International Symposium on Present and Future of Material...
Transcript of International Symposium on Present and Future of Material...
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International Symposium on Present and Future of Material Sciences Osaka university 17-18 november 2015
Solid State chemistry of electron correlated oxides: From perovskite derivatives to triangular metallic lattices Bernard Raveau Laboratoire CRISMAT, UMR 6508 CNRS-ENSICAEN, Univ .of Caen, France
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Electron correlated systems :transition metal oxides
Multiple transitions: structural, electrical,magnetic
Cuprates: high Tc superconductivity Manganites: Colossal MagnetoResistance CMR Cobaltates : high t° thermoelectricity Ferrates : multiferroicity
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New Transition Metal Oxides for New Properties
TM
valence
A: countercation TM
coordination
Oxygen stoichiometry
Transport, dielectric
Magnetic properties
Structure
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La4BaCu5O13
non supercond La2-xBaxCuO4 La2-xSrxCu2O6 YBa2Cu3O7
supercond. supercond. supercond.
- mixed valence Cu2+/ Cu3+
- 2D-Structure : Jahn-Teller effect of copper - Apical/equatorial oxygen O- : Cu3+ 3d8 Cu 2+ 3d9L
3D
superconducting copper oxides
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Maeda & al (1988) Takano & al (1988) Borel &al (1987 )
Bi2Sr2CuO6+δ
Superconductivity up to 110 K
Bi2Sr2CaCu2O8+δ Bi2Sr2Ca2Cu3O10+δ
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Colossal Magnéto-Resistance Perovskites : Ln1-x (Ca,Sr)xMnO3
Transition paramagnetic insulator ferromagnetic metal
- mixed valence Mn3+/Mn4+ : double exchange (« metal ») - Jahn-Teller effect of Mn3+: control of structural distortion
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AFM insulator FM metal charge ordering charge delocalisation Mn3+ and Mn4+ mixed valence J-T effect of Mn3+ Mn3+/Mn4+
Réalisation doping - On Mn3+ sites : Ga3+, Cr3+
or on Ca2+ sites: Ba2+
structural transition
Colossal Magneto-Resistance Perovskites : Pr0.5Ca0.5MnO3
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Thermoelectric cobalt oxides :« misfit »
(Bi0.87SrO2)2(CoO2)1.82
-mixed valence Co3+/Co4+
- 2D-structure - triangular cobalt lattice
- p-type semi-metal - High TEP : ~140 µVK-1 - low thermal conductivity
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Oxygen Deficient Double Perovskites : LnBaCo2O5.5+δ
-mixed valence: Co2+/Co3+ (-0.5<d<0) Co3+/Co4+ (0<d<+0.5) - Charge order and delocalisation - disproportionation: 2Co3+=Co4+ +Co2+
Numerous magnetic transitions e.g. metal-insulator , PM-AFM transition, high magneto-résistance
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Swedenborgite:the « 114 family »
Valldor & al Solid State Sci.4,923(2002)
YBaCoII3CoIII O7
Geometric frustration
Spin glass :Tf =66 K
Antiferromagnet: TN = 110 K
Mixed valence in a tetrahedral system
Kagome layers & triangular layers
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Changing the cobalt mixed valence
into Co2IICo2
III instead of Co3II Co1
III
CaBaCo4O7
Trigonal aH, cH orthorhombic aOaHV3, b~bH, c~cH
Charge ordering (BVS)
Co2, Co3 (K layers) :Co2+
Co1(T layers), Co4(K layers) :Co2+/Co3+
Co3+ =Co3d6 Co2+ = Co3d7L
V..Caignaert et al. Phys.Rev. B 2010
Lifting of the geometric frustration
Noncentro :Pbn21( polar axis :c)
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CaBaCo4O7: Ferrimagnet TC= 64 K
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Magnetic Structure of CaBaCO4O7
FM Co2+ zig zag chains // to b AFM coupled with co3+ and Co2+L
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CaBaCo4O7: dielectric permittivity & loss vs T at 100 kHz.The coincidence of the
peaks and TC evidences the spin and charge coupling.
K.Singh et al Phys. Rev. B 86, 024410 (2012)
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CaBaCo4O7: Electric polarization vs T showing a transition around TC and
sign change of P by reversing E, suggesting spin driven ferroelectricity.
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CaBaCo4O7: Magnetodielectric effect vs magnetic field at different t°.
