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### Towards First-Principles Electronic Structure Calculations of Correlated Materials Using Dynamical Mean Field Theory (DMFT).

### Outline , of Correlated Materials Using Dynamical Mean Field Theory (DMFT).Collaborators, References

Gabriel Kotliar

Physics Department and

Center for Materials Theory

Rutgers University

CMSN-Workshop on Predictive Capabilities for Strongly Correlated Systems

UT November 7-9 2003

A. Poteryaev, A. Lichtenstein and G. Kotliar (preprint) (2003)

S.Savrasov G. Kotliar and E. Abrahams, Nature 410,793 (2001).

X. Dai,S. Savrasov, G. Kotliar,A. Migliori, H. Ledbetter, E. Abrahams Science, Vol300, 954 (2003)

Funding: Basic Energy Sciences DOE..

DMFT and electronic structure calculations

Case study 1: Ti2O3

Case study 2: Elemental Pu

Conclusions: Future developments.

Two limits of the electronic structure problem are well under control.

Band limit, (LDA or GGA)+ GW, gives good spectra and total energy. Physical properties are accessible in perturbation theory in the screened Coulomb interactions

Well separated atoms, in the presence of spin orbital long range order, expansion around the atomic limit, unrestricted HF, and LDA+U work well for ordered Mott insulators.

Challenge ahead: materials that are not in either one of these regimes. Requires combination of many body theory and one electron theory.

Strongly Correlated ElectronsTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Strongly correlated systems are usually treated with model Hamiltonians

- Conceptually one wants to restrict the number of degrees of freedom by eliminating high energy degrees of freedom.
- In practice other methods (eg constrained LDA are used)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Reduce the quantum many body problem to a one site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Instead of using functionals of the density, use more sensitive functionals of the one electron spectral function. [density of states for adding or removing particles in a solid, measured in photoemission]

Dynamical Mean Field TheoryTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

DMFT cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

A. Georges, G. Kotliar (1992)

Phys. Rev. B 45, 6497

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

DMFT action and self consistency condition cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

In general tk is large matrix H[k] , U is a matrix

In the case of cluster is a matrix and is not the self energy, (but can be used to estimate the lattice self energy by projection)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Solving the DMFT equations cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

- Review: A. Georges, G. Kotliar, W. Krauth and M. Rozenberg Rev. Mod. Phys. 68,13 (1996)]

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

DMFT: Effective Action point of view.R. Chitra and G. K Phys Rev. B.62 12715(2000), 63 115110(2001) S Savrasov and G. K. cond-matt 0308053

- 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.
- DMFT, build functionals of the LOCAL spectral function.
- Exact functionals exist. We also have good approximations!
- Extension to an ab initio method. Functional of greens function of electric field and electronic field, functional of the density and the local greens function.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Observable: Local Greens function G Rev. B.62 12715(2000), 63 115110(2001) S Savrasov and G. K. cond-matt 0308053ii (w).

Exact functional G [Gii (w) ].

DMFT Approximation to the functional.(Muller Hartman 89)

DMFT as an approximation to the exact functional of the Greens function, DMFT as a truncation of the BK functional of the full Greens function.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

LDA+DMFT (II) Rev. B.62 12715(2000), 63 115110(2001) S Savrasov and G. K. cond-matt 0308053

Edc

U

DMFT

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

C-DMFT: test in one dimension. Rev. B.62 12715(2000), 63 115110(2001) S Savrasov and G. K. cond-matt 0308053(Bolech, Kancharla GK cond-mat 2002)

Gap vs U, Exact solution Lieb and Wu, Ovshinikov

Nc=2 CDMFT

vs Nc=1

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

1d Hubbard U/t=4 exact diag 2+6.Capone Civelli and GK Rev. B.62 12715(2000), 63 115110(2001) S Savrasov and G. K. cond-matt 0308053

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Two roads for ab-initio calculation of electronic structure of strongly correlated materials

Crystal structure +Atomic positions

Model Hamiltonian

Correlation Functions Total Energies etc.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

ROAD 1: Derive model Hamiltonians, solve by DMFT of strongly correlated materials

(or cluster extensions).

