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C. Doubrovsky 1 , F. Bouquet 1 , C. Pasquier 1 , P. Senzier 1

STUDY OF THE INTERPLAY BETWEEN SPIN, CHARGE AND LATTICE IN MULTIFERROIC OXIDES RMn2O5 (R= Nd , Pr). C. Doubrovsky 1 , F. Bouquet 1 , C. Pasquier 1 , P. Senzier 1 M. Greenblatt 3 , S. Petit 2 , G. Andre 2 , F. Damay 2 , P. Foury 1. phD director, Pascale Foury.

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C. Doubrovsky 1 , F. Bouquet 1 , C. Pasquier 1 , P. Senzier 1

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  1. STUDY OF THE INTERPLAY BETWEEN SPIN, CHARGE AND LATTICE IN MULTIFERROIC OXIDES RMn2O5 (R= Nd, Pr) C. Doubrovsky1, F. Bouquet1, C. Pasquier1, P. Senzier1 M. Greenblatt3, S. Petit2,G. Andre2, F. Damay2, P. Foury1 phD director, Pascale Foury 1Laboratoire de Physique des Solides (LPS), Orsay, France 2Labortaoire Léon Brillouin (CEA-CNRS), CEA Saclay, France 3Wright – RiemanLaboratories, RutgersUniversity, New Jersey

  2. I. 1 Multiferroics Spintronic Type I : Weaklycoupledorders(BiFeO3) 4 states memory Type II : Strongcouplingbetweenordersleading to ferroelectricity (RMn2O5) Electricalwriting/Magneticreading Issue : Microscopicorigin of the magneto-electriccouplingDzyaloshinskiiMoriya or Exchange interaction

  3. I. 2 Origin of the magneto-electriccoupling Magnetostriction effect Non colinear : Dzyaloshinskii-Moriya interaction O2- ligands shifts Colinear : Exchange interaction Mn3+ ions shifts P R3+ Mn4+ Mn3+ S-W Cheong et al. Nature (2007)

  4. J couplings in RMn2O5 Magnetic superexchange interactions Ji = 3,5 are shown by double sided arrows. P G Radaelli et al. J. P Condens. Matter (2008) • (ab) plane– Loops of 5 Mn spins – • J3Mn3+/Mn4+ J4Mn3+/Mn4+ through O2- J5Mn3+/Mn3+ • Along c – Mn4+ chains – • J1throughR3+ J2 through Mn3+

  5. I. 3 Rare earth influence in RMn2O5  Gal case R = Y, Tb, Ho, Er, Tm  3 to 4 transitions (<50K) TbMn2O5 Noda et al. J. P. Condens. Matter(2008) non magnetic R R= Bi (½ 0 ½) CP - ferroelectric R=La (00 ½) CP - not ferroelectric Lighter Rare Earth ?

  6. Syntheses, RutgersUniversity II.1 ThermodynamicProperties Specificheat on a PrMn2O5 powder LPS, PPMS Quantum design. Transitions at 20K and 25K

  7. II.2 MagneticProperties 132K Curie Law: θc = 132K C ~1.46 10-2emu.K.g-1.Oe-1 3,5 µB (<µeff>= <µMn4+ + µMn3+ + µPr3+ > = 4,1 µB ) 25K TC TN1 Susceptibility of a PrMn2O5 powder (SQUID, RowanUniversity, NJ) 25K transition AFM 20K transition not visible (smallrearangement of the magnetic moment)

  8. II.3 DielectricProperties Cp (pF) T(K) Dielectric constant of PrMn2O5 and TbMn2O5 powders(LPS, Orsay) No ferroelectric transition 20K effect ? electromagnon as suggested in TbMn2O5?

  9. III.1Nuclear structure of PrMn2O5 Powder X-ray diffraction pattern takenat 10 and 70K of a polycristallinesample Cristal beam line (SOLEIL) CentrosymmetricPbam structure confirmed No structural variation (> 10-3) between 50 & 10K  No significantmagneto-strictioneffect

  10. III.2Magnetic structure of PrMn2O5 λ= 2,4226 A Magneticspectra of PrMn2O5 powder, recorderd by elastic neutron diffraction (G4.1, Orphée LLB) IntegratedIntensity of the 2 sets of satelitespeaks • 2nd - ordercommensuratemagnetic transitions at : • 25K : q1 (1/2 00) • 20K : q2 (001/2) Origin : Another PrMn2O5 phase?

  11. III.2Magnetic structure of PrMn2O5 TbMn2O5 PrMn2O5 Mn3+ Mn4+ P Pr3+ O2- b a 25K - q1 (1/2 00) q(1/2 01/4) G. R. Blake, Physical Review B (2005) • Similar to TbMn2O5 and other RMn2O5 • All magneticatomsplay part in the magnetic structure

  12. Perspectives • Mesure and Modelisation of spinwaves J coupling values in PrMn2O5 & TbMn2O5 (Inelastic neutron diffraction) • Understanding the low –T transition TbMn2O5

  13. Thankyou for your attention

  14. Interplay between spin, charge and lattice in multiferroics RMn2O5 I.Magnetoelectriccoupling • Multiferroics • Origin of the magnetoelectriccoupling • Rare earthinfluency in RMn2O5 II.PrMn2O5caracterisation • Synthesis of RMn2O5 • Properties of PrMn2O5 III. Nuclear and magnetic structures of PrMn2O5 2/9

  15. In the ‘proper’ ferroelectrics, structural instability towards the polar state, associated with the electronic pairing, is the main driving force of the transition. • On the other hand, if polarization is only a part of a more complex lattice distortion or if it appears as an accidental by-product of some other ordering, the ferroelectricity is called ‘improper’

  16. Solid State Chemistry Pr6O11 + 12Mn 6 PrMn2O5 Mn (metal basis) washed in dilute HCl, dissolved in HNO3 XR- Results 600°C 1100°C O2 Ref. : H. Satoh, S. Suzuki, K. Yamamoto, N Kamegashira, Phase Stabilities of LnMn2O5 (Ln = rare earth), Alloys and Compounds (1995) 6/12

  17. Susceptibility a//H b//H c//H 0 10 20 30 40 50 PrMn2O5Electrolysis 1 mm

  18. TbMn2O5 CM magnetic structure Plan (ab) Along c direction Mn3+ Mn3+ Mn4+ Mn4+ b O2- Tb3+ a Colinear moments on a same site, with quite strange directions. Tb moment shave zero value when it is between AF ordered Mn layers. q(1/2 01/4)

  19. Other magnetic Structure of RMn2O5 TbMn2O5 Magnetic frustration along b b Loops of 5 spins : AFM order cannot be estblished a AFM along a

  20. Reversible flipping of electric polarization in TbMn2O5

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