E and H are perpendicular to each other.
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sharp transition along b @TC=64 K
(100 Oe)
Sharp transition along c @ TC=64 K
(100 kHz)
CaBaCo4O7 : magnetoelectric coupling along c
Specific heat: 0Tblue, 1Tgreen, 2T red
Gigantic variation of the polarisation
along c: ΔP=17mC/m2 @ 10K (Ec=1.1 kV/cm)
But cannot be reversed completely by
changing the polarity of E(14kV/cm)
Caignaert et al PRB 88, 174403 (2013)
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Polarisation along polar axis c, with H along b
Large increase of the polarisation
with the applied magnetic field
Magnetoelect. coeff α32 and β322
Largest ME effects are close TC
Caignaert et al PRB 88, 174403 (2013)
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Research of mixed valent Fe(II)- Fe(III) oxides
Trigonal YBaCo4O7 Spinel Fe3O4
Co(II)-Co(III) Fe(II)-Fe(III)
kagome tetrahedral layers kagome octahedral layers
triangular tetrahedral layers triangular tetrahedral layers
frustrated magnetic structure ferrimagnet
complex magnetic transitions complex charge ordering
« 114 » oxides : CaBaFe4O7 & YBaFe4O7
B.Raveau & al Chem .Mater. V.Caignaert & al chem Mater. 21,1116 (2009)
20, 6295 (2008)
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Fe
1
Fe
2
Trigonal CaBaFe4O7
B.Raveau & al Chem .Mater. 20, 6295 (2008)
0 50 100 150 200 250 300 350 400
0.4
0.6
0.8
1.0
1.2
1.4
1.6
1.8
2.0
2.2
2.4
2.6
Zfc
Fc H = 0.3 T
M (
µB/f
.u.)
T (K)
-6 -5 -4 -3 -2 -1 0 1 2 3 4 5 6
-3.0
-1.5
0.0
1.5
3.0
-3.0
-1.5
0.0
1.5
3.0
-3.0
-1.5
0.0
1.5
3.0
-3.0
-1.5
0.0
1.5
3.0
5K
M (
µb/f
u)
Field (T)
50K
150K
250K
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CaBaFe2IIFe2
IIIO7
Mexp =3mB / f.u.
Fe(II) : HS (tetrahedral) eg3 t2g
3
Fe(III) : HS (tetrahedral) eg2 t2g
3
ferromagnetism : Mth=18mB/f.u.
Ferrimagnetic : AFM coupling between kagome & triangular layers
Geometric frustration +charge ordering ?
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Investigation of Y-Ba-Fe-O system YBaFe4O7 cubic instead of trigonal
ac= 8.9 A ~ aH 2
1/2 similarity with spinel But Fe in tetrahedra only!
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(111)C layers in YBaFe4O7
Kagome
(001)H layers in CaBaFe4O7
YBaFe4O7 CaBaFe4O7
Kagome & Triangular Layers of FeO4 Tetrahedra
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Triangular Tunnels obstructed by YO6 Octahedra
YBaFe4O7 :
View along <110>C
CaBaFe4O7 :
View along <100>H
V.Caignaert & al Chem. Mater. 21, 1116 (2009)
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0 50 100 150 2007,0x10
-5
8,0x10-5
9,0x10-5
1,0x10-4
1,1x10-4
1,2x10-4
1,3x10-4
1,4x10-4
1,5x10-4
1,6x10-4
1,7x10-4
1,8x10-4
0,0030 0,0035 0,0040 0,0045 0,0050 0,0055 0,0060 0,0065 0,0070
102
103
104
105
(
.c
m)
1/T (K-1)
30 40 50 60 701.5x10
-4
1.6x10-4
1.6x10-4
1.7x10-4
1.7x10-4
1.8x10-4
1.8x10-4
1.9x10-4
1000Hz
10000Hz
' (e
mu
.g-1)
T (K)
1000Hz
10000Hz
' (
em
u.g
-1)
T (K)
Spin glass like behavior of YBaFe4O7
V.CAIGNAERT & al Chem. Mater. 21,1116 (2009)
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0 50 100 150 200 250 300
0.010
0.015
0.020
0 100 200 300
0.000
0.001
0.002
ZFC
FC
M (
mB/f
.u.)
Temperature (K) Fig. 1M
FC-M
ZF
C (
mB/f
.u.)
