Introduction to Inelastic Neutron Scattering · 5 Neutron interactions with matter •Neutrons...
Transcript of Introduction to Inelastic Neutron Scattering · 5 Neutron interactions with matter •Neutrons...
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Introduction to Inelastic Neutron Scattering
Bruce D Gaulin McMaster University
Neutrons: Properties and Cross Sections
Excitations in solids
Triple Axis and Chopper Techniques
Practical concerns
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235U + n g
daughter nuclei + 2-3 n + gammas
neutrons: no charge s=1/2 massive: mc2~1 GeV
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5
Neutron interactions with matter
• Neutrons interact with…
• Nucleus
• Crystal structure/excitations (eg. Phonons)
• Unpaired electrons via dipole scattering
• Magnetic structure and excitations
Nuclear scattering Magnetic dipole scattering
Properties of the neutron Mass mn =1.675 x 10-27 kg
Charge 0
Spin-1/2, magnetic moment n = -1.913 N
NXS School
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Wavelength-energy relations
NXS School 6
Neutron as a wave … Energy (E), velocity (v), wavenumber (k), wavelength ()
Energy (meV) Temperature (K) Wavelength (Å)
Cold 0.1 – 10 1 – 120 4 – 30
Thermal 5 – 100 60 – 1000 1 – 4
Hot 100 – 500 1000 – 6000 0.4 – 1
E h2k 2
2mn
h2
2mn
2
2
81.81meV Å2
2
k mnv
h
2
E kBT 0.08617meV K1 T
~ interatomic spacing E ~ excitations in condensed matter
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The Basic Experiment:
(, )
Incident Beam: • monochromatic • “white” • “pink”
Scattered Beam: • Resolve its energy • Don’t resolve its energy • Filter its energy
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Fermi’s Golden Rule within the 1st Born Approximation
W = 2 /h |< f | V | i>|2 (Ef)
= W / = (m/2h2)2 kf / ki |< f | V | i>|2
2 / Ef = kf/ki coh/4 N Scoh(Q, ) + kf/ki incoh/4 N Sincoh(Q, )
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Nuclear correlation functions
NXS School
9
G(r,t) 1
N r'R j ' (0) r'r R j (t)
jj '
dr'
Pair correlation function
I(Q,t) G(r,t)eiQrdr 1
Nexp iQ R j '(0) exp iQ R j (t)
jj'
Intermediate function
S(Q,) 1
2hI(Q,t)eitdt
Scattering function
d2
ddE f
scat
4
k f
ki
NS(Q,)
Differential scattering cross-section
May 31, 2009
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Nuclear (lattice) excitations
NXS School 10
Commonly studied excitations
Phonons
Librations and vibrations in molecules
Diffusion
Collective modes in glasses and liquids
Neutron scattering measures simultaneously the wavevector and energy of collective excitations dispersion relation, (q)
In addition, local excitations can of course be observed
Excitations can tell us about
Interatomic potentials & bonding
Phase transitions & critical phenomena (soft modes)
Fluid dynamics
Momentum distributions & superfluids (eg. He)
Interactions (eg. electron-phonon coupling)
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Atomic diffusion
NXS School 11
Cocking, J. Phys. C 2, 2047 (1969)..
Liquid Na
Auto-correlation function
r2(t) 6Dt
For long times compared to the collision time, atom diffuses
Gs(r,t) 6 r2(t) 3 / 2
exp r2
6 r2(t)
S(Q,) 1
hexp
h
2kBT
DQ2
2 (DQ2)2
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Molecular vibrations
NXS School 12
Prassides et al., Nature 354, 462 (1991). C60 molecule
Large molecule, many normal modes
Harmonic vibrations can determine interatomic potentials
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2 / a
2 / a
Origin of reciprocal space; Remains fixed for any sample rotation
Mapping Momentum – Energy (Q-E) space
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Q
ki
kf
-kf
Bragg diffraction: Constructive Interference Q = Reciprocal Lattice Vector
Elastic scattering : | ki | = | kf |
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Q
ki
kf
-kf
Bragg diffraction: Constructive Interference Q = Reciprocal Lattice Vector
Elastic scattering : | ki | = | kf |
2 / a
a
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Elementary Excitations in Solids
• Lattice Vibrations (Phonons) • Spin Fluctuations (Magnons)
