1
1961 – 1968 IBR-1 (1 – 6 kW)
1969 – 1980 IBR-30 (15 kW)
1981 – 1983 IBR-2 (100 – 1000 kW)
1984 – 2004 IBR-2 (1500 – 2000 kW)
tit
Neutron scattering in condensed matter research.
20 years of regular studies at the IBR-2 pulsed reactor.
Anatoly M. BalagurovCondensed Matter Department of Frank Laboratory of Neutron Physics, JINR
21st-sp
Diffraction TOF patterns: in the past and at present.
Si diffraction pattern, measured at the IBR-1. 1965.
Si diffraction pattern, measured at the IBR-2. 1994.
3Tem
Time-of-Flight (TOF) technique at pulsed neutron source
Alternatives:
Steady state source (reactor) W = 10 – 100 MW, const in time.
Pulsed source (reactor / accelerator) W = 10 – 2000 kW, pulses in time.
These two types are generally considered to be complimentary!
At pulsed neutron source TOF technique is used in a natural way!
Neutrons are separated in energy after traveling over a fixed path (L), permitting neutrons of many different energies and wavelengths to be used for experiments.
Fli
ght
pat
h
Source pulse Time
Low energyHigh energy
4IBR-2
Activecore
IBR-2 pulsed reactor (1984 – present)
The IBR-2 parameters
Fuel PuO2
Active core volume 22 l
Cooling liquid Na
Average power 2 МW
Pulsed power 1500 MW
Repetition rate 5 s-1
Average flux 8·1012 n/cm2/s
Pulsed flux 5·1015 n/сm2/s
Pulse width (fast / therm.) 215 / 320 μs
Number of channels 14
Movable reflector
5Diffr.-IBR2
The IBR-2 pulsed reactor for condensed matter research.Comparison with other pulsed sources.
Source
Parameter
IBR-30
JINR
IBR-2
JINR
ISIS
RAL, UK
SNS
ORNL, USA
Status 1969-80 1984 1986 2006
Power,
kW15 2000 160 1200
Pulse width,
μs120 320 20 20
Frequency,
s-15 5 50 60
6Diffr.-IBR2
The IBR-2 pulsed reactor for condensed matter research.Comparison with other pulsed sources.
Intensity / Counting rate
I ≈ Φ0 · S · Ω/4π [n/s] ≥ 106 n/s
DN-2, IBR-2: Ω ≈ 0.2 sr
GEM, ISIS: Ω ≈ 6.0 sr
Φ0 – neutron flux at a sample, 107 n/cm2/s
S – sample area, 5 cm2
Ω – detector solid angle, 0.2 sr
7Diffr.-IBR2
The IBR-2 pulsed reactor for condensed matter research.Comparison with other pulsed sources.
R = [(Δt0/t)2 + (Δ/tg)2]1/2
Resolution
Δt0 – pulse width,
Δ - geometrical uncertainties,
t ~ L · λ – total flight time,
– Bragg angle.
IBR-2: Δt0 ≈ 320 μs.
ISIS: Δt0 ≈ 20 μs.
TOF component in resolution function is not very important for:
SANS, reflectometry, single crystal diffraction, magnetic diffraction…
For high resolution experiment we use the Fourier technique !
R ≈ 0.01, DN-2.
R ≈ 0.003, GEM.
8chopper
High Resolution Fourier Diffractometer
0.7 mm
Rotor
Stator
Transmission function
Binary signals
Fourier chopper:N=1024
Vmax=9000 rpm
Ω = 150,000 s-1
Sbeam=3x30 cm2
0
R(t) R(t) ≈ g(ω)cos(ωt)dω,
Δt0≈ 1/Ω = (Nωm)-1 ≈ 7 μs
9HRFD
HRFD – High Resolution Fourier Diffractometer
at the IBR-2 pulsed reactor
In collaboration between: FLNP (Dubna), PNPI (Gatchina), VTT (Espoo), IzfP (Drezden)
IBR-2
Fourierchopper
10high-low
0 .7 1 .0 1 .3 1 .6 1 .9 2 .2 2 .5d , Å
Y 1 2 3 -C u /F eH ig h reso lu tio n0 .1 %
Y 1 2 3 -C u /F eL o w reso lu tio n1 %
cufe-h l
Diffraction patterns measured with high and low resolution
HRFDd/d0.001
DN-2d/d0.01
11HRPD-HRFD
Al2O3 standard measured at ISIS and IBR-2
For V=11,000 rpm & L=30 m
Rt=0.0002 (d=2 Å)
The utmost TOF resolution of HRFD
121st-sp
Diffraction TOF experiments with sapphire anvil high-
pressure cells (collaboration with “Kurchatov
Institute”)
Diffractometer DN-12 at the IBR-2
Sapphire anvil high-pressure high-pressure cell, Р up to 7 GPa (cylinder48 mm x 164 mm height).
