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Electronic Structure Near The Mott Transition: Gabriel Kotliar
Electronic Structure Near The Mott Transition: Gabriel Kotliar
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The electron in a solid: wave picture
Momentum Space , bands, k in Brillouin zone is good
quantum number.
e 2 k F (k F l ) Maximum metallic
h resistivity 200 mohm cm
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Standard Model of Solids
Qualitative predictions: low temperature dependence of
thermodynamics and transport
~ const CV ~ T RH ~ const
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The electron in a solid: particle picture.
NiO, MnO, Array of atoms is insulating if a>>aB. Mott:
correlations localize the electron
e_ e_ e_ e_
Superexchange
1
T
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Mott : Correlations localize the electron
Low densities, electron behaves as a particle,use
atomic physics, work in real space.
One particle excitations: Hubbard Atoms: sharp excitation
lines corresponding to adding or removing electrons. In
solids they broaden by their incoherent motion, Hubbard
bands (eg. bandsNiO, CoO MnO.)
H H H+ H H H motion of H+ forms the lower
Hubbard band
Physics. RUTGERS
Localization vs Delocalization
Strong Correlation Problem
A large number of compounds with electrons in partially filled
shells, are not close to the well understood limits (localized
or itinerant). Non perturbative problem.
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Correlated Materials do big things
Huge resistivity changes V2O3.
Copper Oxides. .(La2-x Bax) CuO4 High
Temperature Superconductivity.150 K in the
Ca2Ba2Cu3HgO8 .
Uranium and Cerium Based Compounds.
Heavy Fermion Systems,CeCu6,m*/m=1000
(La1-xSrx)MnO3 Colossal Magneto-
resistance.
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Strongly Correlated Materials.
Large thermoelectric response in CeFe4 P12
(H. Sato et al. cond-mat 0010017). Ando
et.al. NaCo2-xCuxO4 Phys. Rev. B 60,
10580 (1999).
Huge volume collapses, Ce, Pu
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The Mott transition
Electronically driven MIT.
Forces to face directly the localization
delocalization problem.
Relevant to many systems, eg V2O3
range or problems.
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Mott transition in V2O3 under pressure
or chemical substitution on V-site
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Universal and non universal
features. Top to bottom approach
to correlated materials.
Some aspects at high temperatures,
depend weakly on the material (and on the
model).
Low temperature phase diagram, is very
sensitive to details, in experiment (and in
the theory).
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Mott transition in layered organic conductors S Lefebvre et
al. cond-mat/0004455, Phys. Rev. Lett. 85, 5420 (2000)
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Failure of the Standard Model:
NiSe2-xSx Miyasaka and
Takagi (2000)
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Phase Diagrams :V2O3, Ni Se2-x Sx Mc Whan
et. Al 1971,. Czek et. al. J. Mag. Mag. Mat. 3, 58 (1976),
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Outline
Introduction to the strong correlation problem
and to the Mott transition.
DMFT ideas
Applications to the Mott transition problem:
some insights from studies of models.
Towards an electronic structure method:
applications to materials: NiO, Pu, Fe, Ni,
LaSrTiO3, .
Outlook
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Hubbard model
(t
i , j ,
ij m ij )(c c j c ci ) U ni ni
i
j
i
U/t
Doping or chemical potential
Frustration (t/t)
T temperature
Mott transition as a function of doping, pressure
THE STATE UNIVERSITY OF NEW JERSEY
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Mean-Field : Classical vs Quantum
b b b
H MF = - heff So c ( t )[
os t + m- D (t - t ')]cos (t ') +U no no
0 0 0
heff D ( w)
m0 = S0 HMF ( heff )
G = cos (iwn )cos (iwn )SMF (D )
heff = j
J ij m j + h G (iwn ) =
k [D (iwn ) -
1
1
- ek ]
G (iwn )[D ]
G0 Impurity
Solver
S.C.C.
G
S.C.C.