V.Anisimov A Poteryaev V.Korotin V.Anokin andG Kotliar J. Phys. Cond. Mat. 35, 7359 (1997).A.Lichtenstein and M Katsnelson PRB (1998).

ROAD 2: Define a functional of the density and of the local Greens function and extremize the functional to get coupled equations for the density and the spectral function and compute total energies.

G. Kotliar, S.Savrasov, in New Theoretical approaches to strongly correlated systems, Edited by A. Tsvelik, Kluwer Publishers, (2001).

Interfacing DMFT with band theoryTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

The light, SP (or SPD) electrons are extended, well described by LDA. The heavy, D (or F) electrons are localized,treat by DMFT.

LDA already contains an average interaction of the heavy electrons, substract this out by shifting the heavy level (double counting term) . This defines H. The U matrix can be estimated from first principles (Gunnarson and Anisimov, McMahan et.al. Hybertsen et.al) of viewed as parameters.

Anisimov Poteryaev Korotin Anhokin and Kotliar J. Phys. Cond. Mat. 35, 7359 (1997).

LDA+DMFT (I)THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Application to Ti2O3 described by LDA. The heavy, D (or F) electrons are localized,treat by DMFT.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Isostructural to V2O3. All the qualitative physics of the high temperature part of the phase diagram of V2O3 can be understood within single site DMFT. Computations with a realistic density of states, and multiorbital impurity model (K. Held and D. Vollhardt ) substantial quantiative improvement.

Is the same thing true in Ti2O3?

Metal to insulator transition in Ti2O3THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Ti2O3 V2O3 : Resistivities high temperature part of the phase diagram of V2O3 can be understood within single site DMFT. Computations with a realistic density of states, and multiorbital impurity model (K. Held and D. Vollhardt ) substantial quantiative improvement.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Ti2O3 Structure high temperature part of the phase diagram of V2O3 can be understood within single site DMFT. Computations with a realistic density of states, and multiorbital impurity model (K. Held and D. Vollhardt ) substantial quantiative improvement.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Relevant Orbitals: Goodenough picture high temperature part of the phase diagram of V2O3 can be understood within single site DMFT. Computations with a realistic density of states, and multiorbital impurity model (K. Held and D. Vollhardt ) substantial quantiative improvement.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

As a function of temperature, there is no magnetic transition in Ti2O3, unlike V2O3

As a function of temperature, there is no structural change, unlike V2O3 which becomes monoclinic at low temperatures.

In V2O3 the distance between the Vanadium pairs incrases as the temperature decreases. In Ti2O3 the distance between the Vanadium pairs decreases as one lowers the temperature.

LTS 250 K, HTS 750 K.

Ti2O3 vs V2O3THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Band Structure Calculations always produce a good metal. L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

Unrestricted Hartree Fock calculations produce large antiferromagnetic gap. M. Cati, G. Sandrone, and R. Dovesi, Phys. Rev. B. f55 , 16122 (1997).

Earlier work.THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Ti2O3 LDA-DOS L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

HTS

LTS

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Impurity solver. Multiband QMC. L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

Derivation of the effective Hamiltonian. Massive downfolding with O Andersen’s new Nth order LMTOS. Coulomb interactions estimated using dielectric constant W=.5 ev. U on titanium 2 ev. J= .2 ev.

Methodology:1 and 2 site CDMFTTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Single site DMFT fails. LTS L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Two-site CDMFT for beta=20, and beta=10 L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

(T=500,1000)

Poteryaev Lichtenstein and GK

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Important role played by the Coulomb nn repulsion. L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

THE STATE UNIVERSITY OF NEW JERSEY

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Application to Plutonium L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

THE STATE UNIVERSITY OF NEW JERSEY

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Small amounts of Ga stabilize the L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)d phase (A. Lawson LANL)

THE STATE UNIVERSITY OF NEW JERSEY

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Elastic Deformations L.F. Mattheiss, J. Phys.: Condens. Matter 8, 5987 (1996)

Uniform compression:Dp=-B DV/V

Volume conserving deformations:

F/A=c44Dx/L

F/A=c’ Dx/L

In most cubic materials the shear does not depend strongly on crystal orientation,fcc Al, c44/c’=1.2, in Pu C44/C’ ~ 7largest shear anisotropy of any element.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

DFT in the LDA or GGA is a well established tool for the calculation of ground state properties.

