urbana-champaign, 2008 band structure of strongly correlated materials from the dynamical mean field...
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Urbana-Champaign, 2008
Band structure of strongly correlated materials from the Dynamical Mean Field perspective
K HauleRutgers University
Collaborators : J.H. Shim & Gabriel Kotliar
Outline
Dynamical Mean Field Theory in combination with band structure
LDA+DMFT results for 115 materials (CeIrIn5) Local Ce 4f - spectra and comparison to AIPES) Momentum resolved spectra and comparison to ARPES Optical conductivity Two hybridization gaps and its connection to optics Fermi surface in DMFT Iron based superconductors and DMFT predictions
References:•J.H. Shim, KH, and G. Kotliar, Science 318, 1618 (2007).•J.H. Shim, KH, and G. Kotliar, Nature 446, 513 (2007).•KH, J.H. Shim, and G. Kotliar, cond-mat/arXiv:0803.1279.
Standard theory of solidsStandard theory of solids
Band Theory: electrons as waves: Rigid band picture: En(k) versus k
Landau Fermi Liquid Theory applicable
Very powerful quantitative tools: LDA,LSDA,GWVery powerful quantitative tools: LDA,LSDA,GW
Predictions:
•total energies,
•stability of crystal phases
•optical transitions
M. Van SchilfgardeM. Van Schilfgarde
Fermi Liquid Theory does NOT work . Need new concepts to replace rigid bands picture!
Breakdown of the wave picture. Need to incorporate a real space perspective (Mott).
Non perturbative problem.
Strong correlation – Strong correlation –
Standard theory failsStandard theory fails
Bright future!Bright future!
New concepts, new techniques…..
DMFT maybe the simplest approach to describe the physics of strong correlations -> the spectral weight transfer
1B HB model 1B HB model (DMFT):(DMFT):DMFT can describe Mott transition:
V2O3Ni2-xSex organics
Universality of the Mott transitionUniversality of the Mott transition
First order MITCritical point
Crossover: bad insulator to bad metal
1B HB model 1B HB model (DMFT):(DMFT): B
ad in
sula
tor
Bad metal1B HB model 1B HB model (plaquette):(plaquette):
DMFT + electronic structure methodDMFT + electronic structure method
(G. Kotliar S. Savrasov K.H., V. Oudovenko O. Parcollet and C. Marianetti, RMP 2006).
Basic idea of DMFT+electronic structure method (LDA or GW): For less correlated bands (s,p): use LDA or GWFor correlated bands (f or d): add all local diagrams by solving QIM
DMFT is not a single impurity calculation
Auxiliary impurity problem:
High-temperature given mostly by LDA
low T: Impurity hybridization affected by the emerging coherence of the lattice
(collective phenomena)
Weiss field temperature dependent:
Feedback effect on makes the crossover from incoherent to coherent state very slow!
high T
low T
DMFT SCC:
General impurity problem
Diagrammatic expansion in terms of hybridization +Metropolis sampling over the diagrams
•Exact method: samples all diagrams!•Allows correct treatment of multiplets
K.H. Phys. Rev. B 75, 155113 (2007)
An exact impurity solver, continuous time QMC - expansion in terms of hybridization
NCA
OCA
SUNCA
Luttinger Ward functional
every atomic state represented with a unique pseudoparticle
atomic eigenbase - full (atomic) base
, where
general AIM:
Same expansion using diagrammatics – real axis solver
( )
Basic questions to addressBasic questions to address
How to computed spectroscopic quantities (single particle spectra, optical conductivity phonon dispersion…) from first principles?
How to relate various experiments into a unifying picture.
DMFT maybe simplest approach to meet this challenge for correlated materials
Ce
In
Ir
CeIn
In
Crystal structure of 115’s
CeIn3 layer
IrIn2 layer
IrIn2 layer
Tetragonal crystal structure
4 in plane In neighbors
8 out of plane in neighbors
3.27au
3.3 au
Crossover scale ~50K
in-plane
out of plane
•Low temperature – Itinerant heavy bands
•High temperature Ce-4f local moments
ALM in DMFTSchweitzer&Czycholl,1991
Coherence crossover in experiment
•How does the crossover from localized moments to itinerant q.p. happen?
•How does the spectral
weight redistribute?
•How does the hybridization gap look like in momentum space?
?
k
A()
•Where in momentum space q.p. appear?
•What is the momentum dispersion of q.p.?
Issues for the system specific study
Temperature dependence of the local Ce-4f spectra
•At low T, very narrow q.p. peak (width ~3meV)
•SO coupling splits q.p.: +-0.28eV
•Redistribution of weight up to very high frequency
SO
•At 300K, only Hubbard bands
J. H. Shim, KH, and G. Kotliar Science 318, 1618 (2007).
Very slow crossover!