Wide variety of computational tools
(QMC,ED.)Analytical Methods
Extension to ordered states, clusters..
Review: A. Georges, G. Kotliar, W. Krauth and M.
Rozenberg Rev. Mod. Phys. 68,13 (1996)]
THE STATE UNIVERSITY OF NEW JERSEY
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DMFT: Effective Action point of view.
R. Chitra and G. Kotliar Phys Rev. B.
(2000).
Identify observable, A. Construct an exact functional of
<A>=a, G [a] which is stationary at the physical value of a.
Example, density in DFT theory. (Fukuda et. al.)
When a is local, it gives an exact mapping onto a local
problem, defines a Weiss field.
The method is useful when practical and accurate
approximations to the exact functional exist. Example:
LDA, GGA, in DFT.
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Example: DMFT for lattice model (e.g.
single band Hubbard).Muller Hartman 89,
Chitra and Kotliar 99.
Observable: Local Greens function Gii ().
Exact functional G [Gii () ].
DMFT Approximation to the functional.
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Extensions of DMFT.
Renormalizing the quartic term in the local
impurity action.
EDMFT.
Taking several sites (clusters) as local
entity.
CDMFT
Combining DMFT with other methods.
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Outline
Introduction to the strong correlation
problem.
Essentials of DMFT
Applications to the Mott transition problem:
some insights from studies of models.
Towards an electronic structure method:
applications to materials
Outlook
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Schematic DMFT phase diagram Hubbard model
(partial frustration). Evidence for QP peak in V2O3
from optics.
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Schematic DMFT phase diagram one band
Hubbard model (half filling, semicircular
DOS, partial frustration) Rozenberg et.al PRL
(1995)
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Spectral Evolution at T=0 half filling full
frustration. Three peak structure.
X.Zhang M. Rozenberg G. Kotliar (PRL 1993)
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Evolution of the Spectral Function
with Temperature
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Insights from DMFT
Three peak structure of the density of
states.
In the strongly correlated metallic regime
the Hubbard bands are well formed.
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Insights from DMFT
The Mott transition is driven
by transfer of spectral weight
from low to high energy as we
approach the localized phase
Control parameters: doping,
temperature,pressure
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What about experiments?
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Parallel development: Fujimori et.al
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Mott transition in V2O3 under pressure
or chemical substitution on V-site
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Anomalous transfer of optical
spectral weight V2O3
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Anomalous transfer of spectral
weight in v2O3
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Anomalous Spectral Weight Transfer:
Optics
H hamiltonian, J electric current , P polarization
ne2
0 ( )d iV P, J ] m
Below energy H eff , J eff , Peff
ApreciableT dependence
0
( )d
iV
Peff , J eff
found.
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ARPES measurements on NiS2-xSex
.Matsuura et. al Phys. Rev B 58 (1998) 3690. Doniach and Watanabe Phys. Rev. B 57,
3829 (1998)
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Anomalous transfer of optical spectral
weight, NiSeS. [Miyasaka and Takagi
2000]
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Anomalous Resistivity and Mott
transition Ni Se2-x Sx
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Recent exps. Moo et. al. (2003)
Theory Held et. al.
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Transport in 2d organics. Limlet et. al.
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Strong correlation anomalies
Metals with resistivities which exceed the
Mott Ioffe Reggel limit.
Transfer of spectral weight which is non
local in frequency.
Dramatic failure of DFT based
approximations in predicting physical
properties.
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Conclusions: generic aspects
Three peak structure, quasiparticles and
Hubbard bands.
Non local transfer of spectral weight.
Large resistivities.
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Insights from DMFT
.
Important role of the incoherent part of the
spectral function at finite temperature
Physics is governed by the transfer of
spectral weight from the coherent to the
incoherent part of the spectra. Real and
momentum space pictures are needed as
synthesized in DMFT.
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Outline
Introduction to the strong correlation problem.
Essentials of DMFT
Applications to the Mott transition problem: some
insights from studies of models.