Many studies (Freeman, Koelling 1972)APW methods

ASA and FP-LMTO Soderlind et. Al 1990, Kollar et.al 1997, Boettger et.al 1998, Wills et.al. 1999) give

an equilibrium volume of the d phaseIs 30-35% lower than experiment

This is the largest discrepancy ever known in DFT based calculations.

DFT studiesTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

LSDA predicts magnetic long range (Solovyev et.al.) calculation of ground state properties.

Experimentally d 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

DFT StudiesTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Lda vs Exp Spectra calculation of ground state properties.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Energy vs Volume [GGA+U=4 ev] calculation of ground state properties.

EXPT:

Bcc 14.7

Fcc 15.01

THE STATE UNIVERSITY OF NEW JERSEY

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Predicts plutonium to be magnetic. calculation of ground state properties.

Different theories of alpha and delta.

Other problems with LDA+UTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Atomic sphere approximation. calculation of ground state properties.

Ignore crystal field splittings in the self energies.

Fully relativistic non perturbative treatment of the spin orbit interactions.

Impurity solver: interpolative scheme using slave bosons (low frequency ) and eqn of motion (high frequency).

DMFT - Technical details [spectra and energy]THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Full potential LMTO with two kappas. calculation of ground state properties.

Linear response method in LMTO’s (S. Savrasov)

Impurity solver: lowest order projection (Roth method) in the equations of motion.

DMFT- Phonon SpectraTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Pu: DMFT total energy vs Volume ( calculation of ground state properties.Savrasov Kotliar and Abrahams 2001)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Pu Spectra DMFT(Savrasov) EXP ( calculation of ground state properties.Arko Joyce Morales Wills Jashley PRB 62, 1773 (2000)

THE STATE UNIVERSITY OF NEW JERSEY

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Alpha and delta Pu calculation of ground state properties.

THE STATE UNIVERSITY OF NEW JERSEY

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Alpha phase is also a correlated metal. calculation of ground state properties.

It differs from delta in the relative weight of the resonance and the Hubbard band.

Consistent with resistivity and specific heat measurements.

Similar conclusions A. Mc Mahan K. Held and R. Scalettar, for the alpha to gamma transition in Cerium.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Electrons are the glue that hold the atoms together. Vibration spectra (phonons) probe the electronic structure.

Phonon spectra reveals instablities, via soft modes.

Phonon spectrum of Pu had not been measured.

Short distance behavior of the elastic moduli.

Phonon SpectraTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Phonon freq (THz) vs q in delta Pu X. Dai et. al. Science vol 300, 953, 2003

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Inelastic X Ray. Phonon energy 10 mev, photon energy 10 Kev. vol 300, 953, 2003

E = Ei - Ef

Q =ki - kf

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Expts’ Wong et. al. Science 301. 1078 (2003) Theory Dai et. al. Science 300, 953, (2003)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

C’=(C11-C12)/2 = 4.78 GPa et. al. Science 300, 953, (2003)C’=3.9 GPa

C44= 33.59 GPa C44=33.0 GPa

C44/C’ ~ 7 Largest shear anisotropy in any element!

C44/C’ ~ 8.4

Shear anisotropy. Expt. vs TheoryTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

The high temperature phase, (epsilon) is body centered cubic, and has a smaller volume than the (fcc) delta phase.

What drives this phase transition?

Having a functional, that computes total energies opens the way to the computation of phonon frequencies in correlated materials (S. Savrasov and G. Kotliar 2002)

The delta –epsilon transitionTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Phonon frequency (Thz ) vs q in epsilon Pu. cubic, and has a smaller volume than the (fcc) delta phase.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Epsilon is slightly more delocalized than delta, has SMALLER volume and lies at HIGHER energy than delta at T=0. But it has a much larger phonon entropy than delta.

At the phase transition the volume shrinks but the phonon entropy increases.

