measurement of atomic momentum distributions by high energy neutron scattering j mayers (isis)
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MEASUREMENT OF ATOMIC MOMENTUM DISTRIBUTIONS BY HIGH ENERGY NEUTRON SCATTERING J Mayers (ISIS) Lectures 1 and 2. How n(p) is measured The Impulse Approximation . Why high energy neutron scattering measures the momentum distribution n(p) of atoms. The VESUVIO instrument. - PowerPoint PPT PresentationTRANSCRIPT
MEASUREMENT OF ATOMIC MOMENTUM DISTRIBUTIONSBY HIGH ENERGY NEUTRON SCATTERING
J Mayers (ISIS)
Lectures 1 and 2. How n(p) is measured
The Impulse Approximation. Why high energy neutron scattering measures the momentum distribution n(p) of atoms.
The VESUVIO instrument.Time of flight measurements. Differencing methods to determine neutron energy and momentum transfersData correction; background, multiple scatteringFitting data to obtain sample composition, atomic kinetic energiesand momentum distributions.
Lectures 1 and 2. Why n(p) is measured
What we can we learn from measurements of n(p)(i) Lecture 3 n(p) in the presence of Bose-Einstein condensation.(ii)Lecture 4 Examples of measurements on protons.
1
2
The “Impulse Approximation” states that at sufficiently high incident neutron energy.(1) The neutron scatters from single atoms.(2) Kinetic energy and momentum are conserved in the collision.
M
q
q
My
2ˆ.
2
qp
M
p
M 22
)( 22
qpEnergy transfer
Mpi 2/2Initial Kinetic Energy
Mf 2/)( 2qp Final Kinetic Energy
Momentum transfer
Gives momentum componentalong q
3
The Impulse Approximation
pqp
pq dMM
pnS
2
)(
2)(),(
22
),(),,(
0
12
1
102
qSE
Eb
dEd
EEd
Kinetic energy and momentum are conserved
4
Why is scattering from a single atom?
If q >> 1/Δr interference effects between
different atoms average to zero.
Incoherent approximation is good for q such that;Liquids S(q) ~1 q >~10Å-1
Crystalline solids – q such that Debye Waller factor ~0.
. . . . . . ±Δr
5
Why is the incoherent S(q,ω) related to n(p)?
)()(),(2
EEANS ff
f qq
rrrqrq diA ff )().exp()()( *
E = Initial energy of particle
ω= energy transfer
Ef = Final energy of particle
q = wave vector transfer
Single particleIn a potential
6
)exp()( rkr ff iC
IA assumes final state of the struck atoms is a plane wave.
rrrqr diA ff )().exp()(*
ME f
f 2
22k
rrrkqr diCA ff )(]).(exp[)(*
2
].exp[)()( rrprp din
)(22
ff nCA kq
)2
()(),(2
Em
knS f
ff kqq
momentum distribution
8
qkp f
fdVf
kk
32
dpEM
nS
2
)()(),(
2qppq
p in Å-1 throughout - multiply by ħ to get momentum
9
E
MnS
2
)()(),(
2qppq
p
pqp
pq dM
p
MnS
22
)()(),(
22
Final stateis plane wave
Impulse Approximation
Difference due to “Initial State Effects”Neglect of potential energy in initial state.Neglect of quantum nature of initial state.
q→∞ gives identical expressions
10
Infinite Square well
rrrqr diA ff )().exp()(*
12
T=0
ER=q2/(2MED)
13
T=TD
ER=q2/(2MED)
14
Can be shown that (V. F. Sears Phys. Rev. B. 30, 44 (1984).
......)(
72
)(
36)()(
4
4
24
22
3
3
2
2
dy
yJd
q
FM
dy
yJd
q
VMyJyJ IAIA
IA
Thus FSE give further information on binding potential(but difficult to measure)
All deviations from IA are known as Final State Effectsin the literature.