Towards an electronic structure method:
applications to materials: Pu, Fe, Ni, Ce, LaSrTiO3,
NiO,MnO,CrO2,K3C60,2d and quasi-1d organics,
magnetic semiconductors,SrRuO4,V2O3.
Outlook
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Interface DMFT with
electronic structure.
Derive model Hamiltonians, solve by DMFT
(or cluster extensions).
Full many body aproach, treat light electrons by
GW or screened HF, heavy electrons by DMFT .
Treat correlated electrons with DMFT and light
electrons with DFT (LDA, GGA +DMFT)
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DMFT: Effective Action point of view.
R. Chitra and G. Kotliar Phys Rev. B.
(2000).
Identify observable, A. Construct an exact functional of
<A>=a, G [a] which is stationary at the physical value of a.
Example, density in DFT theory. (Fukuda et. al.)
When a is local, it gives an exact mapping onto a local
problem, defines a Weiss field.
The method is useful when practical and accurate
approximations to the exact functional exist. Example:
LDA, GGA, in DFT.
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Spectral Density Functional : effective
action construction (Chitra and GK).
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Very Partial list of application of
realistic DMFT to materials
QP bands in ruthenides: A. Liebsch et al (PRL 2000)
N phase of Pu: Savrasov GK and Abrahams (Nature
2001)
Dai Savrasov GK Migliori Letbetter and Abrahams (Science
2003)
MIT in V2O3: K. Held et al (PRL 2001)
Magnetism of Fe, Ni: A. Lichtenstein et al PRL (2001)
J-G transition in Ce: K. Held et al (PRL 2000); M. Zolfl
et al PRL (2000).
3d doped Mott insulator La1-xSrxTiO3 (Anisimov et.al
1997, Nekrasov et.al. 1999, Udovenko et.al 2003)
Paramagnetic Mott insulators. NiO MnO, Savrasov and
THE STATE UNIVERSITY OF NEW JERSEY
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Physics of Pu
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Plutonium Puzzles
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DFT Studies
LSDA predicts magnetic long range (Solovyev
et.al.)
Experimentally Pu is not magnetic.
If one treats the f electrons as part of the core
LDA overestimates the volume by 30%
DFT in GGA predicts correctly the volume of the
a phase of Pu, when full potential LMTO
(Soderlind Eriksson and Wills) is used. This is
usually taken as an indication that a Pu is a
weakly correlated system
Alternative approach Wills et. al. (5f)4 core+
1f(5f)in conduction band.
THE STATE UNIVERSITY OF NEW JERSEY
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Shear anisotropy fcc Pu (GPa)
C=(C11-C12)/2 = 4.78
C44= 33.59
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Pu: DMFT total energy vs Volume
(Savrasov Kotliar and Abrahams 2001)
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Phonon freq (THz) vs q in delta Pu X.
Dai et. al. Science vol 300, 953, 2003
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Functional approach allows
computation of linear
response.(S. Savrasov and GK
2002)
Apply to NiO, canonical Mott insulator.
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Results for NiO: Phonons (Savrasov and Kotliar
PRL 2002)
Solid circles theory, open circles exp. (Roy et.al, 1976)
DMFT
Phases of Pu
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Dai et. al.
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Epsilon Plutonium.
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Outline
Introduction to the strong correlation
problem.
Essentials of DMFT
Applications to the Mott transition problem:
some insights from studies of models.
Towards an electronic structure method:
applications to materials:
Outlook
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Outlook
Local approach to strongly correlated
electrons.
Many extensions, make the approach
suitable for getting insights and quantitative
results in correlated materials.
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Conclusion
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Outlook
Systematic improvements, short range
correlations, cluster methods, improved
mean fields.
Improved interfaces with electronic
structure.
Exploration of complex strongly correlated
materials. Correlation effects on surfaces,
large molecules, systems out of equilibrium,
illumination, finite currents, aeging.
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Acknowledgements: Development of DMFT
Collaborators: V. Anisimov,G. Biroli, R. Chitra, V.
