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9/8/2009
1
ESM 2009 - Timisoara 1CARPATH
Alexandru STANCU
Professor, Director CARPATH
“Alexandru Ioan Cuza” University, Faculty of Physics, Department of Physics &Centre for Applied Research in Physics and Advanced TecHnologies (CARPATH)
Iasi, ROMANIA
“Alexandru Ioan Cuza” UNIVERSITY
IASI - ROMANIA
Centre for Applied Research in Physics and Advanced Technologies
Center of Excellence in Scientific Research (2006-2011) of The Romanian National Commission for Scientific Research in Universities
Preisach model of hysteresis in magnetic materials and FORC based identification techniques
European School on Magnetism 2009:Models in magnetism : from basic aspects to practical uses
September 1-10th 2009, Timisoara, Romania
ESM 2009 - Timisoara 2CARPATH
Outline
Introduction – about hysteresisScalar Preisach modelFORC identification techniqueExamples – ferromagnetic systemsHysteretic processes in spin-transition materialsConclusions
9/8/2009
2
ESM 2009 - Timisoara 3CARPATH
Which hysteresis model we choose in a given situation ?
How we choose ?Criteria ? To simulate correctly high order magnetization curves ?Identification methodologies …In many papers the identification is made using an arbitrary selection of
magnetization processes. Is it OK?
Can we use for identification only the Major Hysteresis Loop ?
ESM 2009 - Timisoara 4CARPATH
Identical MHL for essentially different systems
-20000 -10000 0 10000 20000
-1.0
-0.5
0.0
0.5
1.0
Nor
mal
ized
mom
ent
Applied field
-20000 -15000 -10000 -5000 0 5000 10000 15000 20000-20000
-15000
-10000
-5000
0
5000
10000
15000
20000
Hα
Hβ
-1.00E-10
2.94E-9
5.98E-9
9.02E-9
1.21E-8
1.51E-8
1.81E-8
2.12E-8
2.42E-8
2.73E-8
3.03E-8-20000 -15000 -10000 -5000 0 5000 10000 15000 20000
-20000
-15000
-10000
-5000
0
5000
10000
15000
20000
Hα
Hβ
-1.00E-10
2.95E-9
6.00E-9
9.05E-9
1.21E-8
1.52E-8
1.82E-8
2.13E-8
2.43E-8
2.74E-8
3.04E-8
9/8/2009
3
ESM 2009 - Timisoara 5CARPATH
To understand … Preisach model
m0/m0s
H
+1
–1
A(Hα,0)B(Hβ,0)
Hc
S(Hs,0)
IHiI
F. Preisach 1935M.A. Krasnoselskii & A.V. Pokrovskii 1983, 1989I.D. Mayergoyz 1986
Ps
H0
x
y
z
ϕ0
ϕ
θθ0
Stoner Wohlfarth model
ESM 2009 - Timisoara 6CARPATH
Preisach plane
T(Hα1,Hβ1)
Hα
Hβ
M(Hα1,Hβ1)
m0/m0s
H
+1
–1
A(Hα1,0)B(Hβ1,0)
O
T0(Hm,–Hm)
M(Hα1,Hβ1)
M0(Hm,−Hm)
Q
Q0
P
P0
P(Hα,Hβ)
Hα
Hβ Hc0
O
hs
hchi
hc=const.
hi=const.