Energy vs Momentum • Forces which bind atoms together in solids
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Phonons
17 Lynn, et al., Phys. Rev. B 8, 3493 (1973).
Normal modes in periodic crystal wavevector
Energy of phonon depends on q and polarization
FCC Brillouin zone
FCC structure
u(l,t) 1
NM j q exp iq l ˆ B qj,t
jq
Longitudinal mode Transverse mode
NXS School
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Phonon intensities
18 Guthoff et al., Phys. Rev. B 47, 2563 (1993).
S1 Q, 1
2NMeQ 2 u2 Q j q
2
j q 1 n Q q j q
jq
Structure (polarization) factor
0 1/2
Trans
Pho
no
n E
ne
rgy
q, [00]
Long
NXS School
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More complicated structures
19
Woods, et al., Phys. Rev. 131, 1025 (1963). Optical phonon
Acoustic phonon
La2CuO4
Chaplot, et al., Phys. Rev. B 52, 7230(1995). NXS School
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Spin excitations
NXS School 20
Spin excitations Spin waves in ordered magnets
Paramagnetic & quantum spin fluctuations
Crystal-field & spin-orbit excitations
Magnetic inelastic scattering can tell us about Exchange interactions
Single-ion and exchange anisotropy (determine Hamiltonian)
Phase transitions & critical phenomena
Quantum critical scaling of magnetic fluctuations
Other electronic energy scales (eg. CF & SO)
Interactions (eg. spin-phonon coupling)
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Spin waves
NXS School 21
Perring et al., Phys. Rev. Lett. 77, 711 (1996).
Ferromagnetic
Shapiro et al., Phys. Rev. B 10, 2014 (1974).
Antiferromagnetic
Ferrimagnetic
McQueeney et al., Phys. Rev. Lett. 99, 246401 (2007).
Fe3O4
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22
Scattering experiments Single-crystal
Instrument and sample (powder or single-crystal) determine how (Q,) space is sampled
Powder S(|Q|,)
NXS School
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Bragg’s Law: n = 2d sin()
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Bragg’s Law: n = 2d sin()
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| ki | = 2 / i
| kf | = 2 / f
Brockhouse’s Triple Axis Spectrometer
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Momentum Transfer: Q = ki – kf
kf
- kf
ki
Q
Energy Transfer: E = h2/2m (ki
2 – kf2)
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Two Axis Spectrometer: • 3-axis with analyser removed
• Powder diffractometer • Small angle diffractometer • Reflectometers
Diffractometers often employ working assumption that all scattering
is elastic.
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Soller Slits: Collimators Define beam direction to +/- 0.5, 0.75 etc. degrees
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Filters: Remove /n from incident or scattered beam, or both
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n = 2d sin() Get: , /2 , /3 , etc.
Single crystal monochromators: Bragg reflection and harmonic contamination
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Pyrolitic graphite filter:
E = 14.7 meV = 2.37 A v = 1.6 km/s 2 x v = 3.2 km/s 3 x v = 4.8 km/s
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Constant kf Constant ki
Two different ways of performing constant-Q scans
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2 / a
2 / a
Origin of reciprocal space; Remains fixed for any sample rotation
Mapping Momentum – Energy (Q-E) space
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Elementary Excitations in Solids
• Lattice Vibrations (Phonons) • Spin Fluctuations (Magnons)
Energy vs Momentum • Forces which bind atoms together in solids
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Constant Q, Constant E 3-axis technique allow us to Put Q-Energy space on a grid, And scan through as we wish
Map out elementary excitations In Q-energy space (dispersion Surface)
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Samples • Samples need to be BIG
– ~ gram or cc – Counting times are long (mins/pt)
• Sample rotation • Sample tilt
May 31, 2009 NXS School 38
HB3-HFIR
IN14-ILL
Co-aligned CaFe2As2 crystals
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Monochromators
• Selects the incident wavevector
• Reflectivity
• focusing
• high-order contamination eg./2 PG(004)
l
Q(hkl) 2
d(hkl) 2ki sin
Q(hkl)
Mono d(hkl) uses
PG(002) 3.353 General
Be(002) 1.790 High ki
Si(111) 3.135 No/2
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Detectors
• Gas Detectors
• n + 3He 3H + p + 0.764 MeV
• Ionization of gas
• e- drift to high voltage anode
• High efficiency
• Beam monitors
• Low efficiency detectors for measuring beam flux
NXS School 40
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Resolution
• Resolution ellipsoid – Beam divergences
– Collimations/distances
– Crystal mosaics/sizes/angles
• Resolution convolutions
NXS School 41
I(Q0,0) = S(Q0,0) R(QQ0, 0)dQd
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Resolution focusing
• Optimizing peak intensity
• Match slope of resolution to dispersion
May 31, 2009 NXS School 42
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Neutrons have mass so higher energy means faster – lower energy means slower
We can measure a neutron’s energy, wavelength by measuring its speed
v (km/sec) = 3.96 / (A) • 4 A neutrons move at ~ 1 km/sec • DCS: 4 m from sample to detector • It takes 4 msec for elastically scattered 4 A neutrons to travel 4 m • msec timing of neutrons is easy • E / E ~ 1-3 % - very good !