Dobrosavlevic, X. Dai, D. Fisher, A. Georges, H.
Kajueter, K. Haujle, W.Krauth, E. Lange, A. Lichtenstein,
G. Moeller, Y. Motome, O. Parcollet , G. Palsson, M.
Rozenberg, S. Savrasov, Q. Si, V. Udovenko, I. Yang,
X.Y. Zhang
Support: NSF DMR 0096462
Support: Instrumentation. NSF DMR-0116068
Work on Fe and Ni: ONR4-2650
Work on Pu: DOE DE-FG02-99ER45761 and
LANL subcontract No. 03737-001-02
THE STATE UNIVERSITY OF NEW JERSEY
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THE STATE UNIVERSITY OF NEW JERSEY
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THE STATE UNIVERSITY OF NEW JERSEY
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Expts Wong et. al.
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THE STATE UNIVERSITY OF NEW JERSEY
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THE STATE UNIVERSITY OF NEW JERSEY
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E-DMFT references
H. Kajueter and G. Kotliar (unpublished and
Kajuters Ph.D thesis (1995)).
Q. Si and J L Smith PRL 77 (1996)3391 .
R. Chitra and G.Kotliar Phys. Rev. Lett 84, 3678-
3681 (2000 )
Y. Motome and G. Kotliar. PRB 62, 12800 (2000)
R. Chitra and G. Kotliar Phys. Rev. B 63, 115110
(2001)
S. Pankov and G. Kotliar PRB 66, 045117 (2002)
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DMFT Impurity cavity construction
i , j ,
(tij m ij )(ci c j c j ci ) U ni ni
i
Vij ni n j
b b i , j
- 1
1
D0- 1
(iwn ) =
k
Vk - P (iwn )
+ P (iwn )
S (iwn )[G0 ] = G0- 1 (iwn ) + [ca (iwn )cb (iwn )S (G0 ) ]- 1
- 1
1
G0 (iwn ) =
- 1
k
iwn - tk + m- S (iwn )
+ S (iwn )
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Cluster extensions of DMFT
Two impurity method. [A. Georges and G. Kotliar
(1995 unpublished ) and RMP 68,13 (1996) , A.
Schiller PRL75, 113 (1995)]
M. Jarrell et al Dynamical Cluster Approximation
[Phys. Rev. B 7475 1998]
Periodic cluster] M. Katsenelson and A.
Lichtenstein PRB 62, 9283 (2000).
G. Kotliar S. Savrasov G. Palsson and G. Biroli
Cellular DMFT [PRL87, 186401 2001]
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C-DMFT G0
G0ac b tij
tija b S
S c
ab
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C-DMFT: test in one dimension.
(Bolech, Kancharla GK cond-mat 2002)
Gap vs U, Exact solution
Lieb and Wu,
Ovshinikov
Nc=2 CDMFT
vs Nc=1
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DMFT plus other methods.
DMFT+ LDA , V. Anisimov, A. Poteryaev, M. Korotin, A.
Anokhin and G. Kotliar, J. Phys. Cond. Mat. 35, 7359-7367
(1997).
A Lichtenstein and M. Katsenelson Phys. Rev. B 57, 6884
(1988).
S. Savrasov and G.Kotliar, funcional formulation for full self
consistent implementation. Savasov Kotliar and Abrahams .
Application to delta Pu Nature (2001)
Combining EDMFT with GW. Ping Sun and Phys. Rev. B 66,
085120 (2002). G. Kotliar and S. Savrasov in New
Theoretical Approaches to Strongly Correlated Systems,
A. M. Tsvelik Ed. 2001 Kluwer Academic Publishers. 259-
301 . cond-mat/0208241
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ARPES measurements on NiS2-xSex
.Matsuura et. Al Phys. Rev B 58 (1998) 3690. Doniaach and Watanabe Phys. Rev. B 57,
3829 (1998)
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LDA+DMFT Self-Consistency loop
c ka | 2 + Vxc (r ) | c k a = H LMTO ( k ) E
Impurity
G0 Solver G
S.C.C.