15
Increasing q,ωDensity of States
16
FSE in Pyrolytic GraphiteA L Fielding,, J Mayers and D N Timms Europhys Lett 44 255 (1998)
Mean width of n(p) V2
17
q=40.8 Å-1
q=91.2 Å-1
FSE in ZrH2
18
Measurements of momentum distributions of atoms
Need q >> rms p
For protons rms value of p is 3-5 Å-1
q > 50 Å-1, ω > ~20 eV required
Only possible at pulsed sources such as ISIS UK, SNS USA
Short pulses ~1μsec at eV energies allow accurate measurement of energyand momentum transfers at eV energies.
Lecture 2
• How measurements are performed
L0
L1
v0
v1
θ
Source
Detector
Sample
1
1
0
0
v
L
v
Lt
Time of flight measurements
cos2 2122
21
2 kkkkq
0
0
mvk
10 EE
Time of flight neutron measurements
202
10 mvE
Wave vectortransfer
Energytransfer
1
1
0
0
v
L
v
Lt 1vFixed v0 (incident v)
(Direct Geometry)
1
1
0
0
v
L
v
Lt 0vFixed v1 (final v)
(Inverse Geometry)
1
1
mvk 2
121
1 mvE
22
The VESUVIO Inverse Geometry Instrument
23
VESUVIO INSTRUMENT
Foil out
Difference
Foil in
E M Schoonveld, J. Mayers et al Rev. Sci. Inst. 77 95103 (2006)
Foil cycling method
25
Cout=I0 A
C=Cout-Cin= I0 [ 1-A2]
Foil out
Cin=I0 (1-A)A
Foil in
26
Filter Difference Method
Cts = Foil out – foil in
6Lidetector
gold foil “in”
27
Blue = intrinsic width of lead peak
Black = measurement using Filter difference method
Red = foil cycling method
28
Foil cyclingFilter difference
YAP detectors give
Smaller resolution width
Better resolution peak shape
100 times less counts on filter in and filter out measurementsThus less detector saturation at short times
Similar count rates in the differenced spectra
Larger differences between foil in and foil out measurementstherefore more stability over time.
30
Energy Transfer (eV)
-20 0 200.0
0.2
0.4
0.6
0.8
1.0MARI
Ei=100 eV
MARIEi=40 eV
MARIEi=20 eV
VESUVIO
Comparison of chopper and resonance filter spectrometers at eV energiesC Stock, R A Cowley, J W Taylor and S. M. Bennington Phys Rev B 81, 024303 (2010)
31
Θ =62.5º
Θ =~160º
32
YAPdetector
PrimaryGold foil
Secondarygold foil “in”
Secondarygold foil "“out”
new
Gamma background
Pb
old Pb
33
YAPdetector
PrimaryGold foil
Secondarygold foil “in”
Secondarygold foil "“out” old
new
ZrH2
ZrH2
34
Need detectors on rings
Rotate secondary foils keeping the foil scattering angle constant
Should almost eliminate gamma background effects
35
Nearest
Furthest
corrections
for gamma
Background
Pb
36
corrections
for gamma
Background
ZrH2
37
p2n(p) without a background correction
with a background correction
ZrH2
38
Multiple Scattering
Total scattering
Multiple scattering
J. Mayers, A.L. Fielding and R. Senesi, Nucl. Inst. Methods A 481, 454 (2002)
39
Back scattering ZrH2
A=0.048. A=0.092, A=0.179, A=0.256.
Forward scattering ZrH2
Multiple Scattering
40
Forwardscattering
Backscattering
41
Correction for Gamma Background and Multiple Scattering
30 second input from user
Correction procedure runs in ~10 minutes
Automated procedure. Requires;
Sample+can transmission
Atomic Masses in sample + container
Correction determined by measured data
42
Uncorrected
Corrected
Data AnalysisImpulse Approximation implies kinetic energy and momentum are conserved in the collision between a neutron and a single atom.
M
q
q
M
2ˆ.
