x-ray scattering with synchrotron radiation e. ercan alp advanced photon source argonne national...
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X-Ray Scatteringwith synchrotron radiation
E. Ercan AlpAdvanced Photon Source
Argonne National Laboratory, Argonne, Illinois 60439
JASS’02, October 19-28, 2002Amman, Jordan
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Advanced Photon Source
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Argonne National Laboratory, Illinois USA
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What is x-ray scattering ?
• Scattering – Coherent or incoherent
• Diffraction– Always coherent
• Spectroscopy– Frequency distribution
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atom
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transverseElements of Modern X-Ray Physics
Jens Als-Nielsen & Des McMorrowJ. Wiley, 2001
X-rays are transverse electromagnetic waves where electric and magneticfields are perpendicular to the direction of propagation (Barla, 1904).
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Spatial variation k= wave number=wavelength
Temporal variation = angular frequency
Top view showing high and low field amplitudes
Electromagnetic waves
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The incident plane wave incident upon an electron sets the electronin oscillation. The oscillating electronthen radiates, experiencing a
phase shift of
In-plane
Out-of-plane
Classical description of
scattering of radiation
by a charged particle
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Scattering from one electron can be classically viewed as radiation emitted from a dipole.
The radiated field at a distance R as a function of time is given by:
Erad (R,t) e
40c2R
aX ( t ), t t R c
• P
Q•
•O
r r
r r
s
r
V
Principles of Optics
Born & WolfCambridge University
Press 7th edition (1999)
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Acceleration = force/mass
Acceleration seen by the observer at = /2 is zero:
x
y
z
p̈
n
r
aX ( t ) e
mEx 0e
i t cos e
mEine i R c cos
Erad R,t e
40c2R
em
Eine i R c cos
Erad R,t Ein
e40c
2R em
e ikR
Rcos
r0 e 2
40mc 22.8210 13m
Classical electron radiusThomson scattering length
Classical electron radius
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Iscattered
Iincident
dd
Erad2 R2
Einc
2A0
r02 cos2
when all angles are included
dd
8
3
r0
2 0.655 barn, 1 barn = 10-24 cm2
The interesting aspect of this result is that the classical scatteringCross-section from an electron is INDEPENDENT of energy
Differential Scattering cross-section
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dd
r0
2P
1 synchrotron radiation, vertical scattering plane
P cos2 synchrotron radiation, horizontal scattering plane
12
1 cos2 unpolarized source like x - ray tube
Scattering cross-section (cont’d)
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Momentum and energy transfer in a scattering process
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Scattering of electromagnetic waves from charged
particles Born Approximation
Consider a monochromatic electromagnetic field scattering from a isotropic, static medium with :
2E(r,) k 2n2(r,)E(r,) 0This equation has already some simplifications like dielectric constant has a slow variation with position,
where n is the index-of-refraction, or refraction index of the medium._______________Born & Wolf, Principles of Optics, 7th edition, pp 695-700 (1999)
(r,) n2 r,
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If we take a single Cartesian component of E (r,) as U (r,), we can write the following scalar equation :
2U(r,) k 2n2(r,)U(r,) 0
2U(r,) k 2U(r,) 4F(r,)U(r,)
F(r,) 1
4n2(r,) 1 : scattering potential
If the field U(r,) is considered to be sum of incident and scattered fields
U(r,) U i (r,) U s (r,)
One can approximate the incident field to be a plane wave,
which propogate according to Helmholtz equation:
(2 k 2)U i (r,) 0
and the scattered field
(2 k 2)U s (r,) 4F(r,)U(r,)
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An inhomogeneous differential equation can be solved usingGreen’s function approach:
2 k2 G(r r ,) 4
r r
and choose G(r
r ,) e ik r - r
r -
r
When the field propagates in a specific direction in real space, s
0,
the time independent part of Ui r,w eik s 0
r , and
U r, eik s 0
r F( r ,)
V
U r , e ik r - r
r -
r d3 r
This is an integral equation for the total field U(r,) within the scattering volume V. If the solution inside the volume V (i.e inside the scatterer, for which we have no idea, that’s the reason we are doing the experiment) is known, then the solution for the exterior can be
obtained.
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First order Born approximation For weakly scattering media, it is possible to obtain solution to theintegral equation by a perturbation approach, provided that the scattering medium is weakly interaction with the probe of x-rays.
The first order Born approximation states that amplitude of the scattered wave far away from the scatterer depends entirely on one and only one Fourier component of the scattering potential, namely the one that corresponds to the transferred momentum K=k(s-s0).
K=k-k’
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Conservation of momentum has a correspondence between classical and quantum mechanical treatment:
p k
p p p k
If a plane wave is incident on the scatterer in the direction of s, the Fourier component of the scattering potential can be determined.
And if one has the ability to vary the amount of momentum transfer at will, then, the scattering potential can be reconstructed.
This is the essence of x-ray scattering experiments.
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k 1,1
k 2,2
q
1 2 energy transferredq =
k 1
k 2 momentum transferred
Scattering geometry and physics
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The goal of the experiments is to measure the scattering cross - section
d2
ddq ,
d2
ddq , d
d
T hompson
Sq , resonant terms
Sq , 1
2dte it i e
iq r
j't e
iq rj 0
jj' f
is the Fourier transform of the correlation of the phase of the scattering
amplitude at different times
What is really measured ?