U
DMFT
r (r) = T
iw
G( r, r, iw)e iw 0+
nHH = T iw
+
GHH (r , r , iw)eiw 0
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QP in V2O3 was recently
found Mo et.al
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Ni and Fe: theory vs exp
m( T=.9 Tc)/ mB ordered moment
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LDA+DMFT Self-Consistency loop
c ka | 2 + Vxc (r ) | c k a = H LMTO ( k ) E
Impurity
G0 Solver G
S.C.C.
U
DMFT
r (r) = T
iw
G( r, r, iw)e iw 0+
nHH = T iw
+
GHH (r , r , iw)eiw 0
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LDA+DMFT functional
G LDA DMFT [ r (r ) G a b VKS(r )ab]
Tr log[iwn + 2 / 2 VKS c * a R ( r )S a b c b R ( r )]
VKS ( r )r ( r ) dr - iwn
TrS (iwn )G (iwn ) +
1 r ( r )r ( r ')
LDA
Vext ( r )r ( r ) dr + drdr '+ E xc [r ] +
2 | r- r '|
R
F [G ] - F DC
F DC [G ] = Un(n - 1)
2
n= T ab (iw)e
i0
)
abiw
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Anomalous Spectral Weight Transfer:
Optics
H hamiltonian, J electric current , P polarization
ne2
0 ( )d iV P, J ] m
Below energy H eff , J eff , Peff
AppreciableT dependence
0
( )d
iV
Peff , J eff
found.
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Comments on LDA+DMFT
Static limit of the LDA+DMFT functional ,
with F= FHF reduces to LDA+U
Removes inconsistencies of this
approach,
Only in the orbitally ordered Hartree Fock
limit, the Greens function of the heavy
electrons is fully coherent
Gives the local spectra and the total
energy simultaneously, treating QP and H
bands on the same footing.
THE STATE UNIVERSITY OF NEW JERSEY
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LSDA+DMFT functional
G LDA DMFT [ r (r ) m (r ) G a b VKS(r ) BKS(r ) ab]
Tr log[iwn + 2 / 2 VKS c *a R (r )S a bc b R (r )]
VKS (r )r (r )dr - B KS
(r )m(r )dr - iwn
TrS (iwn )G (iwn ) +
1 r (r )r (r ')
Vext (r )r (r )dr +
2 | r- r'|
drdr '+ ExcLDA [r ] +
R
F [G ] - F DC
F DC [G ] = Un(n - 1)
2
n= T ab (iw)e
i0
)
abiw
RUTGERS
DMFT: Effective Action point of view.
R. Chitra and G. Kotliar Phys Rev. B.
(2000).
Identify observable, A. Construct an exact functional of
<A>=a, G [a] which is stationary at the physical value of a.
Example, density in DFT theory. (Fukuda et. al.)
When a is local, it gives an exact mapping onto a local
problem, defines a Weiss field.
The method is useful when practical and accurate
approximations to the exact functional exist. Example:
LDA, GGA, in DFT.
It is useful to introduce a Lagrange multiplier l conjugate
to a, G [a, l ].
It gives as a byproduct a additional lattice information.
RUTGERS
Solving the DMFT equations
G Impurity
0 Solver G
G0 Impurity
Solver
S.C.C.
G
S.C.C.
Wide variety of computational tools
(QMC,ED.)Analytical Methods
Extension to ordered states.
Review: A. Georges, G. Kotliar, W. Krauth and M.
Rozenberg Rev. Mod. Phys. 68,13 (1996)]
THE STATE UNIVERSITY OF NEW JERSEY
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LDA+DMFT Self-Consistency loop
Impurity
G0 Solver G
U
S.C.C.
DMFT
r (r) = T
iw
G( r, r, iw)e iw 0+
nHH = T iw
+
GHH (r , r , iw)eiw 0
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