2
qpMomentum along q
M
p
M
qp
22
)( 22
Energy transfer
Mpi 2/2 Mqpf 2/)( 2
Initial Kinetic Energy Final Kinetic Energy
Momentum transfer
Y scaling
M
q
q
My
2ˆ.
2
qp
In the IA q and ω are no longer independent variables
Any scan in q,ω space which crosses the line ω=q2/(2M) gives the same information in isotropic samples
Detectors at all angles give the same information for isotropic samples
45
M
MM d
dEd
dNEDEI
L
E
mtC
1
2
100
2/30
2/1
)()(2
2)(
)(0
12
1
2
MMMM yJ
q
M
E
Eb
dEd
d
M
q
q
MyM 2
2
Data Analysis
2
2
2 2exp
2
1)(
M
M
M
MMw
y
wyJ
Strictly valid only if(1) Atom is bound by harmonic forces(2) Local potential is isotropic
Spectroscopy shows that both assumptions are well satisfied in ZrH2
Spectroscopy implies that wH is 4.16 ± 0.02 Å-1
VESUVIO measurements give
47
wtd mean width= 4.141140 +- 7.7802450E-03 mean width = 4.134780 st dev= 9.9052470E-03
48
WH
3356 Sep 2008 4.15
3912 Nov 2008 4.13
4062 Dec 2008 4.11
4188 May 2009 4.16
4642 Nov 2009 4.15
5026 Jul 2010 4.13
Expected ratio for ZrH1.98 is 1.98 x 81.67/6.56 =24.65
Mean value measured is 21.5 ± 0.2
Intensity shortfall in H peak of 12.7 ± 0.8%
AH/AZr
21.8
21.3
21.9
20.8
21.5
21.5
ZrH2 Calibrations
Momentum Distribution of proton
50
Sum of 48detectors atforward angles
M
q
q
My
2
2
y in Å-1
51
Sep 2008Dec 2008May 2009Nov 2009
Measured p2n(p) for ZrH2
Lecture 3.
What can we learn from a measurement
of the momentum distribution n(p).
Bose-Einstein condensation
53
Bose-Einstein CondensationT>TB 0<T<TB T~0
D. S. Durfee and W. Ketterle Optics Express 2, 299-313 (1998).
ħ/L
54
Kinetic energy of helium atoms. J. Mayers, F. Albergamo, D. Timms Physica B 276 (2000) 811
T.R. Sosnick, W.M SnowP.E. Sokol Phys Rev B 41 11185 (1989)
3.5K 0.35K
BEC in Liquid He4
f =0.07 ±0.01
55
Interference between separately prepared condensates
of ultra-cold atoms
Quantised vortices in 4He and ultra-cold trapped gases
http://cua.mit.edu/ketterle_group/
Macroscopic Quantum Effects
56
Superfluid helium becomesmore ordered as the temperatureIncreases. Why?
57
Line width of excitationsin superfluid helium is zero as T → 0. Why?
58
Basis of Lectures
J. Mayers J. Low. Temp. Phys 109 135 (1997) 109 153 (1997)
J. Mayers Phys. Rev. Lett. 80, 750 (1998) 84 314 (2000)
92 135302 (2004)
J. Mayers, Phys. Rev.B 64 224521, (2001) 74 014516, (2006)
J Mayers Phys Rev A 78 33618 (2008)
59
2
11212 ).exp(),..,(,..)( rrprrrrrp diddn NN
Quantum mechanical expression for n(p) in ground state
What are implications of presence of peak of width ħ/L for properties of Ψ?