9/8/2009
4
ESM 2009 - Timisoara 7CARPATH
MHL
Hα
Hβ
O
Q0
P0
+
–
M0
L(t)
Hα
Hβ
O
Q0
P0
+
–
M0
H
-Hm
Hm
Hα
Hβ
O
Q0
P0
+ –
M0
H
-Hm
Hm
-3000 -2000 -1000 0 1000 2000 3000
-1.0
-0.5
0.0
0.5
1.0
H
MHL(+) MHL(–)
Nor
mal
ised
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
ESM 2009 - Timisoara 8CARPATH
Magnetization processes
Hα
Hβ
O
Q0
P0
M
L1 (Hα=H)
L2
M0
Hα=Hβ
Hα
Hβ
O
Q0
P0
I
II
III
L1 (Hα=H)
L2 (Hβ=H)
M0
Hα
Hβ
O
Q0
P0
I
II
III
L1 (Hα=H)
L2 (Hβ=H)
M0
H
H
H
9/8/2009
5
ESM 2009 - Timisoara 9CARPATH
For more examples … Hystersoft
http://www.eng.fsu.edu/~pandrei/HysterSoft/index1.html
Petru AndreiDepartment of Electrical and Computer EngineeringFlorida State University and Florida A&M University
Univ. of Florida - Iasi University – Technical Univ. Wien
ESM 2009 - Timisoara 10CARPATH
Generalized use of FORCs
Conclusion: FORC diagram can be calculated for ANY hysteretic system.
9/8/2009
6
ESM 2009 - Timisoara 11CARPATH
Conclusion …
FORC distribution and FORC diagram can be obtained from experimental data.
Problems:How we “decode” the information contained in an experimental FORC diagram ? Does it contain sufficient information to identify ANY hysteresis model ?
ESM 2009 - Timisoara 12CARPATH
-200.0n0.0200.0n400.0n
600.0n800.0n1.0µ1.2µ1.4µ1.6µ1.8µ
-1000
-500
0
500
-200.0n0.0
200.0n400.0n600.0n800.0n
1.0µ1.2µ1.4µ1.6µ1.8µ
-1000
-500
0
5000 1000 2000
Hi (Oe) Hi (Oe)
Hc (Oe)
0 90 180 270 3600
90
180
270
360
θ (deg)
θ r (deg
)
100 110 120 130 140 150100
110
120
130
140
150
TA(K)
T B(K
)
Ni
Co
Zn
Fe pure
9/8/2009
7
ESM 2009 - Timisoara 13CARPATH
FORC diagram method.
-3000 0 3000
-0.7
0.0
0.7MHL+
MHL-
m-FORC
(Hr,H)
Hr
Nor
mal
ized
mag
netic
mom
ent
Applied magnetic field (Oe)
H
( ) ( )2 ,1,2
FORC rr
r
m H HH H
H Hρ
−∂= −
∂ ∂
T(Hα1,Hβ1)
Hα
Hβ
M(Hα1,Hβ1)
m0/m0s
H
+1
–1
A(Hα1,0)B(Hβ1,0)
O
T0(Hm,–Hm)
M(Hα1,Hβ1)
M0(Hm,−Hm)
Q
Q0
P
P0
Rectangular hysteron
Preisach plane
P(Hα,Hβ)
Hα
Hβ Hc0
O
hs
hchi
hc=const.
hi=const.-3000 -2000 -1000 0 1000 2000 3000
-1.0
-0.5
0.0
0.5
1.0
m
H
ESM 2009 - Timisoara 14CARPATH
FORC distribution
-2.0 -1.5 -1.0 -0.5 0.0 0.5 1.0 1.5 2.0-2.0
-1.5
-1.0
-0.5
0.0
0.5
1.0
1.5
2.0dH=dH
αdHr=dH
β
B(H+dH,Hr+dHr)A(H,Hr)
Hβ
Hα
-2.0 -1.5 -1.0 -0.5 0.0 0.5 1.0 1.5 2.0-1.0
-0.5
0.0
0.5
1.0
H=Hα
Hr=Hβ
Nor
mal
ized
mag
netic
mom
ent
A
B
A
B
A
B
Case A ρ = 0
Case B ρ < 0
Case C ρ > 0
9/8/2009
8
ESM 2009 - Timisoara 15CARPATH
Symmetry
-0.2 0.0 0.2 0.4
-0.4
-0.2
0.0
0.2
Hα
Hβ
-0.2 0.0 0.2 0.4
-0.4
-0.2
0.0
0.2
Hα
Hβ
-8 -4 0 4 8-1.0
-0.5
0.0
0.5
1.0
m
H (arb.units)
-2 0 2 4 6-6
-4
-2
0
2
H (arb. units)
Hr (
arb.
