Lecture Notes Introduction to Strongly Correlated Electron ... · Jahn-Teller-Effect Orbitals...
Transcript of Lecture Notes Introduction to Strongly Correlated Electron ... · Jahn-Teller-Effect Orbitals...
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Lecture Notes
Introduction to Strongly Correlated Electron
Systems
Mohsen Abd-Elmeguid
II. Institute of Physics, University of Cologne, Germany
WS 2014/ 2015
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II. Classes of strongly correlated electron systems
(a) Transition metal compounds: 3d-electrons
- Hubbard model, Mott insulator, metal-insulator transition
- Spin, charge, and orbital degrees of freedom and ordering phenomena, selected materials
(b) Heavy fermion systems: 4f (5f) – electrons
- The Kondo effect, heavy fermion systems, non-Fermi liquid behavior,
- Quantum phase transitions, unconventional superconductivity, selected materials
(c) Nanoscale structures:
- Quantum confinement, unusual properties for potential applications
III. Pressure effect on the ground state properties: - Recent experimental results on heavy fermions and transition metal compounds
IV. Summary and open discussion
I. Introduction
Brief summary of electrons in solids, origin of strong electron correlations
Introduction to strongly correlated electron systems
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?
Hubbard
U
Crystal field
Band
formation
Transition metal systems and electron correlations
systems can be quite close to the borderline U~ W (t)
Thus many interesting transitions to unusual ground states can occur by changing
T, P, filling, structure, etc.
more discussion with examples later!
Delicate balance
Orbital
Spin Charge
Hund's coupling
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Orbital degree of freedom
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3d orbitals in central potential of a free atom/ ion
3d: n=3, =2, m= -2,-1,0,1,2 5 orbitals
5-fold degenerate 3d orbitals
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d-Orbitals and Ligand Interaction (Octahedral Field)
d-orbitals not pointing directly at axis are least affected
(stabilized) by electrostatic interaction
d-orbitals pointing directly at axis
are affected most by electrostatic
interaction
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Orbitals degeneracy
YTiO3
3d1
Orbitals degeneracy is lifed by:
1) Exchange interactions
2) Coupling to the lattice
more details later!
eg
t2g
eg
t2g
eg
t2g
YVO3
3d2
LaMnO3
3d4
„pseudo-Cubic“ Perovskites
orbitals degeneracy
orbital degree of freedom
1. Lattice distortion (Jahn-Teller)
2. orbital and spin dependent
superexchange
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Differences between Orbitals and Spins
Distortion Anisotropy
The orbitals are usually strong coupled to the lattice
cubic
eg
t2g
3d4 distorted
rotated orbitals are not equivalent
Spins in 1. approximation invariant;
e.g. In Ferromagnets alle spins are
aligned in the same direction, but this
direction is arbitary
Lifts the orbital degeneracy
If, however, exchange interaction is domenating,
orbitals will be strongly coupled to the spins
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Lower Symmetry
t2g
- Orbitals
(xy, xz und yz)
eg – Orbitals
(x2-y2 and 3z2-r2)
3d
cubic eg
t2g
compress stretch
tetragonal
t2g
eg
xy
yz
zx
x2-y2
3z2-r2
orthorhombic
z2
x2-y2
xy
xz,yz xz,yz t2g
eg
xy
x2-y2
z2
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Orbital degeneracy is lifted by:
1. Lattice distortion (Jahn-Teller) and/ or
2. orbital and spin dependent superexchange
Both mechanisms lead to orbital order
periodic arrangement of specific orbitals
which leads to a long-range ordered pattern
LaMnO3
Orbital Order
orbital order:
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i j
i j
Ferro-orbital ordering:
the same orbital is occupied at each site
Antiferro-orbital ordering:
different orbitals are occupied at neighboring sites
Types of orbital ordering
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En
erg
y
distortion r
lattice
orbitals
total energy
Jahn-Teller-Effect
Orbitals degeneracy is lifted by spontaneous distortion
Distortion of the octahedron leads to:
-Linear reduction of the electron energy
-Quadratic increase of the lattice energy
E(r) at minimum when distortion r = g/c
e.g.: 3d1 in
cubic crystal field
xy
t2g
eg z2
x2-y2
xz,yz
Jahn-Teller active Ions (orbital degeneracy):
1, 2, 4, or 5 elektrons in t2g-Orbitals; or
1 or 3 elektrons in eg-Orbitals
r rr 2
2( )E
cg
By the distortion, the orbital degree of freedom is „quenched“; but spin
degree of freedom remains preserved .
g electron phonon coupling
c bulk modulus
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Orbital Order- Cooperative JT effect
Jahn-Teller effect mediates interaction between orbitals
of next neighbors sites, thereby leading to orbital order
stretching of next neighbors Octahedra in
direction perpendicular to each other.
Cooperative Jahn-Teller effect
Coupling between local distortions on different sites
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2. Orbital and spin dependent superexchange
exchange mechanism which couples Orbital and magnetic order
Kugel-Khomskii model
K. I. Kugel and D. I. Khomskii, Sov. Phys. JETP 37, 725 (1973);
K. I. Kugel and D. I. Khomskii, Sov. Phys. Ups. 25, 231 (1982)
For more details, see:
description and comments, see board!