1rr Nrrs ,..2
2
).exp(),()( rrpsrsp didnħ/L
Ground state wave function
60
)(/),()( ssrrS P
rsrs dP2
),()(
spsp S dnPn )()()(
23
3)/.exp()(
1)( rrprp SS din
61
2),( sr is pdf for N coordinates r,s
2)(rS is conditional pdf for r given N-1 coordinates s
1)(2
rrS d
ΨS(r) is “conditional wave function”
rsrs dP2
),()( is pdf for N-1 coordinates s
62
ħ/L
What are implications of presence of peak of width ħ/L for properties of ψS?
spsp S dnPn )()()(
23
3)/.exp()(
1)( rrprp SS din
Δp Δx ~ħ
ψS(r) must be delocalised over length scales ~L
Delocalized, BEC
Localized, No BEC
64
Feynman - Penrose - Onsager Model
Ψ(r1,r2, rN) = 0 if |rn-rm| < a a=hard core diameter of He atom
Ψ(r1,r2, rN) = C otherwise
65
f ~ 8%O. Penrose and L. Onsager Phys Rev 104 576 (1956)
J. Mayers PRL 84 314, (2000) PRB64 224521,(2001)
24 atoms
192atoms
Periodic boundary conditions.Line is Gaussian with same mean and standard deviation as simulation. rrS d)(
Has same value for allpossible s to within terms~1/√N
2)(1 rrSS d
Vf
f
f
N/1
Δf
66
Macroscopic Single Particle Quantum Behaviour (MSPQB)
N
nnN
121 )(),...,( rrrr
η(r) is non-zero over macroscopic length scales
Coarse grained average
)(
2
21)( 1
2
21 ),...,(..1
),...,(1 N
NNNN ddrr
rrrrrrrr
Smoothing operation – removes structure on length scales ofinter-atomic separation. Leaves long range structure.
Coarse Grained
average over r
Nfd /1~)()(
1)(
)(rrrr
r SS
volume Ω
containing
NΩ atoms
NFdFF /1~)()]([
1)]([
)(rrrr
r SS
)(
22)(
1)(
r SS rrr d
N/1~)()(22
rrS
2)()( rssr S dPN Density at r
N/1~)()(2
rr
)(
2
)( 21)(
1..
1r Sr
rrrrs dddPN
NN
)(
2
21)( 1 ),...,(..1
1 NNNN
ddrr
rrrrr
2)()( rssr S dPN Density at r
NddPN
NN/1~)(..
1)( 21
rrrsr
70
2
21 ),...,( Nrrr NP N /1~)()..( 12 rrr
N
nnN
1
2
21 )(),...,( rrrr
Provided only properties which are averages over regions of spacecontaining NΩ particles are considered |Ψ|2 factorizes to ~1/√NΩ
NP N /1~)()..,( 231 rrrr
NP N /1~)()..,,( 3421 rrrrr
71
)()()()()(
2 2
22
nn rrrr
r
r
nnneff
n
Vm
)]([)( rr effV
η(r) is macroscopic function. Hence MSPQB.
Quantised vortices, NCRI, macroscopic density oscillations.
2)()()]([ rrr cc
Weak interactions
Gross-PitaevskiEquation
)()(2
rr
Schrödinger Equation (Phys Rev A 78 33618 2008)
72
Depends only upon
(a) ψS(r) is delocalized function of r – must be so if BEC is present
(b) ψS(r) has random structure over macroscopic length scales – liquids and gases.
NOT TRUE IN ABSENCE OF BEC, WHEN ψS(r) IS LOCALIZED
Summary T=0
BEC implies ψS(r) is delocalized function of r non-zero over macroscopic length scales
Delocalization implies integrals of functionals of ψS(r) over volumescontaining NΩ atoms are the same for all s to within ~1/√N Ω
Hence BEC implies MSPQB
73
Finite T
At T=0 only ground state is occupied. Unique wave function Ψ0(r1,r2…rN)
At Finite T many occupied N particle states
Measured properties are average over occupied states
i
ii ETBTU )()(
)/exp()( TETB ii
NNiNii dddHE rrrrrrrrr ...)...,(ˆ)...,( 212121*
74
Delocalisation implies MSPQB
ψS(r) for occupied states cannot be delocalized at T=TB
Consider one such “typical” occupied state with wave function Ψ(r,s)
But typical occupied state is delocalized as T→0
MSPQB does not occur for T=TB
Typical occupied state Ψ(r,s) must change from localised to delocalised function as T is reduced below TB.