uni
ts)
-2 0 2 4 6-6
-4
-2
0
2
H (arb. units)
Hr (
arb.
uni
ts)
ESM 2009 - Timisoara 16CARPATH
Magnetic characterization of samples using FORC diagrams
Main problemsState dependent interaction field distributionReversible magnetization processes
9/8/2009
9
ESM 2009 - Timisoara 17CARPATH
Mean field interactions
( )0
m f HH H mα
⎧ =⎨
= +⎩
H
m 1
α
-4000 -2000 0 2000 4000
-1.0
-0.5
0.0
0.5
1.0 m(Happl+αm)
Magnetic field (Oe)
Nor
mal
ized
mag
netic
mom
ent
ESM 2009 - Timisoara 18CARPATH
Preisach – singular distributions
α=0
9/8/2009
10
ESM 2009 - Timisoara 19CARPATH
Preisach – singular distributions
α<0
0 2 4 6 8 10 12
-6
-4
-2
0
2
4
6
Hc (a. u.)
Hi (
a. u
.)
ESM 2009 - Timisoara 20CARPATH
Preisach – singular distributions
α>0
9/8/2009
11
ESM 2009 - Timisoara 21CARPATH
Operative plane
-4000 -2000 0 2000 4000
-1.0
-0.5
0.0
0.5
1.0 m(Happl+αm)
Magnetic field (Oe)
Nor
mal
ized
mag
netic
mom
ent
-0.2 0.0 0.2 0.4
-0.4
-0.2
0.0
0.2
Hα
Hβ
-0.2 0.0 0.2 0.4
-0.4
-0.2
0.0
0.2
Hα
Hβ
ESM 2009 - Timisoara 22CARPATH
FORC – patterned medium
0 2 4 6 8 10 12
-6
-4
-2
0
2
4
6
Hc (a. u.)
Hi (
a. u
.)
0 2 4 6 8 10 12
-6
-4
-2
0
2
4
6
Hc (a. u.)
Hi (a
. u.)
0 2 4 6 8 10 12
-6
-4
-2
0
2
4
6
Hc (a. u.)
Hi (a
. u.)
9/8/2009
12
ESM 2009 - Timisoara 23CARPATH
Magnetizing mean field interactions
-3000 -2000 -1000 0 1000 2000 3000
-1.0
-0.5
0.0
0.5
1.0
m
H
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
0 1000 2000
ESM 2009 - Timisoara 24CARPATH
Alpha = 0
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
0 1000 2000 3000 4000
9/8/2009
13
ESM 2009 - Timisoara 25CARPATH
Alpha = 300
0.0000000
0.0000005
0.0000010
0.0000015
0.0000020
0
0.0000000
0.0000005
0.0000010
0.0000015
0.0000020
0
0 1000 2000 3000 4000
ESM 2009 - Timisoara 26CARPATH
Alpha = 500
0.00000000.00000020.00000040.00000060.00000080.00000100.0000012
0
1000
0.00000000.00000020.00000040.00000060.00000080.00000100.0000012
0
10000 1000 2000 3000 4000
9/8/2009
14
ESM 2009 - Timisoara 27CARPATH
Alpha = 600
0.0000000
0.0000002
0.0000004
0.0000006
0.0000008
-1000
0
1000
0.0000000
0.0000002
0.0000004
0.0000006
0.0000008
-1000
0
1000
0 1000 2000 3000 4000
ESM 2009 - Timisoara 28CARPATH
Alpha = 1000
0.0000000
0.0000001
0.0000002
0.0000003
0.0000004
-1000
0
1000
0.0000000
0.0000001
0.0000002
0.0000003
0.0000004
-1000
0
1000
0 1000 2000 3000 4000
9/8/2009
15
ESM 2009 - Timisoara 29CARPATH
Operative plane
0 200 400 600 800 1000
-100
-50
0
50
100
150
200
250H
iMax
alpha
HiMax
0.00000000.00000020.00000040.00000060.00000080.0000010
0
0.0000000
0.0000002
0.0000004
0.0000006
0.0000008
0.0000010
0
0 1000 2000 3000 4000
200 400 600 800 1000 1200 1400 1600 1800 2000 2200
-100
0
100
200
300
400
500
600
700
HiM
ed, H
iSig
Hc
HiMed HiSig
ESM 2009 - Timisoara 30CARPATH
0.00000000.00000020.00000040.00000060.00000080.0000010
0
0.0000000
0.0000002
0.0000004
0.0000006
0.0000008
0.0000010
0
0 1000 2000 3000 4000
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
0