Estimates of the phase transition following Drumont and Ackland et. al. PRB.65, 184104 (2002); (and neglecting electronic entropy). TC ~ 600 K.

Phonon entropy drives the epsilon delta phase transitionTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Phonons epsilon SMALLER volume and lies at HIGHER energy than delta at T=0. But it has a much larger phonon entropy than delta.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Develop new methods for treating realistic (system specific) strongly correlated electrons.

The DMFT machinery is in a very primitive state.

Study interesting materials science problems, develop some qualitative understanding of materials properties. Perform quantitative calculations.

DMFT- in its current state of the art, allows us to do both.

ConclusionTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Serious bottle neck of current interface of DMFT and band theory: U as a frequency independent parameter. Solution: E-DMFT +GW. [G. Kotliar, S.Savrasov, in New Theoretical approaches to strongly correlated systems, Edited by A. Tsvelik, Kluwer Publishers, (2001). Cond-matt 0308053, S. Biermann F. Aeryasetiwan, A. Georgs PRL 2003]

Fully implemented at the level of model Hamiltonian [Ping Sun’s talk]. Needs to be carried over to electronic structure.

Need further improvements of both electronic structure and many body tools. Illustrated compromises [Ti2O3 cluster, single site QMC +downfolding, Pu spectra and energy IPT+ ASA, Pu Phonons single site DMFT full potential+very primitive solver.

ConclusionTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Careful comparison with experiments. What do we need to reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

Need further developments in linear response dynamics to accommodate better solvers.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

THE STATE UNIVERSITY OF NEW JERSEY reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

RUTGERS

Colossal Magneto-resistance LaSrMnO3 reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

Double PerovskitesChattopadhyay:2001:PRB}

LaSrTiO3 doping driven Mott transition

Itinerant Magnetism: Iron Nickel

Half Metals

Pressure Driven Mott Transition V2O3

Presssure Driven Metal to Charge Transfer Insulator NiSeS

Kappa Organics

A partial list of applications of DMFT to materials.THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Cerium : alpha to gamma transition reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

Plutonium: delta and epsilon phase

Mott insulators, phonons and spectra, NiO, MnO

Bandwith control CaSrVO3, CaVO3 SrVO3

Heavy fermion without f eleLiV$_{2}$O$_{4}$ctrons

Fullerines K$_{n}$C$_{60}$}

Bechgaard Salts

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Biermann:2001 reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

Quantum criticality of CeCuAu Si et.al.

Heavy Fermion Insulators. Saso et.al.

CrO$_2$. Laad et.al.

FlNaV$_{2}$O$_{5}$ Fluctuating charge order

Chattopadhyay:2001Magnetic Semiconductors

Strongly Inhomogenous systems, surfaces and surface phase transitions.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Perfetti:2003, reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

Liebsch:2003}.

{Ruthenates} Sr$_{2}$RuO$_{4}$ Orbital differentiation.

Ti2O3 Metal to insulator transition

VO2 Metal to Insulator Transition.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Start with the TOE reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Rewrite the TOE as an electron boson problem. reproduce the softening of the 111 phonon ? Better solver at the single site level? Or cluster treatment of fcc Pu.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Build effective action for the local greens functions of the fermion and Bose field

- r=R+r
- R unit cell vector
- r position within the unit cell. Ir>=|R, r>
- Couple sources to

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

- Legendre transfor the sources, eliminating the field fermion and Bose field f,
Build exact functional of the correlation functionsW(r R,r’ R)

and G (r R,r’ R)

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

(E)DMFT pproximation to fermion and Bose field

Sum over all LOCAL 2PI graphs (integrations are restricted over the unit cell ) built with W and G

Map into impurity model to generate G and W

Go beyond this approximation by returning to many body theory and adding the first non local correction.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

THE STATE UNIVERSITY OF NEW JERSEY fermion and Bose field

RUTGERS

THE STATE UNIVERSITY OF NEW JERSEY fermion and Bose field

RUTGERS

LDA+DMFT functional fermion and Bose field

F Sum of local 2PI graphs with local U matrix and local G

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

THE STATE UNIVERSITY OF NEW JERSEY fermion and Bose field

RUTGERS

Outer loop relax fermion and Bose field

Edc

G0

Impurity Solver

Imp. Solver: Hartree-Fock

G,S

U

SCC

DMFT

LDA+U

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Static limit of the LDA+DMFT functional , fermion and Bose field

with FatomFHF reduces to the LDA+U functional

of Anisimov Andersen and Zaanen.