T*
Slow crossover pointed out by NPF 2004
Buildup of coherence in single impurity case
TK
cohere
nt
spect
ral
weig
ht
T scattering rate
coherence peak
Buildup of coherence
Crossover around 50K
Remarkable agreement with Y. Yang & D. Pines Phys. Rev. Lett. 100, 096404 (2008).
Anom
alo
us
Hall
coeffi
cient
Fraction of itinerant heavy fluid
m* of the heavy fluid
Consistency with the phenomenological approach of NPF
ARPESFujimori, 2006
Angle integrated photoemission vs DMFT
Experimental resolution ~30meV, theory predicts 3meV broad band
Surface sensitive at 122eV
Angle integrated photoemission vs DMFT
ARPESFujimori, 2006
Nice agreement for the• Hubbard band position•SO split qp peak
Hard to see narrow resonance
in ARPES since very little weight
of q.p. is below Ef
Lower Hubbard band
T=10K T=300Kscattering rate~100meV
Fingerprint of spd’s due to hybridization
Not much weight
q.p. bandSO
Momentum resolved Ce-4f spectraAf(,k)
Hybridization gap
Momentum resolved total spectra A(,k)
Fujimori, 2003
LDA+DMFT at 10K ARPES, HE I, 15K
LDA f-bands [-0.5eV, 0.8eV] almostdisappear, only In-p bands remain
Most of weight transferred intothe UHB
Very heavy qp at Ef,hard to see in total spectra
Below -0.5eV: almost rigid downshift
Unlike in LDA+U, no new band at -2.5eV
Large lifetime of HBs -> similar to LDA(f-core)rather than LDA or LDA+U
Optical conductivity
Typical heavy fermion at low T:
Narrow Drude peak (narrow q.p. band)
Hybridization gap
k
Interband transitions across hybridization gap -> mid IR peak
CeCoIn5
no visible Drude peak
no sharp hybridization gap
F.P. Mena & D.Van der Marel, 2005
E.J. Singley & D.N Basov, 2002
second mid IR peakat 600 cm-1
first mid-IR peakat 250 cm-1
•At 300K very broad Drude peak (e-e scattering, spd lifetime~0.1eV) •At 10K:
•very narrow Drude peak•First MI peak at 0.03eV~250cm-1
•Second MI peak at 0.07eV~600cm-1
Optical conductivity in LDA+DMFT
CeIn
In
Multiple hybridization gaps
300K
e V
10K
•Larger gap due to hybridization with out of plane In•Smaller gap due to hybridization with in-plane In
non-f spectra
Fermi surfaces of CeM In5 within LDA
Localized 4f:LaRhIn5, CeRhIn5
Shishido et al. (2002)
Itinerant 4f :CeCoIn5, CeIrIn5
Haga et al. (2001)
T decreasing
How does the Fermi surface change with temperature?
Electron fermi surfaces at (z=0)
LDA+DMFT (10 K)LDA LDA+DMFT (400 K)
X M
X
XX
M
MM
2 2
Slight increase of the
electron FS with decr T
R A
R
RR
A
AA
3
a
3
LDA+DMFT (10 K)LDA LDA+DMFT (400 K)
Electron fermi surfaces at (z=)No a in DMFT!No a in Experiment!
Slight increase of the
electron FS with decr T
LDA+DMFT (10 K)LDA LDA+DMFT (400 K)
X M
X
XX
M
MM
c
2 2
11
Electron fermi surfaces at (z=0)Slight increase of the electron FS
with decr T
R A
R
RR
A
AA
c
2 2
LDA+DMFT (10 K)LDA LDA+DMFT (400 K)
Electron fermi surfaces at (z=)No c in DMFT!No c in Experiment!