0 1000 2000 3000 4000
Compare the results…
9/8/2009
16
ESM 2009 - Timisoara 31CARPATH
Reversible vs. irreversible magnetization processes
-3000 0 3000
-0.7
0.0
0.7MHL+
MHL-
m-FORC(Hr,H)
Hr
Nor
mal
ized
mag
netic
mom
ent
Applied magnetic field (Oe)
H
ESM 2009 - Timisoara 32CARPATH
Relation with deltaM measurement
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
-1000 0 1000
-0.5
0.0
0.5
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
Stancu A., Bissell PR, Chantrell RW, JAP, 2001
9/8/2009
17
ESM 2009 - Timisoara 33CARPATH
Problems with deltaM/Henkel plots
Sensitive to the quality of the demagnetization state in IRM processNegative (demagnetizing-like) deltaM is compatible with statistical interactions (no preference to demagnetizing interactions)
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
-2000 -1000 0 1000 2000 3000
-3000
-2000
-1000
0
1000
2000--3
2234567899
2
ESM 2009 - Timisoara 34CARPATH
BaFe (oriented sample)-positive deltaM
-3000 -2000 -1000 0 1000 2000 3000
-1.0
-0.5
0.0
0.5
1.0
m
H
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
-1000
0
1000
-0.0000010.0000000.0000010.0000020.0000030.0000040.0000050.000006
-1000
0
10000 1000 2000
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
Stancu A., Bissell PR, Chantrell RW, JAP, 2001
9/8/2009
18
ESM 2009 - Timisoara 35CARPATH
BaFe (random sample)
-4000 -2000 0 2000 4000
-1.0
-0.5
0.0
0.5
1.0
m
H
-0.00000020.00000000.00000020.00000040.00000060.00000080.00000100.00000120.00000140.00000160.0000018
-1000
0
1000
-0.00000020.00000000.00000020.00000040.00000060.00000080.00000100.00000120.00000140.00000160.0000018
-1000
0
1000
0 1000 2000 3000
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
Stancu A., Bissell PR, Chantrell RW, JAP, 2001
ESM 2009 - Timisoara 36CARPATH
Video magnetic tape
-2000 -1000 0 1000 2000-1.0
-0.5
0.0
0.5
1.0
IRM DCD MHL deltaM
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
0.0000000
0.0000005
0.0000010
0.0000015
0.0000020
-1000
0
1000
0.0000000
0.0000005
0.0000010
0.0000015
0.0000020
-1000
0
1000
0 2000
Stancu A., Bissell PR, Chantrell RW, JAP, 2001
9/8/2009
19
ESM 2009 - Timisoara 37CARPATH
Experimental procedure - SORC
Order “0”
Order “1”
Order “2”
-1000 0 1000
-0.5
0.0
0.5
Nor
mal
ized
Mag
netic
Mom
ent
Applied Magnetic Field (Oe)
ESM 2009 - Timisoara 38CARPATH
Second-Order Reversal Curves
- 8 - 6 - 4 - 2 0 2 4 6 8- 1 . 0
- 0 . 8
- 0 . 6
- 0 . 4
- 0 . 2
0 . 0
0 . 2
0 . 4
0 . 6
0 . 8
1 . 0
m/m
s
A p p l i e d f i e l d ( a . u . )- 8 - 6 - 4 - 2 0 2 4 6 8
- 1 . 0
- 0 . 8
- 0 . 6
- 0 . 4
- 0 . 2
0 . 0
0 . 2
0 . 4
0 . 6
0 . 8
1 . 0
A p p l i e d f i e l d ( a . u . )
-4 -2 0 2 4-4
-2
0
2
4
H
Hr
-4 -2 0 2 4-4
-2
0
2
4
H
Hr
-0.20
-0.10
0
0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80-4 -2 0 2 4
-4
-2
0
2
4
H
Hr
-0.050
-0.040
-0.030
-0.020
-0.010
0
0.010
0.020
0.030
0.040
0.050
0.060
0.070
0.080
0.090
0.10
FORC SORC FORC-SORC
Stancu A., Andrei P., JAP, 2005
Error evaluation !!!