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orbital occupancy determine the sign and magnitude
of exchange interaction, see board!
Examples:
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order patterns: LaVO3
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order patterns: LaMnO3
eg – Orbitals
(x2-y2 and 3z2-r2)
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Experimental methods for investigation of Orbital Ordering
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Charge Ordering in Nd0.5Sr0.5MnO3
0
50
100
150
200
250
300
350
19 21 23 25 27 29 31
2-Theta (Degrees)
Inte
ns
ity
160 K
Incipient CO Phase
0
50
100
150
200
250
300
350
19 21 23 25 27 29 31
2-Theta (Degrees)
Inte
ns
ity
50 K
T = 160 K Valence Mixed State
T = 60 K Charge Ordered State
Synchrotron X-ray Powder Diffraction Data (NSLS-X7A)
A series of weak superstructure reflections arise (1% intensity at the
strongest) that indicate doubling of the a -axis.
Woodward, Cox, Vogt, Rao, Cheetham, Chem. Mater. 11, 3528-38 (1999).
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Orbital Ordering in Nd0.5Sr0.5MnO3
5.30
5.35
5.40
5.45
5.50
5.55
0 100 200 300
Temperature (K)
Cel
l P
ara
met
er (
A)
(b)
c
a
b/sqrt(2)
Upon cooling below 150 K, the a & c-axes expand and the
b-axis contracts. This is the signature of orbital ordering
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Examples of Orbital Ordering
22.18 Å
21.91 Å
21.94 Å
22.07 Å
LaMnO3 (298 K)
Rodriguez-Carvajal, et al.
Phys. Rev. B 57, R3189
(1998).
NdSrMn2O6 (50 K)
Woodward, et al. Chem.
Mater. 11, 3528-38
(1999).
Mn3+
Mn4+
41.90 Å
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First in short: X-ray absorption spectroscopy
Experimental methods for investigation of Orbital Ordering
Resonant Inelastic X-ray Scattering (RIXS)
For an excellent review see:
Amen et. al; Rev. Mod. Phys. 83 705 (2011)
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X-ray absorption spectroscopy
Each edge of each element has
a characteristic binding energy
Absorption occurs when the
energy of the incident photon is
sufficient to eject the electron.
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X-ray fluorescence spectroscopy (XFS)
Principle: X-ray fluorescence lines:
an element specific technique!
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core level energies
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Examples for different edges
Examples:
Cu K-edge ~9000 eV
Cu L-edges ~930 eV
Cu M-edges ~70-120 eV
Fe K-edge ~7000 eV
Fe L-edges ~720 eV
Fe M-edges ~50-100 eV
S K-edge ~2472 eV
S L-edges ~200 eV
• An edge results when a core electron absorbs energy equal to or greater
than its binding energy
• Results in transitions to unoccupied atomic or molecular orbitals
• Edges are labeled according to the shell the core electron originates from
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Jahn-Teller distortion and/ or Superexchange lead to
orbital order
Excitations are different! Local crystal field excitations vs. dispersing orbitons
Superexchange: spins and orbitals entangle. Jahn-Teller: spins and orbitals decouple, orbitals frozen out at low temperatures.
Orbital Order
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Ament et. al; Rev. Mod. Phys. 83 705 (2011)
Elementary excitations in condensed matter
crystal field transitions between different d-orbitals
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Resonant Inelastic X-ray Scattering (RIXS)
For an excellent review see:
Amen et. al; Rev. Mod. Phys. 83 705 (2011)
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Photon promotes a core electron to
empty band
electron from a different state in
valence band decays and annihilates
the core level hole
electron-hole excitation
RIXS creates excitation in the valence band with momentum ℏk’- ℏk and energy ℏk’ - ℏk
Direct RIXS
Amen et. al; Rev. Mod. Phys. 83 705 (2011)
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Indirect RIXS
electron is excited from a deep-lying core level into the valence shell. Excitations are created through the Coulomb interaction UC between the core hole (and in some cases the excited electron) and the valence electrons. The photoelectron subsequently decays leaving behind an excitation in the valence
band with momentum ℏk’- ℏk and energy ℏk’ - ℏk
Amen et. al; Rev. Mod. Phys. 83 705 (2011)
The measured photon energy transfer and momentum transfer in a RIXS experiment is
directly related to the energy and momentum of the created excitations (spinons, orbitons)
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RIXS Instrument f0r soft x-rays: SAXS at the Swiss Light Source
L3-edge resonance
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RIXS Instrument for hard x-rays: IDB 30 beamline at APS, USA
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Energy dependence of elementary excitations in Sr2CuO3
observed with RIXS at the copper L3-edge resonance.
J Schlappa et al. Nature 485, 82 (2012)
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orbital excitation from the ground-state copper 3d x2 − y2
orbital to an excited copper 3d xy or xz orbital
J Schlappa et al. Nature 485, 82 (2012)
dispersion of orbital and spin excitations across the first Brillouin zone