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Time-of-flight methods
NXS School 44
velocity selector
sample
detector banks
Scattered neutrons
Spallation neutron source Pharos – Lujan Center
Effectively utilizes time structure of pulsed neutron groups
t d
v
m
hd
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Fermi Choppers
• Body radius ~ 5 cm
• Curved absorbing slats – B or Gd coated
– ~mm slit size
• f = 600 Hz (max)
• Acts like shutter, Dt ~ s
NXS School 48
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T-zero chopper
• Background suppression
• Blocks fast neutron flash
NXS School 49
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Position sensitive detectors
• 3He tubes (usu. 1 meter)
• Charge division
• Position resolution ~ cm
• Time resolution ~ 10 ns
NXS School 50
MAPS detector bank
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Sample environment
• Temperature, field, pressure
• Heavy duty for large sample environment
– CCR
– He cryostats
– SC magnets
– …
• Can be machined from Al
~ neutron transparent
relatively easy to work with
May 31, 2009 NXS School 51
HB3-HFIR
IN14-ILL
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Guides
• Transport beam over long distances
• Background reduction
• Total external reflection
– Ni coated glass
– Ni/Ti multilayers (supermirror)
NXS School 52
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Size matters
• Length = resolution
– Instruments ~ 20 – 40 m long
– E-resolution ~ 2-4% Ei
• More detectors – SEQUOIA – 1600 tubes, 144000 pixels
– Solid angle coverage 1.6 steradians
• Huge data sets
• 0.1 – 1 GB
NXS School 53
SEQUOIA detector vacuum vessel
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Kinematic limitations • Many combinations of ki,kf for same Q,
– Only certain configurations are used (eg. Ef-fixed)
• Cannot “close triangle” for certain Q,due to kinematics
May 31, 2009 NXS School 54 Kinematic limits, Ei=160 meV
ki
kf
Q
ki kf
Q
Minimum accessible Q
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Data visualization
• Large, complex data from spallation sources • Measure S(Q,) – 4D function
Ye et al., Phys. Rev. B, 75 144408 (2007).
La1-xCaxMnO3
NXS School
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Field-induced order in the Pyrochlore Yb2Ti2O7: Weak magnetic field // [110] induces LRO
appearance of long-lived spin waves at low T and moderate H
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References
NXS School 57
General neutron scattering G. Squires, “Intro to theory of thermal neutron scattering”, Dover, 1978. S. Lovesey, “Theory of neutron scattering from condensed matter”, Oxford, 1984. R. Pynn, http://www.mrl.ucsb.edu/~pynn/.
Polarized neutron scattering Moon, Koehler, Riste, Phys. Rev 181, 920 (1969).
Triple-axis techniques Shirane, Shapiro, Tranquada, “Neutron scattering with a triple-axis spectrometer”, Cambridge, 2002.
Time-of-flight techniques B. Fultz, http://www.cacr.caltech.edu/projects/danse/ARCS_Book_16x.pdf