Unconventional Continuous Structural Disorder at the Order-Disorder Phase Transition in the Hexagonal Manganites

Skjærvø, Sandra H.; Meier, Quintin N.; Feygenson, Mikhail; Spaldin, Nicola A.; Billinge, Simon J. L.; Bozin, Emil S.; Selbach, Sverre M.

doi:10.1103/PhysRevX.9.031001

Title: Unconventional Continuous Structural Disorder at the Order-Disorder Phase Transition in the Hexagonal Manganites

Journal Article · Mon Jul 01 00:00:00 EDT 2019 · Physical Review. X

DOI:https://doi.org/10.1103/PhysRevX.9.031001· OSTI ID:1530478

Skjærvø, Sandra H.; Meier, Quintin N.; Feygenson, Mikhail; Spaldin, Nicola A.; Billinge, Simon J. L.; Bozin, Emil S.;

The improper ferroelectricity in YMnO₃ and other related multiferroic hexagonal manganites are known to cause topologically protected ferroelectric domains that give rise to rich and diverse physical phenomena. The local structure and structural coherence across the ferroelectric transition,however, were previously not well understood. Here we reveal the evolution of the local structure with temperature in YMnO₃ using neutron total scattering techniques, and interpret them with the help of first-principles calculations and with a first-principles-based effective Hamiltonian. The results show that, at room temperature, the local and average structures are consistent with the established ferroelectric P6₃cm symmetry. On heating, both local and average structural analyses show striking anomalies from ~800K up to the Curie temperature and signatures of a locally more preserved structure than on average, consistent with increasing fluctuations of the order parameter angle. These fluctuations result in an unusual local symmetry lowering into a continuum of structures on heating. This local symmetry breaking persists into the high-symmetry non-polar phase,constituting an unconventional type of order-disorder transition, and we pinpoint it as the reason for the anomalous behaviour near the phase transition. The hidden disorder revealed in YMnO₃ by total scattering is expected to find analogies in other materials with structural frustration or characteristic energy barriers of different magnitudes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1530478

Alternate ID(s):: OSTI ID: 1524558

Report Number(s):: BNL-211732-2019-JAAM; PRXHAE; 031001

Journal Information:: Physical Review. X, Journal Name: Physical Review. X Vol. 9 Journal Issue: 3; ISSN 2160-3308

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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References (69)