Slight increase of the electron FS
with decr T
LDA+DMFT (10 K)LDA LDA+DMFT (400 K)
X M
X
XX
M
MM
g h
Hole fermi surfaces at z=0
g h
Big change-> from small hole like to large electron like
1
LaOFeP 3.2K, JACS-2006
a=3.964A, c=8.512A
PrFxO1-xFeAs d) 52K, unpublished
a=3.985A, c=8.595A
SmFxO1-xFeAs c) 43K, cm/0803.3603
a=3.940A, c=8.496A
CeFxO1-xFeAs b) 41 K, cm/0803.3790
a=3.996A, c=8.648A
LaFxO1-xFeAs a) 26 K, JACS-2008
a=4.036A, c=8.739 A
La1-xSrxOFeAs 25K, cm/0803.3021,
a=4.035A, c = 8.771A
LaCaxO1+xFeAs 0 K
LaFxO1-xNiAs 2.75K, cm/0803.2572a=4.119A , c=8.180A
La1-xSrxONiAs 3.7K, cm/0803.3978
a=4.045A, c=8.747A
x~5-20%
Fe,Ni
As,P
La,Sm,Ce
O
•2D square lattice of Fe•Fe - magnetic moment•As-plays the role of O in cuprates
Sm
aller
cH
igh
er
Tc
Iron based high-Tc superconductors
a) Y. Kamihara et.al., Tokyo, JACSb) X.H. Chen, et.al., Beijing, cm/0803.3790c) G.F. Chen et.al., Beijing, cm/0803.3603d) Z.A. Ren et.al, Beijing, unpublished
Y. Kamihara et.al., J. Am. Chem. Soc. XXXX, XXX (2008)
A.S. Sefat. et.al., cond-mat/0803.2403
Specific heat consistent with nodes! Possibly d wave..
Kink in resistivitymaybe SDW
LaFxO1-xFeAs
Y. Kamihara, J. Am. Chem. Soc. XXXX, XXX (2008)
Undoped compound:•Huge resistivity
Doped compound:•Large resistivity >> opt. dop. Cuprates
•Huge spin susceptibility( >> 100 bigger than in
LSCO50 x Pauli)
•Spin susceptibility of an almost free spins
~C/(T+120K) with C of S~1
Wilson’s ratioR~1 F0
a small
LaFxO1-xFeAs
LDA: phonons-Tc<1K
KH, J.H. Shim, G. Kotliar, cond/mat 0803.1279
LDA: Mostly iron bands at EF (correlations important)
LDA DOS
6 electrons in 5 Fe bands:Filling 6/10
LDA for LaOFeAs
x2-y2
yz, xz
z2
xy 60meV
160meV
60meV
LDA+DMFT: LaOFeAs is at the verge of the metal-insulator transition (for realistic U=4eV, J=0.7eV)For a larger (U=4.5, J=0.7eV) Slater insulator
Not a one band model: all 5 bands important (for J>0.3)
DMFT for LaFxO1-xFeAs
Need to create a singlet out of spin and orbit
In LaOFeAs semiconducting gap is openingLarge scattering rate at 116K
Optical conductivity of a bad metal
No Drude peak
Electron pockets around M and A upon doping
DMFT for LaFxO1-xFeAs
T=116 K
10% doping
DMFT can describe crossover from local moment regime to heavy fermion state in heavy fermions. The crossover is very slow.
Width of heavy quasiparticle bands is predicted to be only ~3meV. We predict a set of three heavy bands with their dispersion.
Mid-IR peak of the optical conductivity in 115’s is split due to presence of two type’s of hybridization
Ce moment is more coupled to out-of-plane In then in-plane In which explains the sensitivity of 115’s to substitution
of transition metal ion
Fermi surface in CeIrIn5 is gradually increasing with decreasing temperature but it is not saturated even at 5K.
LaOFeAs is very bad metal within LDA+DMFT. With doping it becomes Fermi liquid with coherence temperature ~100K.
ConclusionsConclusions
Electrical resistivity & specific heat
J. C. Lashley et al. PRB 72 054416 (2005)
Heavy ferm. in an element
closed shell Am
Itinerant
Curium versus Plutonium
nf=6 -> J=0 closed shell
(j-j: 6 e- in 5/2 shell)(LS: L=3,S=3,J=0)
One hole in the f shell One more electron in the f shell
No magnetic moments,large massLarge specific heat, Many phases, small or large volume
Magnetic moments! (Curie-Weiss law at high T, Orders antiferromagnetically at low T) Small effective mass (small specific heat coefficient)Large volume
Standard theory of solids:DFT:
All Cm, Am, Pu are magnetic in LSDA/GGA LDA: Pu(m~5), Am (m~6) Cm (m~4)
Exp: Pu (m=0), Am (m=0) Cm (m~7.9)Non magnetic LDA/GGA predicts volume up to 30% off.In atomic limit, Am non-magnetic, but Pu magnetic with spin ~5B
Can LDA+DMFT account for anomalous properties of actinides?
Can it predict which material is magnetic and which is not?
Many proposals to explain why Pu is non magnetic: Mixed level model (O. Eriksson, A.V. Balatsky, and J.M. Wills) (5f)4 conf. +1itt. LDA+U, LDA+U+FLEX (Shick, Anisimov, Purovskii) (5f)6 conf.