Double differentialScattering cross-section
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The physical origin of the correlations depends on how 1q compares with lc ,
the characteristic length, of the system related to the spatial inhomogeneity.
when q lc 1 COLLECTIVE BEHAVIOUR
when q lc 1 SINGLE PARTICLE BEHAVIOUR
when 1q d and phonon frequency Collective ion excitation
when 1q rc and plasma frequency Valence electron excitation
Scattering geometry and physics
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•Study of atomic, electronic and collective excitations •as a function of energy and spatial extension. •Energy transfers from neV to keV (1012 eV)•Momentum transfers from 1 to 100 nm-1 (102 nm-1 )•Bulk probe, non-destructive•Suitable for wide range of parameter space:
–Temperature–Pressure–Magnetic field–Chemical doping
Inelastic X-Ray Scattering
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Energy EnergyTransfer
Science
Nuclear ResonantInelastic X-RayScattering
6-30 keV neV-100 meV Phonons, magnons,thermodynamic and elasticproperties
Collective latticeexcitations
10-30 keV 1-200 meV Lattice dynamics, thermaland elastic properties ofsolids and liquids, phonons
Electronicexcitations
0.1-10 keV 1-40 eV Details of electronic energylevels, symmetry inCorrelated electron systems
Compton scattering 10-100 keV keVFermi surface in correlatedelectron systems, rare-earthcompounds, heavy fermions
Inelastic X-Ray Scattering (cont’d)
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Set-up at 3-ID-C, APS
Analyzer
Detector
Sample
Mirror
High Resolutionmonochromator
Firstmonochromator
Undulator
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200 m
1 mm
4 mm 1.6 mm
80 m
Monochromatization and energy analysis is going to be covered next time
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IXS in Al with 1 meV resolution at 25.701
keV January 30,2002, @ 3-ID of the APS
PHONONANNIHILATION
PHONONCREATION
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Be phonon dispersion measurementsM
omen
tum
tra
nsf
er
Energy transfer (meV)
Sca
tteri
ng c
ross
-sect
ion
, S(q
,)
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Be phonon form factor, A. Alatas (2002)
lowest possible by diffraction
NEW
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Al phonon measurements
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Ahmet AlatasPhD thesis, 2002
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Liquid Sapphire @ 2400 K (H. Sinn, D. Price, M. L. Saboungi)Liquid Sapphire @ 2400 K (H. Sinn, D. Price, M. L. Saboungi)
Speed of sound is extracted from Q-dependence of the peak energy,
Viscosity can be extracted from Q-dependence of either width of theinelastic peak (Brillouin), , or the intensity of the elastic peak (Rayleigh)
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Compton scattering by free electrons
The change in energy of photons as they are scattered by an electronis proportional to Compton scattering length given by
c
mc
r0
c
1137
It is interesting to note that the ratio between classical electron radiusand Compton scattering length is a fundamental constant.
kk
1 Ck(1 cos)
Furthermore, it should be noted that Compton scattering is an extremeexample of inelastic x-ray scattering, and it can be used to differentiatebetween localized (core) electrons and valence (free) electrons.
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Energy loss during Compton scattering as a function of angle, andfor different incident energies (after Jens Als-Nielsen)
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Compton Scattering3-D reconstruction of electron momentum density in Li
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Y. Tanaka, et alPhys. Rev. B 63 (2001) 045120
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Magnetic Compton Scattering
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Measurement of population of (x2-y2) and (3z2-r2) of eg orbitals in La2-2xSr1+2xMn2O7
(A. Koizumi, et al, Phys. Rev. Lett. 86 (2001) 5589.
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Magnetic Compton Scattering @ APS
Measurement of the ratio of magnetic electrons to the total electrons
3.1 %
2.6 %
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•6.35 eV Charge transfer excitation•3.8 eV Exciton-like feature.•1.7 eV d-d optically forbidden excitation.
CMC-CAT
c-axis
Q along c-axis
Resolution = 0.3 eV
Excitation Spectrum of CuGeO3
Resonant Inelastic X-ray ScatteringCourtesy to : J. P. Hill, Brookhaven Nat. Lab.
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For incident photon energies near an absorption edge, a large resonant enhancement is observed in the inelastic scattering:
CMC-CAT
CuGeO3
Mom
en
tum
tra
nsfe
r
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Copper
Oxygen
()
(,0)
CMC-CAT
In 1d CuGeO3 no dispersion of
exciton. In 2d La2CuO4 two excitons
seen, with significant dispersion. Provides unique information on UHB and LHB and role of correlations.
Kim, Hill et al.
La2CuO4
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Electronic orbitals
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Octahedral and cubic fields
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10-13
10-11
10-9
10-7
10-5
10-3
10-1
ener
gy r
esol
utio
n (e
V)
meV resolution IXS
neV resolution NRS
µeV resolutioninterferometry / NLE
0.2 meV
500 neV
1992-2002
1995-2002
GAP
High energy resolution x-ray scattering
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