Dynamical Response of Ferroelectrics in Terms of a Classical Anharmonic-Oscillator Model Onodera, Yositaka Journal of the Physical Society of Japan, Vol. 73, Issue 5 https://doi.org/10.1143/JPSJ.73.1216	journal	May 2004
Goldstone-like phonon modes in a (111)-strained perovskite Marthinsen, A.; Griffin, S. M.; Moreau, M. Physical Review Materials, Vol. 2, Issue 1 https://doi.org/10.1103/PhysRevMaterials.2.014404	journal	January 2018
Epitaxially grown YMnO ₃ film: New candidate for nonvolatile memory devices Fujimura, Norifumi; Ishida, Tadashi; Yoshimura, Takeshi Applied Physics Letters, Vol. 69, Issue 7 https://doi.org/10.1063/1.117969	journal	August 1996
Emergence of Long-Range Order in ${BaTiO}_{3}$ from Local Symmetry-Breaking Distortions Senn, M. S.; Keen, D. A.; Lucas, T. C. A. Physical Review Letters, Vol. 116, Issue 20 https://doi.org/10.1103/PhysRevLett.116.207602	journal	May 2016
Order-disorder-order phase transitions in the pyrochlore superconductor ${Cd}_{2} {Re}_{2} O_{7}$ Knee, C. S.; Holmlund, J.; Andreasson, J. Physical Review B, Vol. 71, Issue 21 https://doi.org/10.1103/PhysRevB.71.214518	journal	June 2005
Goldstone-like States in a Layered Perovskite with Frustrated Polarization: A First-Principles Investigation of ${PbSr}_{2} {Ti}_{2} O_{7}$ Nakhmanson, S. M.; Naumov, Ivan Physical Review Letters, Vol. 104, Issue 9 https://doi.org/10.1103/PhysRevLett.104.097601	journal	March 2010
Dynamic structural disorder in cristobalite: neutron total scattering measurement and reverse Monte Carlo modelling Tucker, Matthew G.; Squires, Matthew P.; Dove, Martin T. Journal of Physics: Condensed Matter, Vol. 13, Issue 3 https://doi.org/10.1088/0953-8984/13/3/304	journal	December 2000
Dielectric spectroscopy of paraelectric soft modes Petzelt, J.; Kozlov, G. V.; Volkov, A. A. Ferroelectrics, Vol. 73, Issue 1 https://doi.org/10.1080/00150198708227912	journal	June 1987
The evolution of multiferroics Fiebig, Manfred; Lottermoser, Thomas; Meier, Dennis Nature Reviews Materials, Vol. 1, Issue 8 https://doi.org/10.1038/natrevmats.2016.46	journal	July 2016
Collective Magnetism at Multiferroic Vortex Domain Walls Geng, Yanan; Lee, N.; Choi, Y. J. Nano Letters, Vol. 12, Issue 12 https://doi.org/10.1021/nl301432z	journal	February 2012
Coexistence of the Phonon and Relaxation Soft Modes in the Terahertz Dielectric Response of Tetragonal ${BaTiO}_{3}$ Hlinka, J.; Ostapchuk, T.; Nuzhnyy, D. Physical Review Letters, Vol. 101, Issue 16 https://doi.org/10.1103/PhysRevLett.101.167402	journal	October 2008
Partial glass isosymmetry transition in multiferroic hexagonal $ErMn O_{3}$ Barbour, A.; Alatas, A.; Liu, Y. Physical Review B, Vol. 93, Issue 5 https://doi.org/10.1103/PhysRevB.93.054113	journal	February 2016
Nonlinear optical signatures of the tensor order in Cd2Re2O7 Petersen, Jesse C.; Caswell, Michael D.; Dodge, J. Steven Nature Physics, Vol. 2, Issue 9 https://doi.org/10.1038/nphys392	journal	August 2006
The origin of ferroelectricity in magnetoelectric YMnO3 Van Aken, Bas B.; Palstra, Thomas T. M.; Filippetti, Alessio Nature Materials, Vol. 3, Issue 3 https://doi.org/10.1038/nmat1080	journal	February 2004
High-temperature phase transitions of hexagonal YMnO $_{3}$ Gibbs, Alexandra S.; Knight, Kevin S.; Lightfoot, Philip Physical Review B, Vol. 83, Issue 9 https://doi.org/10.1103/PhysRevB.83.094111	journal	March 2011
Ferroelectric phase transitions in perovskites with off-center ion displacements Girshberg, Yakov; Yacoby, Yizhak Solid State Communications, Vol. 103, Issue 7 https://doi.org/10.1016/S0038-1098(97)00024-0	journal	August 1997
Insulating interlocked ferroelectric and structural antiphase domain walls in multiferroic YMnO3 Choi, T.; Horibe, Y.; Yi, H. T. Nature Materials, Vol. 9, Issue 3 https://doi.org/10.1038/nmat2632	journal	February 2010
