) , 2008 .

[24]  K. Postava,et al.  Far-infrared spectroscopy of terbium-scandium-aluminium garnet and terbium-scandium perovskite , 2010, Polish-Slovak-Czech Optical Conference on Wave and Quantum Aspects of Contemporary Optics.

[25]  R. Uecker,et al.  Spiral formation during Czochralski growth of rare-earth scandates , 2006 .

[26]  Chang-Beom Eom,et al.  Strain Tuning of Ferroelectric Thin Films , 2007 .

[27]  R. Waser,et al.  Misfit dislocations in nanoscale ferroelectric heterostructures , 2005 .

[28]  G. Pourtois,et al.  Cation charge anomalies and high-κdielectric behavior inDyScO3:Ab initiodensity-functional and self-interaction-corrected calculations , 2007 .