Introductory lectures on

Angle-resolved photoemission
spectroscopy (ARPES)
and its application to the experimental study
of the electronic structure of solids

Andrs Felipe Santander-Syro

Universit Paris-Sud
and
Ecole Suprieure de Physique et Chimie Industrielles - Paris
 Resources
BOOKS
S. Hfner. Photoelectron Spectroscopy Principles and Applications, third edition,
Springer (Berlin), 2003.
REVIEW ARTICLES
F. Reinert and S. Hfner, New Journal of Physics 7, 97 (2005).
A. Damascelli, Z.-X. Shen, S. Hussain, Rev. Mod. Phys. 75, 473 (2003).
J. C. Campuzano, M. R. Norman, M. Randeria, cond-mat/0209476.
J. Braun. The theory of angle-resolved ultraviolet photoemission and its application to
ordered materials. Rep. Prog. Phys. 59, 1267-1338 (1996).

INTERNET
www-bl7.lbl.gov/BL7/who/eli/SRSchoolER.pdf
(by Eli Rotenberg, Advanced Light Source, Berkeley)
www.physics.ubc.ca/~quantmat/ARPES/PRESENTATIONS/ Lectures/Exciting2003.pdf
(by Andrea Damascelli, UBC)
ftp://ftp.espci.fr/shadow/bontemps/cargese2005.zip
(ARPES lectures by Ralph Claessen, Augsburg)
 Condensed (crystalline) matter in a nutshell
Allowed electronic states Many properties of solids are determined
Repeated-zone scheme by electrons within a narrow energy slice
-kF kF (~kBT) around EF (dc conductivity,
magnetism, superconductivity)
Fermi Surface

3D

2D

1D

Adapted from A. Damascellis Exciting-2003 lecture (at room temperature, kBT = 25 meV)
and E. Rotenbergs lecture
ARPES: energy and momentum conservation
Kinetic energy analyzer
v
v h , A Fixed during experiment
h , A z
Ekin, W, , Measured
e- Detector

y Conservation laws

x Sample
Ekin = h W E B
k vacuum
||
= k solid
||
In the solid
EB
k || hk vacuum = 2mEkin sin
||
 To make it work

Pull the electron out of its bound state

W ~ 2 5 eV 0 < Ekin = h W E B
E B ~ 0 1 eV (Valence band)
h ~ 10 2000 eV

d
xe
E B 1500 eV (interesting core levels)

Fi
The electron has to make its way up to the samples surface
Experimentally:
esc = electron escape depth
(Ekin~ 10 2000 eV) [10 2000 eV] 10 50

PES is a surface technique: one needs clean surfaces and work under ultra-
high vacuum
ARPES needs, furthermore, atomically-flat surfaces (for ideal conservation
of surface-parallel momentum): prepare surfaces in-situ, cleave,
 Furthermore, one has to make sure that the
photoemission process itself does not modify
the electronic structure of the material
SUDDEN APPROXIMATION
The ejected electron should be fast enough to neglect its
interaction with the hole left behind
2 At h 25 eV
e- - e- interaction ee Ekin ~ 20 eV
P
2 Ekin esc ~ 10
e- time of escape esc /
m For cuprates
2
1 esc P h P ~ 1 eV
<< ee Ekin >> m
2 2 / ee 0.1
 When all of this works
ARPES gives direct access to the single-particle electronic structure of a crystal:
Band structure
Spectral line-shapes and widths: electron scattering rate Interactions

a = CuO = 3.82
EB [eV]
Y
M
X

0.6
3
kx /a
ky

h = 22 eV
Bi2Sr2CaCu2O8+
 Instrumentation and implementation

Kinetic energy analyzer

v
Light source h , A z

e- Detector

y
x Sample

Samples surface preparation

Sample moving, rotating, cooling
 Radiation sources
Laboratory sources
Gas discharge lamps (h ~ 20-50 eV)
X-ray tubes (h ~ 1500 eV)
Synchrotron radiation
Tunable (h ~ 10 eV 10 keV)
Brilliant
Polarized (linear and circular)
Temporal structure (time-resolved experiments)
Laser
IR laser + 2*(frequency doubling): h ~ 6 7 eV (Ekin ~ 1-2 eV)
esc ~ 50 100
Sudden approximation ?!
Probes reciprocal space only near -point
Under development: UV and soft X-ray laser (IR laser + high-
harmonic generation inside rare-earth gas)
 Electron energy analyzer

Adapted from A. Damascellis Exciting-2003 lecture

 Interaction effects on ARPES spectra
I (k , ) = I 0 (k , , A ) f ( )A(k , ) A(k,) = Probability of adding or
removing one electron at (k,)

1 (k, )
A(k, ) = E B h , h = 1
[ k (k, )]2 + [(k, )]2

Energy renormalization
Many-body physics
Lifetime of dressed e-

k k() I(k,)
(k,)
EF (renormalization)
(k,)
(life-time)

EF
k Binding energy EB
 Lifetime of the photo-electron
and measured line-widths
Assuming Lorentzian line-shapes, the
total (measured) width is given by:
tot
vh
tot h + e
ve

~ meV ~ eV

Spectrum dominated by final-

state (photo-electron) line-widths,
unless
vh << ve

2D and 1D systems !
Adapted from:
T.-C. Chiang, Chemical Physics 251, 133-140 (2000) Adapted from R. Claessens Cargese-2005 lectures
 Spectra analysis: EDCs
Line-shapes and widths many-body physics