Observation of persistent centrosymmetricity in the hexagonal manganite family Kumagai, Yu; Belik, Alexei A.; Lilienblum, Martin Physical Review B, Vol. 85, Issue 17 https://doi.org/10.1103/PhysRevB.85.174422	journal	May 2012
Anisotropic conductance at improper ferroelectric domain walls Meier, D.; Seidel, J.; Cano, A. Nature Materials, Vol. 11, Issue 4 https://doi.org/10.1038/nmat3249	journal	February 2012
Elastic anomalies associated with structural and magnetic phase transitions in single crystal hexagonal YMnO ₃ Thomson, R. I.; Chatterji, T.; Howard, C. J. Journal of Physics: Condensed Matter, Vol. 26, Issue 4 https://doi.org/10.1088/0953-8984/26/4/045901	journal	January 2014
Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators Liechtenstein, A. I.; Anisimov, V. I.; Zaanen, J. Physical Review B, Vol. 52, Issue 8 https://doi.org/10.1103/PhysRevB.52.R5467	journal	August 1995
$γ$ and $β$ cerium: $LDA + U$ calculations of ground-state parameters Amadon, B.; Jollet, F.; Torrent, M. Physical Review B, Vol. 77, Issue 15 https://doi.org/10.1103/PhysRevB.77.155104	journal	April 2008
Orbital Correlations in the Pseudocubic $O$ and Rhombohedral $R$ Phases of ${LaMnO}_{3}$ Qiu, Xiangyun; Proffen, Th.; Mitchell, J. F. Physical Review Letters, Vol. 94, Issue 17 https://doi.org/10.1103/PhysRevLett.94.177203	journal	May 2005
A brief introduction to the ABINIT software package Gonze, Xavier Zeitschrift für Kristallographie - Crystalline Materials, Vol. 220, Issue 5/6 https://doi.org/10.1524/zkri.220.5.558.65066	journal	January 2005
Hidden order in hexagonal $R Mn O_{3}$ multiferroics ( $R = Dy$ –Lu, In, Y, and Sc) Cano, A. Physical Review B, Vol. 89, Issue 21 https://doi.org/10.1103/PhysRevB.89.214107	journal	June 2014
Critical Neutron Scattering in SrTi $O_{3}$ and KMn $F_{3}$ Shapiro, S. M.; Axe, J. D.; Shirane, G. Physical Review B, Vol. 6, Issue 11 https://doi.org/10.1103/PhysRevB.6.4332	journal	December 1972
Equation of State Calculations by Fast Computing Machines Metropolis, Nicholas; Rosenbluth, Arianna W.; Rosenbluth, Marshall N. The Journal of Chemical Physics, Vol. 21, Issue 6 https://doi.org/10.1063/1.1699114	journal	June 1953
Reconciliation of local and long-range tilt correlations in underdoped ${La}_{2 - x} {Ba}_{x} {CuO}_{4} (0 \leq x \leq 0.155)$ Bozin, Emil S.; Zhong, Ruidan; Knox, Kevin R. Physical Review B, Vol. 91, Issue 5 https://doi.org/10.1103/PhysRevB.91.054521	journal	February 2015
Scaling Behavior and Beyond Equilibrium in the Hexagonal Manganites Griffin, S. M.; Lilienblum, M.; Delaney, K. T. Physical Review X, Vol. 2, Issue 4 https://doi.org/10.1103/PhysRevX.2.041022	journal	December 2012
Ferroelectric transition in $Y Mn O_{3}$ from first principles Fennie, Craig J.; Rabe, Karin M. Physical Review B, Vol. 72, Issue 10 https://doi.org/10.1103/PhysRevB.72.100103	journal	September 2005
Ferroelectricity in the multiferroic hexagonal manganites Lilienblum, Martin; Lottermoser, Thomas; Manz, Sebastian Nature Physics, Vol. 11, Issue 12 https://doi.org/10.1038/nphys3468	journal	September 2015
High-temperature structural evolution of hexagonal multiferroic YMnO ₃ and YbMnO ₃ Jeong, Il-Kyoung; Hur, N.; Proffen, Th. Journal of Applied Crystallography, Vol. 40, Issue 4 https://doi.org/10.1107/S0021889807025101	journal	July 2007
Hexagonal YMnO ₃ Aken, Bas B. van; Meetsma, Auke; Palstra, Thomas T. M. Acta Crystallographica Section C Crystal Structure Communications, Vol. 57, Issue 3 https://doi.org/10.1107/S0108270100015663	journal	March 2001
Topological defects as relics of emergent continuous symmetry and Higgs condensation of disorder in ferroelectrics Lin, Shi-Zeng; Wang, Xueyun; Kamiya, Yoshitomo Nature Physics, Vol. 10, Issue 12 https://doi.org/10.1038/nphys3142	journal	November 2014
Pair-distribution functions of ferroelectric perovskites: Direct observation of structural ground states Kwei, George H.; Billinge, Simon >J. L.; Cheong, S-W. Ferroelectrics, Vol. 164, Issue 1 https://doi.org/10.1080/00150199508221830	journal	February 1995