9/8/2009
20
ESM 2009 - Timisoara 39CARPATH
Experimental data
-5000 -4000 -3000 -2000 -1000 0 1000 2000 3000 4000 5000-0.15
-0.10
-0.05
0.00
0.05
0.10
0.15
m
H -5000 -4000 -3000 -2000 -1000 0 1000 2000 3000 4000 5000-0.15
-0.10
-0.05
0.00
0.05
0.10
0.15
m
H-5000 -4000 -3000 -2000 -1000 0 1000 2000 3000 4000 5000
-0.15
-0.10
-0.05
0.00
0.05
0.10
0.15
m
H
0 1000 2000 3000 4000 5000-5000
-4000
-3000
-2000
-1000
0
0 1000 2000 3000 4000 5000-5000
-4000
-3000
-2000
-1000
0
0 1000 2000 3000 4000 5000-5000
-4000
-3000
-2000
-1000
0
ESM 2009 - Timisoara 40CARPATH
FORC-Preisach distributions
The distribution of the interaction fields is NOT stable. It depends on the magnetic state. Preisach distribution is moving and has variable variance.Reversible magnetization processes are coupled with the irreversible ones
9/8/2009
21
ESM 2009 - Timisoara 41CARPATH
FORC …
FORC distribution gives a static, average image of the interactions while the interaction field distribution is changing during the magnetization processesWithout a proper model the dynamics can’t be observed and evaluated
ESM 2009 - Timisoara 42CARPATH
FORC technique applied to other systems
Preisach and FORC identification technique can be applied to ANY hysteretic system …
9/8/2009
22
ESM 2009 - Timisoara 43CARPATH
Spin crossover systems
Fe(II)d6
Low spin state
Diamagnetic S=0 Paramagnetic S=2
Different colors
Different volumes
High spin state
Different vibrational properties
Δ0 t2g
eg egt2g
Ea
Ener
gy
Metal-ligand distance
LS HS Δ
0 200 400 600 800 10000.0
0.2
0.4
0.6
0.8
1.0
nHS
Pressure[bar]
110 120 130 140 150 1600.0
0.2
0.4
0.6
0.8
1.0
nHS
T[K]
0 10000 20000 30000 40000 50000 60000 700000.0
0.2
0.4
0.6
0.8
1.0
55 K
50 K
45 K
nHS
temps(sec)
ESM 2009 - Timisoara 44CARPATH
Thermal hysteresis in spin transition materials
115 120 125 130 135 140 145 1500.0
0.2
0.4
0.6
0.8
1.0
n HS
T(K)
a
110 115 120 125 130 135 1400.0
0.2
0.4
0.6
0.8
1.0
b
n HS
T(K)
100 105 110 115 120 125 1300.0
0.2
0.4
0.6
0.8
1.0
n HS
T(K)
c
95 100 105 110 1150.0
0.2
0.4
0.6
0.8
1.0
n HS
T(K)
d
fast
514 nm
3T2
1T2
slow
fast
fast
kHL
1A1
5T2
3T1
1T1
ΔHS
LSmetal-ligand distance
ener
gy LIESST
The LIESST Effect (Light Induced Excited Spin State Trapping)
9/8/2009
23
ESM 2009 - Timisoara 45CARPATH
Preisach model for thermal hysteresis
0.4 0.6 0.8 1.0 1.2 1.4 1.6
0.4
0.6
0.8
1.0
1.2
1.4
1.6
P'(Tα,T
β)
Tα=T
β
Tβ
Tα
0.4 0.6 0.8 1.0 1.2 1.4 1.6
0.4 0.6 0.8 1.0 1.2 1.4 1.6
0.0
0.2
0.4
0.6
0.8
1.0
P(T,Tr)