Cannot account for anomalous transport and thermodynamics
-Plutonium
0
1
2
3
4
-6 -4 -2 0 2 4 6
DO
S (
stat
es/e
V)
Total DOS
f DOS
Curium
0
1
2
3
4
-6 -4 -2 0 2 4 6ENERGY (eV)
DO
S (
stat
es/e
V)
Total DOS f, J=5/2,jz>0f, J=5/2,jz<0 f, J=7/2,jz>0f, J=7/2,jz<0
Starting from magnetic solution, Curium develops antiferromagnetic long range order below Tc above Tc has large moment (~7.9 close to LS coupling)Plutonium dynamically restores symmetry -> becomes paramagnetic
J.H. Shim, K.H., G. Kotliar, Nature 446, 513 (2007).
-Plutonium
0
1
2
3
4
-6 -4 -2 0 2 4 6
DO
S (
stat
es/e
V)
Total DOS
f DOS
Curium
0
1
2
3
4
-6 -4 -2 0 2 4 6ENERGY (eV)
DO
S (
stat
es/e
V)
Total DOS f, J=5/2,jz>0f, J=5/2,jz<0 f, J=7/2,jz>0f, J=7/2,jz<0
Multiplet structure crucial for correct Tk in Pu (~800K)and reasonable Tc in Cm (~100K)
Without F2,F4,F6: Curium comes out paramagnetic heavy fermion Plutonium weakly correlated metal
Magnetization of Cm:
Photoemission and valence in Pu
|ground state > = |a f5(spd)3>+ |b f6 (spd)2>
f5<->f6
f5->f4
f6->f7
Af(
)
approximate decomposition
Curium
0.0
0.3
0.6
0.9
-6 -4 -2 0 2 4 6ENERGY (eV)
Pro
bab
ility
N =8
N =7
N =6
J=7/
2,g =
0
J=5,
g =0
J=6,
g =0
J=4,
g =0
J=3,
g =0
J=2,
g =0
J=5,
g =0
J=2,
g =0
J=1,
g =0
J=0,
g =0
J=6,
g =0
J=4,
g =0
J=3,
g =0
f
f
f
-Plutonium
0.0
0.3
0.6
Pro
bab
ility
N =6
N =5
N =4
JJ=
0,g =
0J=
1,g =
0J=
2,g =
0J=
3,g =
0J=
4,g =
0J=
5,g =
0
J=6,
g =1
J=4,
g =0
J=5,
g =0
J=2,
g =0
J=1,
g =0
J=2,
g =1
J=3,
g =1
J=5/
2, g
=0
J=7/
2,g =
0J=
9/2,
g =0
f
f
f
Valence histograms
Density matrix projected to the atomic eigenstates of the f-shell(Probability for atomic configurations)
f electron fluctuates
between theseatomic states on the time scale t~h/Tk
(femtoseconds)
One dominant atomic state – ground state of the atom
Pu partly f5 partly f6
Probabilities:
•5 electrons 80%
•6 electrons 20%
•4 electrons <1%
J.H. Shim, K. Haule, G. Kotliar, Nature 446, 513 (2007).
Gradual decrease of electron FS
Most of FS parts show similar trend
Big change might be expected in the plane – small hole like FS pockets (g,h) merge into electron FS 1 (present in LDA-f-core but not in LDA)
Fermi surface a and c do not appear in DMFT results
Increasing temperature from 10K to 300K:
Fermi surfacesFermi surfaces
SUNCA vs QMCtwo band Hubbard model, Bethe lattice, U=4D
three band Hubbard model,
Bethe lattice, U=5D, T=0.0625D
three band Hubbard model,
Bethe lattice, U=5D, T=0.0625D
CeIn3 CeCoIn5 CeRhIn5 CeIrIn5 PuCoG5 Na
Tc[K] 0.2K 2.3K 2.1K 0.4K 18.3K n/a
Tcrossover ~50K ~50K ~50K ~370K
Cv/T[mJ/molK^2] 1000 300 400 750 100 1
Phase diagram of CeIn3 and 115’s
N.D. Mathur et al., Nature (1998)
CeIn3
0
1
2
3
4
?SC
SCSC
X
0.50.50.5 IrRh CoCo
AFM
T* (
K)
CeCoIn5 CeRhIn5CeIrIn5 CeCoIn5
CeXIn5
layering
Tcrossover α Tc
LDA+U corresponds to LDA+DMFT when impurity is solved in the Hartree Fock approximation
observable of interestobservable of interest is the "local“is the "local“ Green's functionsGreen's functions (spectral (spectral function)function)
Currently feasible approximations: LDA+DMFT and GW+DMFT:
S. Y. Savrasov et al.,PRB 69, 245101 (2004)
Spectral density functional theory
basic idea: sum-up all local diagrams for electrons in correlated orbitals
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