Origin of morphotropic phase boundaries in ferroelectrics Ahart, Muhtar; Somayazulu, Maddury; Cohen, R. E. Nature, Vol. 451, Issue 7178 https://doi.org/10.1038/nature06459	journal	January 2008
Probing Local and Long-Range Structure Simultaneously: An In Situ Study of the High-Temperature Phase Transition of α-AlF ₃ Chupas, Peter J.; Chaudhuri, Santanu; Hanson, Jonathan C. Journal of the American Chemical Society, Vol. 126, Issue 15 https://doi.org/10.1021/ja031553n	journal	April 2004
Polarization Rotation via a Monoclinic Phase in the Piezoelectric 92% ${PbZn}_{1 / 3} {Nb}_{2 / 3} O_{3}$ -8% ${PbTiO}_{3}$ Noheda, B.; Cox, D. E.; Shirane, G. Physical Review Letters, Vol. 86, Issue 17 https://doi.org/10.1103/PhysRevLett.86.3891	journal	April 2001
Global Formation of Topological Defects in the Multiferroic Hexagonal Manganites Meier, Q. N.; Lilienblum, M.; Griffin, S. M. Physical Review X, Vol. 7, Issue 4 https://doi.org/10.1103/PhysRevX.7.041014	journal	October 2017
Crystallography and structural phase transitions, an introduction Salje, E. K. H. Acta Crystallographica Section A Foundations of Crystallography, Vol. 47, Issue 5 https://doi.org/10.1107/S0108767391004300	journal	September 1991
Crystal structure, chemical expansion and phase stability of HoMnO3 at high temperature Selbach, Sverre M.; Nordli Løvik, Amund; Bergum, Kristin Journal of Solid State Chemistry, Vol. 196 https://doi.org/10.1016/j.jssc.2012.07.024	journal	December 2012
Molecular-dynamics study of structural-phase transitions. I. One-component displacement models Schneider, T.; Stoll, E. Physical Review B, Vol. 13, Issue 3 https://doi.org/10.1103/PhysRevB.13.1216	journal	February 1976
Improper ferroelectricity and multiferroism in 2 $H$ -BaMnO $_{3}$ Varignon, Julien; Ghosez, Philippe Physical Review B, Vol. 87, Issue 14 https://doi.org/10.1103/PhysRevB.87.140403	journal	April 2013
Crystal structure and magnetic properties of hexagonal $R {MnO}_{3} (R = Y,$ Lu, and Sc) and the effect of doping Katsufuji, T.; Masaki, M.; Machida, A. Physical Review B, Vol. 66, Issue 13 https://doi.org/10.1103/PhysRevB.66.134434	journal	October 2002
First-principles computation of material properties: the ABINIT software project Gonze, X.; Beuken, J. -M.; Caracas, R. Computational Materials Science, Vol. 25, Issue 3 https://doi.org/10.1016/S0927-0256(02)00325-7	journal	November 2002
Goldstone-Mode Phonon Dynamics in the Pyrochlore ${Cd}_{2} {Re}_{2} O_{7}$ Kendziora, C. A.; Sergienko, I. A.; Jin, R. Physical Review Letters, Vol. 95, Issue 12 https://doi.org/10.1103/PhysRevLett.95.125503	journal	September 2005
Experimental evidence for an intermediate phase in the multiferroic YMnO ₃ Nénert, G.; Pollet, M.; Marinel, S. Journal of Physics: Condensed Matter, Vol. 19, Issue 46 https://doi.org/10.1088/0953-8984/19/46/466212	journal	October 2007
The Nanoscale Ordered MAterials Diffractometer NOMAD at the Spallation Neutron Source SNS Neuefeind, Jörg; Feygenson, Mikhail; Carruth, John Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 287 https://doi.org/10.1016/j.nimb.2012.05.037	journal	September 2012
Symmetry and coupling of magnetic and electric order parameters in YMnO[sub 3] Lottermoser, Th.; Fiebig, M.; Fröhlich, D. Journal of Applied Physics, Vol. 91, Issue 10 https://doi.org/10.1063/1.1448790	journal	January 2002
Theory of displacive phase transitions in minerals Dove, Martin T. American Mineralogist, Vol. 82, Issue 3-4 https://doi.org/10.2138/am-1997-3-401	journal	April 1997
Structural phase transitions. II. Static critical behaviour Bruce, Alastair D. Advances in Physics, Vol. 29, Issue 1 https://doi.org/10.1080/00018738000101356	journal	February 1980
Momentum-resolved observations of the phonon instability driving geometric improper ferroelectricity in yttrium manganite Bansal, Dipanshu; Niedziela, Jennifer L.; Sinclair, Ryan Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-017-02309-2	journal	January 2018