T/T0
T=T0
nHS
/NT=T
α
Tr=T
β
Normalized sample temperature
90 100 110 120 1300.0
0.2
0.4
0.6
0.8
1.0
nH
S
T[K]
Tanasa et al, PRB 2005; Enachescu et al, PRB 2005
ESM 2009 - Timisoara 46CARPATH
Thermal hysteresis. Effect of impurities
100 110 120 130 140 150100
110
120
130
140
150
TA(K)
T B(K
)
Ni
Co
Zn
Fe pure
0 5 10 15 20 25105
110
115
120
125
130
135
140
c(K)
b(K
)
9/8/2009
24
ESM 2009 - Timisoara 47CARPATH
Pressure & temperature hysteresis
0 200 400 600 800 1000 12000.0
0.2
0.4
0.6
0.8
1.0
p2n H
S
p(bar)
Δp=180bar
p1
168 170 172 174 176 178 180 1820.0
0.2
0.4
0.6
0.8
1.0
n HS
T (K)
ΔT=2K
600 750 900
0.0
0.2
0.4
0.6
0.8
1.0
170 175 180 1850.0
0.2
0.4
0.6
0.8
1.0600 750 900
p(bar)3
T (K)
2
1
12
34
4
5 6
5
6
7
7
8
9
9
8
p(bar)
initial statefinal state
nHSn
HS
0400
8001200
1600
0.0
0.2
0.4
0.6
0.8
1.0
160165
170175
180185
n HS
tempe
ratur
e T(K
)
pression p(bar)
Multi-ferroic materials
ESM 2009 - Timisoara 48CARPATH
Elastic model of hysteresis
Low spin state
High spin state
Molecular volume change during transitionelastic interactions appear inside the sample
System shape and volume change during transition
L. Stoleriu, C. Enachescu, A. Stancu, A. Hauser, IEEE Trans. Magn., 2008C. Enachescu L. Stoleriu, A. Stancu, A. Hauser, PRL 2009
9/8/2009
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ESM 2009 - Timisoara 49CARPATH
Elastic model of hysteresis and relaxation
Low spin state
High spin state
For every particle the following differential system is solved at every step:
2
2
2
2
⎧= −⎪⎪
⎨⎪ = −⎪⎩
i ixi
i iyi
d x dxm F
dtdtd y dy
m Fdtdt
μ
μ
Fxi are the algebraic sums of forces acting on particule on the two directionsµ is the damping constant
ESM 2009 - Timisoara 50CARPATH
Cooperativity effect – ralaxation process
0 2 4 6 8 10
0,0
0,2
0,4
0,6
0,8
1,0
Hig
h sp
in fr
actio
n
Monte Carlo time
9/8/2009
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ESM 2009 - Timisoara 51CARPATH
Size effects in nanoparticulate spin transition materials
A. Rotaru, Ph.D. Thesis, 2009
ESM 2009 - Timisoara 52CARPATH
ConclusionsThe extensive use of the FORC technique induced a new interest in the Preisach modelUnfortunately, in many cases the analysis is not completeWe recommend at least a mean field analysis / work in the operative planeAll FORC analysis should be coupled with a statistical model specific to the physical system analyzed
9/8/2009
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ESM 2009 - Timisoara 53CARPATH