75
Delocalized Localized
),( rsD ),( rsL
),()(),()(),( rsrsrs LD TT
α(T) =1 at T=0 α(T) =0 at T=TB
76
)()()()()( rrr SSSSS LD TbTa
1)()()(222 rrrrrr SSS ddd LD
1)( TaS 0)( TaS0T BTT
)()( 0 rr SS D),(),( 0 rsrs D
(a) r space
(b) p space
VD ~)(~ pS
NVL /~)(pS
Vp /1~
VD /1~)(rS
VNL /~)(rS
NVr /~
Overlap region ~1/√N
V
(a) r space
p space
VN /~
VD ~)(~ pS~V~-V
NVL /~)(pS
Vp /1~
VD /1~)(rS
VN /~
NVr /~
Overlap region ~1/√N
N/V
79
CTdbdad LD )(
22
)(
22
)(
2)()()(
r SSr SSr S rrrrrr
CCdbaCT LD )(
** )()(r SSSS rrr
)(rSL Localised within )(rNd
CT
L
1~
)()(
2
r S rr
)(rSL Localised outside )(r 0CT
Contribution of CT is at most ~1/√N
Two fluid behaviour
ssrr S dPN )()()(2
NLD /1~)()()( rrr
Fluiddensity
)(
)(1
)(r
rrr d
NLD /1~)()()( rFrFrF
srrsrF SS dm
P )()()()(2
Fluidflow
Flow of delocalised component is quantised
No such requirement for flow of localised component
Localised component is superfluid
Delocalized component is normal fluid
),()(),()(),( rsrsrs LD TT
NTT LD /1~)()()()()(22 rrr
)()(2
TT S )()(2
TT N
Superfluid fraction Normal fluid fraction
More generally true that
in any integral of Ψ(r1,r2…rN) over (r1,r2…rN)
overlap between ΨD and ΨL is ~1/√N
E=ED +EL
n(p)=nD(p)+nL (p)
S(q,ω)=SD(q,ω)+SL(q,ω)
S(q)=SD(q)+SL(q)
84
)()()( rrr LNDS EEE
)()()( rrr LNDS PPP
J. Mayers Phys. Rev. Lett. 92 135302 (2004)
)0(
)(
T
85
)0()()( fTTf s
)0(
)(
f
Tf
Superfluid fractionJ. S. Brooks and R. J. Donnelly, J Phys. Chem. Ref. Data 6 51 (1977).
Normalised condensate fraction
o o T. R. Sosnick,W.M.Snow and P.E. Sokol Europhys Lett 9 707 (1989).x x H. R. Glyde, R.T. Azuah and W.G. Stirling Phys. Rev. B 62 14337 (2000).
J. Mayers Phys. Rev. Lett. 92 135302 (2004)
),(),( 0 rsrs D
86
More spaces give smaller pair correlations
)()()( 0 qqq LNS SSS
As T increases, superfluid fraction increases, pair correlations reduce
)()()( 0 qqq LNS SSS
1)(
1)()(
qS
qST
B
T
SB-1
ST -1
)]0(1)[(1)( TT S
α(T)
V.F. Sears and E.C. Svensson, Phys. Rev. Lett. 43 2009 (1979).