1 (k , )
A(k , ) =
[ k (k , )]2 + [(k , )]2

EDC: Lorentzian if and only if

and independent of
 Spectra analysis: MDCs
Line-shapes and widths many-body physics
1 (k , )
A(k , ) =
[ k (k , )]2 + [(k , )]2

MDC: Lorentzian if and only if

kc = k F + [ ( )] / vF0
k HWHM = ( ) / vF0
 Many-body physics Effects of the
interactions on the band structure:
Example of surface states of Mo(110)

ee ~ 2
Mo(110) band along N
T = 70 K e-ph Eliashberg
e-imp = const

T. Valla et al., PRL 83, 2085 (1999)

Strongly-correlated electron
systems
(brief recall)
 Transition-metal
oxides: solid-state
SCES

MH ~ 1-2 eV
Cu O Cu
 Transition-metal oxides
Strongly-correlated electrons systems

New physics displaying exotic electronic states

in a solid sample
 Cuprates:
antiferromagnetic insulators that become
high-Tc superconductors upon doping!

Crystal unit-cell

Antiferromagnetic unit cell

 Cuprates: (rough) phase diagram

Coexistence ?
Electron-doped cuprates:

Generalities
R2-xCexCuO4 : crystal structure

CuO2 plane

(R,Ce)2O2 block
R/Ce

CuO2 plane

(R,Ce)2O2 block

CuO2 plane
 Electron-doped cuprates:
effects of Ce-doping and annealing

H. J. Kang et al., Nature Materials 6, 224 (Feb. 2007).

L. Shan et al., cond-mat/0703256 (March 2007).
 Fermi surfaces, Brillouin zones and AF-zones:
hole-doped vs electron-doped cuprates

Nd2-xCexCuO4 (x = 0.15) Tl2Ba2CuO6+d

N. P. Armitage et al., PRL 88, 257001 (2002) M. Plat et al., PRL 95, 077001 (2005)
Antiferromagnetic-induced band-folding in
underdoped Sm2-xCexCuO4 (x = 0.14)

S. R. Park et al., cond-mat/0612419 (Dec. 2006)

Effects of annealing on band structure at optimal
doping: the case of Pr1.85Ce0.15CuO4

Annealed

As-grown

P. Richard et al., cond-mat/0704.0453 (Apr. 2007)

 Electronic structure and
signatures of interactions in
Sm1.84Ce0.16CuO4
Coworkers - collaborators
Takeshi Kondo, Adam Kaminski
(Ames Lab - Iowa)
Stphane Pailhs (PSI and LLB)
Johan Chang, Ming Shi, Luc Patthey (PSI)
Alexandre Zimmers
(CSR Maryland and INP P6)
Bing Liang, Pengcheng Li, Rick Greene
(CSR - Maryland)
Sm2-xCexCuO4 : Fermi surface and doping
0.0

Binding energy [eV]

-0.1
(,)
Max
-0.2

-0.3
(,0)
Min
-0.4

0.6
0.2
0.4

0.8
1.0
1.2
1.4
-
Momentum along AFZB [2 /a]
(,) Doping from FS volume:
x = 0.16 0.01
Single-band FS (no band-folding)
Suppressed spectral weight at hot-spots
(,0) Tight-binding fit
 Sm2-xCexCuO4 (x = 0.16) :
Nodal vs anti-nodal ARPES spectra

N
AN
0.0 AN 0.0 N

Binding energy [eV]

Binding energy [eV]

-0.2 -0.2
Max Max

-0.4 -0.4

-0.6 Min
-0.6
Min
-1
0.1 -1
0.1
-0.8 kAFZB -0.8
kAFZB
 Sm2-xCexCuO4 (x = 0.16) : N

Nodal and anti-nodal MDCs AN

AN = -200 meV N = -200 meV

= -100 meV
= -100 meV

-1 -1
0.1 0.1 = 0 meV
= 0 meV

Relative momentum Relative momentum

Anti-nodal and nodal MDCs are Lorentzians
MDC peak maximum gives the quasi-particle dispersion
MDC width is proportional to quasi-particle scattering rate (self-energy)
 Sm2-xCexCuO4 (x = 0.16) :
Nodal vs anti-nodal EDCs
Hump AN
N
AN AN

-0.8 -0.4 0.0

AN Binding energy [eV]

Anti-node
N Peak-hump structure close to kF
Lorentzian EDCs at energies > 300 meV

Node
-0.8 -0.6 -0.4 -0.2 0.0 No clear peak-hump structure
Binding energy [eV] EDCs are not Lorentzian
 Sm2-xCexCuO4 (x = 0.16) :
Nodal vs anti-nodal dispersions
0.0

-0.1
Binding energy [eV]

-0.2
AN
-0.3

-0.4 N
N AN
-0.5 -1
0.1

-0.6
Relative momentum
 Sm2-xCexCuO4 (x = 0.16) :
Nodal vs anti-nodal line-widths

0.4 ( ) = vband
0
k HWHM

0.3
Im() [eV]

0.2
AN
0.1
From EDC-width
N
0.0
-0.5 -0.4 -0.3 -0.2 -0.1 0.0
Binding energy [eV]
 Conclusions
When it works
ARPES is a powerful technique for the study of the
electronic structure of complex systems

Detailed band structures and Fermi surfaces

k-dependent Fermi velocity and effective mass
Gaps
Many-body effects in the QP dispersion
Kinks
Fermi-surface nesting

Outlook (and dreams)

Spin-resolved ARPES
Time-resolved ARPES
Micro-ARPES