Crude approximation. Reasonable in ordered Mott insulators.

Total energy in DMFT can be approximated by LDA+U with an effective U . Extra screening processes in DMFT produce smaller Ueff.

ULDA+U < UDMFT

LDA+DMFT and LDA+UTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

C-DMFT: test in one dimension. fermion and Bose field (Bolech, Kancharla GK PRB 2002)

Gap vs U, Exact solution Lieb and Wu, Ovshinikov

Nc=2 CDMFT

vs Nc=1

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

QP bands in ruthenides: A. Liebsch et al (PRL 2000) fermion and Bose field

N phase of Pu: S. Savrasov G. Kotliar and E. Abrahams (Nature 2001)

MIT in V2O3: K. Held et al (PRL 2001)

Magnetism of Fe, Ni: A. Lichtenstein M. Katsenelson and G. Kotliar et al PRL (2001)

J-G transition in Ce: K. Held A. Mc Mahan R. Scalettar (PRL 2000); M. Zolfl T. et al PRL (2000).

3d doped Mott insulator La1-xSrxTiO3 Anisimov et.al 1997, Nekrasov et.al. 1999, Udovenko et.al 2002)

………………..

Very Partial list of application of realistic DMFT to materialsTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Anisimov Poteryaev Korotin Anhokin and Kotliar J. Phys. Cond. Mat. 35, 7359 (1997).

Lichtenstein and Katsenelson PRB (1998).

Reviews:

Held Nekrasov Blumer Anisimov and Vollhardt et.al. Int. Jour. of Mod PhysB15, 2611 (2001).

A. Lichtenstein M. Katsnelson and G. Kotliar (2002)

LDA+DMFT ReferencesTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Introduce local orbitals, Cond. Mat. 35, 7359 (1997).caR(r-R), and local GF

G(R,R)(i w) =

The exact free energy can be expressed as a functional of the local Greens function and of the density by introducing sources for r(r) and G and performing a Legendre transformation, G[r(r),G(R,R)(iw)]

Spectral Density Functional : effective action constructionTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

LDA+DMFT Self-Consistency loop Cond. Mat. 35, 7359 (1997).

E

U

DMFT

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Static limit of the LDA+DMFT functional , with Cond. Mat. 35, 7359 (1997).F= FHF reduces to LDA+U

Gives the local spectra and the total energy simultaneously, treating QP and H bands on the same footing.

Luttinger theorem is obeyed.

Functional formulation is essential for computations of total energies, opens the way to phonon calculations.

Comments on LDA+DMFTTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

LDA+DMFT: Cond. Mat. 35, 7359 (1997).

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 G.Kotliar funcional formulation for full self consistent implementation of a spectral density functional.

Application to Pu S. Savrasov G. Kotliar and E. Abrahams (Nature 2001).

ReferencesTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Long range Coulomb interactios, E-DMFT. R. Chitra and G. Kotliar

Combining E-DMFT and GW, GW-U , G. Kotliar and S. Savrasov

Implementation of E-DMFT , GW at the model level. P Sun and G. Kotliar.

Also S. Biermann et. al.

ReferencesTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Put in the loop of dmft +lda and the functional Kotliar

And chitra. Put in the effective action perspective. Put in the coupling constant integration.

Put in the cluster.

Think of formula for simga-lattice.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Basic idea: reduce the quantum many body problem to a one site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Basic idea: instead of using functionals of the density, use more sensitive functionals of the one electron spectral function. [density of states for adding or removing particles in a solid, measured in photoemission]

Dynamical Mean Field TheoryTHE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Master plan. 1) Fix titanite section by putting meet. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

2) Fix plutonium section by transporting and putting meet. From Berkeley.

3) Put the ideology. Overview of how really DMFT is used. Models + non models. And within models two pictures. Including the effective action perspective. 1] Coupling constant integration formula for DMFT models.