PDFfit2 and PDFgui: computer programs for studying nanostructure in crystals Farrow, C. L.; Juhas, P.; Liu, J. W. Journal of Physics: Condensed Matter, Vol. 19, Issue 33 https://doi.org/10.1088/0953-8984/19/33/335219	journal	July 2007
Functional electronic inversion layers at ferroelectric domain walls Mundy, J. A.; Schaab, J.; Kumagai, Y. Nature Materials, Vol. 16, Issue 6 https://doi.org/10.1038/nmat4878	journal	March 2017
Accurate and simple analytic representation of the electron-gas correlation energy Perdew, John P.; Wang, Yue Physical Review B, Vol. 45, Issue 23, p. 13244-13249 https://doi.org/10.1103/PhysRevB.45.13244	journal	June 1992
Measurements and ab initio molecular dynamics simulations of the high temperature ferroelectric transition in hexagonal RMnO ₃ Tyson, T. A.; Wu, T.; Chen, H. Y. Journal of Applied Physics, Vol. 110, Issue 8 https://doi.org/10.1063/1.3656698	journal	October 2011
Lattice instabilities, isotope effect, and high- $T_{c}$ superconductivity in ${La}_{2 - x}$ ${Ba}_{x}$ ${CuO}_{4}$ Pickett, W. E.; Cohen, R. E.; Krakauer, H. Physical Review Letters, Vol. 67, Issue 2 https://doi.org/10.1103/PhysRevLett.67.228	journal	July 1991
Landau theory of topological defects in multiferroic hexagonal manganites Artyukhin, Sergey; Delaney, Kris T.; Spaldin, Nicola A. Nature Materials, Vol. 13, Issue 1 https://doi.org/10.1038/nmat3786	journal	October 2013
Domains in ferroelectric YMnO3 šafránková, M.; Fousek, J.; KiŽaev, S. A. Czechoslovak Journal of Physics, Vol. 17, Issue 6 https://doi.org/10.1007/BF01695179	journal	June 1967
Crossover between displacive and order/disorder behaviour in the Phi ⁴ model Padlewski, S.; Evans, A. K.; Ayling, C. Journal of Physics: Condensed Matter, Vol. 4, Issue 21 https://doi.org/10.1088/0953-8984/4/21/005	journal	May 1992
Electrostatic topology of ferroelectric domains in YMnO3 Jungk, Tobias; Hoffmann, Ákos; Fiebig, Manfred Applied Physics Letters, Vol. 97, Issue 1 https://doi.org/10.1063/1.3460286	journal	July 2010
Emergence of central mode in the paraelectric phase of ferroelectric perovskites Weerasinghe, Jeevaka; Bellaiche, L.; Ostapchuk, T. MRS Communications, Vol. 3, Issue 1 https://doi.org/10.1557/mrc.2013.5	journal	February 2013
The crystallography of correlated disorder Keen, David A.; Goodwin, Andrew L. Nature, Vol. 521, Issue 7552 https://doi.org/10.1038/nature14453	journal	May 2015
High-temperature lattice-dynamics evolution of $YMn O_{3}$ and $YbMn O_{3}$ Bouyanfif, H.; Salah, A. M.; Zaghrioui, M. Physical Review B, Vol. 91, Issue 22 https://doi.org/10.1103/PhysRevB.91.224104	journal	June 2015
Spin-phonon coupling and high-temperature phase transition in multiferroic material YMnO ₃ Gupta, Mayanak Kumar; Mittal, Ranjan; Zbiri, Mohamed Journal of Materials Chemistry C, Vol. 3, Issue 44 https://doi.org/10.1039/C5TC02096D	journal	January 2015
Effect of Ga doping on the multiferroic properties of $R {Mn}_{1 - x} {Ga}_{x} O_{3}$ $(R = Ho, Y)$ Zhou, H. D.; Denyszyn, J. C.; Goodenough, J. B. Physical Review B, Vol. 72, Issue 22 https://doi.org/10.1103/PhysRevB.72.224401	journal	December 2005
Implementation of the projector augmented-wave method in the ABINIT code: Application to the study of iron under pressure Torrent, Marc; Jollet, François; Bottin, François Computational Materials Science, Vol. 42, Issue 2 https://doi.org/10.1016/j.commatsci.2007.07.020	journal	April 2008
Unusual ferroelectric and magnetic phases in multiferroic $2 {H − BaMnO}_{3}$ ceramics Kamba, Stanislav; Nuzhnyy, Dmitry; Savinov, Maxim Physical Review B, Vol. 95, Issue 17 https://doi.org/10.1103/PhysRevB.95.174103	journal	May 2017
Y–O hybridization in the ferroelectric transition of YMnO3 Kim, Jinyoung; Cho, Kyung Chul; Koo, Yang Mo Applied Physics Letters, Vol. 95, Issue 13 https://doi.org/10.1063/1.3233943	journal	September 2009