T (K)
mixed valence iron oxides: Fe3+/Fe4+ ? Perovskites Ln2Ba3Fe5O15-δ
Sm0.4Ba0.6FeO3-x: cubic Short range AFM interactions from PXRD under low field Tapez une équation ici.
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Nanoscale Ordered Quintuple perovskite Ln2Ba3Fe5O15- δ
HRTEM : Tetragonal « 5ap »:
Semi ordered distribution of Sm/Ba layers
Sequence: Sm-(Ba/Sm)4-Sm ?
Ln2Ba3Fe5O15-δ
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High angle annular dark field STEM
HAADF-STEM
I~ Z2: Z=56 for Ba , Z=62 for Sm
Layered ordering is:
« Sm-Ba-Sm/Ba-Sm/Ba-Ba-Sm »
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Ln2Ba3Fe5O15-δ :EELS elemental mapping
HAADF Fe Sm Ba O-K colour
Sm
Ba
Sm/Ba
Sm/Ba
Ba
Sm
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Schematic representation of quintuple perovskite structure of
Ln2Ba3Fe5O15-δ represented as intergrowth of
double and triple perovskite structures.
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EELS fine structure of Sm2-εBa3+εFe5O15-δ; (Left panel) O-K edge fine
structure signatures from the regions indicated in the central panel.
Structural model with indicated EELS integration areas. (Right panel) Fe-L2,3
fine structure signatures from the regions indicated in the central panel with
references for 4, 5 and 6-fold coordinated Fe3+, and a simultaneously acquired
and energy-shifted Ba M5 edge.
O vacancies in the median layers
Fe3+/Fe4+ mixed valence
Fe3+3d5 Fe3+3d5 L
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Ln2Ba3Fe5O15-δ: Nanoscale chemical twinning
HRTEM
HAADF-STEM Hinders long range AFM ordering
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Key Factors: Impact on Physics
TM valence: single, mixed, charge ordering, possible transitions vs T « A » Counter Cation: influences the structure (size) and TM valence (acido-basic: bond competition) TM coordination: Tetrahedral, octahedral, pyramidal,square influences structure, crystal field and chemical bonding Oxygen issue : stoichiometry, order- disorder of vacancies, influences TM valence and coordination, influences structure, issue of charge (O2- or O-) Structure : geometry of the lattice («square » or « triangular »),cationic & anionic order-disorder, struct. distortions, dimensionality, centro or non-centro symmetry, commensurability (or non)
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Aknowledgements
V. Caignaert (Caen) S. Turner ( Antwerp) O. Lebedev (Caen) Md. Motin Seikh (Santiniketan) V. Hardy (Caen) A. Kundu (New Dehli) N. Gauquelin (Antwerp) V. Cherepanov (Ekaterinburg)
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PERSEVERANCE WORK LUCK
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Interactions 3d-4f: Ba2LnFeO5 apparentés aux pérovskites
Ba2YFeO5: AFM, TN=5.1 K Super-super échange Fe-O-O-Fe: J5
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10
20
0
10
20
30
0
10
20
30
0 2 4 6 8 10 12 14
5
10
0 5 10 15 20 25 300
10
20
30
10
20
4
8
12
10
20(c) Gd
Cp (J
K-1 m
ol -1)
Cp (
J K
-1 m
ol-1
)
(e) Dy
(f) Ho
(d) Y
T(K)
(h) Yb
Ba2LnFeO
5(a) Sm
(b) Eu
(g) Er
0 1 2 3 4 5 6 7 8 90
2
4
6
8
10
M(m
B/f
.u.)
H(Tesla)
Ba2LnFeO
5
Sm
Eu
Gd
Dy
Ho
Y
Er
Yb
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0.86 0.88 0.90 0.92 0.94 0.96
4
5
6
7
8
9
10
11
Sm
Eu
Gd
DyHo
Y
Er
Yb
ionic radius VI (A)
tran
sit
ion
tem
pera
ture
(K
) from specific heat
from magnetic data
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What about the Future of Solid State Chemistry in Strongly Correlated Oxides?
Discovery of new oxides for new properties
Numerous results on nanomaterials, hybrids.
but
Chemistry of bulk materials: very few new compounds
Methods of synthesis: e.g.high pressure,
soft chemistry, electrochemistry, laser ablation in thin films
and or
Use new methods of investigation for design of new
frameworks: HRTEM, HAADF-STEM,EELS