4) Conclusion. EDMFT in r,r’ and non local corrections around it. Indirect evidence, Ping successes . Indirect evidence, from local GW, that it gives the U’s we need for DMFT……….

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

Correlated electrons. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Model Hamiltonians.

DMFT-two perspectives-models and functionals.

cavity.-mention cluster.

How good the local approximation is.

Functional perspective-effective action

DMFT as an exact functional-DMFT as an approximation.

Interface with electronic structure-Anisimov.

Interace with a functional.

THE STATE UNIVERSITY OF NEW JERSEY

RUTGERS

THE STATE UNIVERSITY OF NEW JERSEY site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

RUTGERS

Introduce local orbitals, site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.caR(r-R)orbitals, and local GF

G(R,R)(i w) =

The exact free energy can be expressed as a functional of the local Greens function and of the density by introducing sources for r(r) and G and performing a Legendre transformation, G[r(r),G(R,R)(iw)]

Approximate functional using DMFT insights.

Spectral Density Functional : effective action construction (Chitra and GK).THE STATE UNIVERSITY OF NEW JERSEY

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DMFT Model Hamiltonian. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

+

Exact functional of the

local Greens function A

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DMFT for model Hamiltonians. Kohn Sham formulation. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Introduce auxiliary field

Exact “local self energy”

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About XC functional. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

- One can derive a coupling constant integration formulae (Harris Jones formula) for
- Generate approximations.
- The exact formalism generates the local Greens function and S ii is NOT the self energy. However one can use the approach as starting point for computing other quantities.

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Atoms as a reference point. Expansion in t. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Locality does not necessarily mean a single point. Extension to clusters.

Jii --- Jii Ji i+d

Aii --- Ai i+d

S ii --- S i i+d

Exact functional G[Aii ,Ai i+d]

The lattice self energy and other non local quantities extending beyond the cluster are OUTSIDE the formalism and need to be inferred.

Comments on functional constructionTHE STATE UNIVERSITY OF NEW JERSEY

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Comments on funct. construction. site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

- Construction of approximations in the cluster case requires care to maintain causality.
- One good approximate construction is the cellular DMFT: a) take a supercell of the desired range,b)

- c) obtain estimate of the lattice self energy by restoring translational symmetry.
- Many other cluster approximations (eg. DCA, the use of lattice self energy in self consitency condition, restrictions of BK functional, etc. exist). Causality and classical limit of these methods has recently been clarified [ G Biroli O Parcollet and GK]

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Basic idea: reduce the quantum many body problem to a one site or a cluster of sites, in a medium of non interacting electrons obeying a self consistency condition.

Basic idea: instead of using functionals of the density, use more sensitive functionals of the one electron spectral function. [density of states for adding or removing particles in a solid, measured in photoemission]

Dynamical Mean Field TheoryTHE STATE UNIVERSITY OF NEW JERSEY

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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 and Abrahams funcional formulation for full self consistent Nature {410}, 793(2001).

Reviews: Held et.al. , Psi-k Newsletter \#{\bf 56} (April 2003), p. 65 Lichtenstein Katsnelson and Kotliar cond-mat/0211076:

Realistic applications of DMFT References: combinations of DMFT with band theory.THE STATE UNIVERSITY OF NEW JERSEY

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THE STATE UNIVERSITY OF NEW JERSEY Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997).

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THE STATE UNIVERSITY OF NEW JERSEY Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997).

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Comparaison with the Hartree Fock static limit: LDA+U. Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997).

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THE STATE UNIVERSITY OF NEW JERSEY Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997).

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Dependence on structure Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997).

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The local Greens function A, and the auxilliary quantity Kotliar, J. Phys. Cond. Mat. 35, 7359-7367 (1997). S, can be computed from the solution of an impurity model that describes the effects of the rest of the lattice on the on a selected central site.

One can arrive at the same concept via the cavity construction.

Mapping onto impurity models.THE STATE UNIVERSITY OF NEW JERSEY

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Two roads for ab-initio calculation of electronic structure of strongly correlated materials

Crystal structure +Atomic positions

Model Hamiltonian

Correlation Functions Total Energies etc.

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