J. Mayers Phys. Rev. Lett. 92 135302 (2004)
α(0)
Lattice model
Fcc, bcc, sc all give same dependence on T as that observed
Only true if N/V and diameter d of He atoms is correct
Change in d by 10% is enough to destroy agreement
J. Mayers PRL 84 314, (2000) PRB64 224521,(2001)
Seems unlikely that this is a coincidence
90
)()(),(2
EEAS ff
f qq
srsrrqsrq ddiNA ff ),().exp(),()( *
),()(),()(),( 0 rsrsrs LTT
Identical particles
),(),(),( 0 qqq LNS SSS
Only S0 contributes to sharp peaks
91
Anderson and StirlingJ. Phys Cond Matt (1994)
92
New prediction
)()()( 0 rrr LNS
)(0 r Has density oscillations identical to gnd state
)(rL Has no density oscillations
Measure density oscillations close to gnd state
Measure superfluid fraction wD before release of traps
Simple prediction of visibility of density oscillations
Summary
Most important physical properties of BE condensedsystems can be understood quantitatively purely from the form of n(p)
Non classical rotational inertia – persistent flow
Quantised vortices
Interference fringes between overlapping condensates
Two fluid behaviour
Anomalous behaviour of S(q)
Anomalous behaviour of S(q,ω)
Amomalous behaviour of density
Lecture 4.
What can we learn from a measurement
of the momentum distribution n(p).
Quantum fluids and solids Protons
95
Measurement of flow without viscosity in solid helium
E. Kim and M. H. W. ChanScience 305 2004
96
can
He4
Focussed data Fitted widths on Individual detectors
97
liquid
O single crystal high purity He4 X polycrystal high purity He4□ 10ppm He3 polycrystal
solid
Focussed data after subtraction of can. Dotted line is resolution function
98
T (K) (101) (002) (100)
0.115 2.759 (7) 3.1055 (300) 0.400 2.759 (7) 3.1055 (300) 0.150 2.758 (7) 3.1056 (300) 0.070 2.758 (7) 3.1055 (300)
0.075 2.758 (2) 2.934 (4) 3.131 (2)
0.075 2.757 (3) 2.940(3) 3.128 (2)
Measured hcp lattice spacings
99
• No change in KE, no change in vacancy concentration through SS transition.
• Implies SS transition quite different to SF transition in liquid.
• Probably not BEC of atoms• What is cause??
100
3He mean kinetic energy, EK as a function of the molar volume: experimental values (solid circles), diffusion Monte- Carlo values (open circles).self-consistent phonon method (dashed line).
R. Senesi, C. Andreani, D. Colognesi, A. Cunsolo, M. Nardone,
Phys. Rev. Lett. 86 4584 (2001)
Kinetic Energy of He3
101101
n(p) is the “diffraction pattern” of the wave function
2
).exp()()( rrprp din
Measurements of protons
101n(p) in Å-1Position in Å
If n(p) is known ψ(r) can be reconstructed in a model independent way
In principle ψ(r) contains all the information which can be known about themicroscopic physical behaviour of protons on very short time scales.
pp
ppr
rp
rp
de
dMp
eVE
i
i
)(~
)(~2)(.
2.
rrp rp dei .)()(~
Potential can also be reconstructed
103
VESUVIO Measurements on Liquid H2
J Mayers (PRL 71 1553 (1993)
2
2
2
)(exp)(
Rr
Cr
2R
2
).exp()()( rdrpirpn
104
2
).exp()()( rdrpirpn
105
Puzzle
QM predicts R=bond length not ½ bond length
Fit to data givesR=0.36 σ=5.70
Spectroscopy givesR=0.37 σ=5.58
R should be 0.74!
106
Red data H2 1991Black YAP 2008
J(y)
p2n(p)
107
R=0.37R=0.74
108
Heavy Atoms
Single crystals
H
109
Reconstruction of Momentum Distribution from Neutron Compton Profile
mln
mllnmln qYyHay
yqJ,,
,2,,
2
)ˆ()()exp(
),ˆ(
Spherical HarmonicHermite polynomial
)ˆ()()1(!2exp(
)( 22/1,,
,,
22/3
2
pYpLpanp
pn lmln
lmln
n
mln
ln
Laguerre polynomial
an,l,m is Fitting coefficient
110
111
112
Nafion
113
114
115
116
In press PRL (2010)
Measurements of n(p) give unique information
on the quantum behaviour of protons in a wide
range of systems of fundamental importance