13Mono-DKDP
2D cross-section of (400) spot of KD2PO4 single crystalmeasured by 1D PSD at T=80 K.
А.M. Balagurov, I.D. Dutt, B.N. Savenko and L.A. Shuvalov, 1980.
Simultaneous sweep
along TOF and 2 axes.
About 4000 points have
been measured in parallel.
TOF scale
2 scale
14real-time
Time / temperature scale: Tstart=94 K, Tend=275 K. The heating rate is ≈1 deg/min.
Diffraction patterns have been measured each 5 min. Phase VIII is transformed into high density amorphous phase hda, then into cubic phase Ic, and then into hexagonal ice Ih.
Ice VIII
Ic
Ih
Phase transformations of high pressure heavy ice VIII.Time-resolved experiment with t=5 min.
hda
TOF scale
Time & temperature scale
15spn
V. Lauter-Pasyuk, H. Lauter, B. Toperverg et al., 1999.
Magnetic off-specular neutron scattering from (001)
[Cr(12Å)/57Fe(68Å)]x12 /Al2O3 multilayer
Intensity map of specular and off-specular scattered neutrons from the Fe/Cr multilayer (SPN data).
Result of the supermatrix calculations with the model of non-collinear domains.
Neutron wavelength, Å Neutron wavelength, Å
16prem
Development and realization of new methods
in time-of-flight neutron diffraction studies
at pulsed and steady state nuclear reactors
State Prize of the Russian Federation in 2000
FLNP, JINRVictor L. Aksenov
Anatoly M. Balagurov
Vladimir V. Nietz
Yuri M. Ostanevich
RRC KI, MoscowVictor P. Glazkov
Victor A. Somenkov
PNPI RAS, GatchinaValery A. Kudryashev
Vitaly A. Trounov
17
Condensed Matter Department at FLNP
tit
Permanent staff 45Directorate staff 22Ph.D. + students 13
Doctor of science 7
Candidate of science 26
Main goals: Research at the actual fields of condensed matter science and technology. Assistance to external users at the IBR-2 spectrometers. Operation of spectrometers at the IBR-2 and their further development.
10
14
8
4
9 9
7
10
6
3
0
2
4
6
8
10
12
14
16
18
20
20-24 25-29 30-34 35-39 40-44 45-49 50-54 55-59 60-64 65-70
Age distributionA new goal: Realization of education program
for young scientists.
18IBR-2
Spectrometers at the IBR-2 reactor
HRFDDN-2TEST
SKATEPSILONNERA
DN-12FSDIZOMER (NP)
YuMO DIN
KDSOG
REFLEX
REMUR(SPN)
KOLHIDA (NP)
Main experimental
techniques at IBR-2: Neutron diffraction: 7 SANS: 2 Reflectometry: 2 INS: 3
19Tem
Main research topics
Atomic and magnetic structure of new materials.HRFD, DN-2
Atomic and magnetic dynamics.DIN, NERA, KDSOG
Non-crystalline materials, liquids, polymers, colloidal solutions.YuMO
Surfaces, nanostructures of low dimension.REMUR, REFLEX
Biological materials and macro-molecules.YuMO
High pressure physics.DN-12, DN-2
Internal stresses in industrial materials and components.HRFD, FSD
Texture and properties of rocks.SKAT, EPSILON
20Rietv
Rietveld refinement of HgBa2CuO4.12 structure; IBR-2, HRFD
H g -1 2 0 1n (O 3 )= 0 .1 2
0 .8 1 .0 1 .2 1 .4 1 .6 1 .8 2 .0d , Å
Nor
mal
ized
inte
nsit
y
- 505
hg5f-c
0 .8 0 .9 1 .0 1 .1
Mercury based high-Tc superconductors.
Collaboration FLNP – MSU (Moscow)
21Hg-Tc
The temperature of SC phase transition at HgBa2Cu(O/F)4+
as a function of oxygen / fluorine content
Тhe temperature of phase transition depends on charge!
22Hg-F-dist.
Interatomic (apical) distances in HgBa2CuO4(O/F)
Apical distances depend on the amount of anions!
From: A.M. Abakumov et al.,PRL 80 (1998) 385.
23cmr
Colossal_Magneto_Resistivity (CMR) – effect in
T1-xDxMnO3 manganites, T = La, Pr, D = Ca, Sr.
Electrical resistivity decreases in 107 times under the influence
of magnetic field!
24
(La0.25Pr0.75)0.7Ca0.3MnO3, isotope enriched:
18O, 75% (O-18) insulating down to 4 K 16O, 99.7% (O-16) metallic at T<100 K
LPCM/Samples
0 .8 1 .0 1 .2 1 .4 1 .6 1 .8 2 .0 2 .2 2 .4 2 .6 2 .8d , Å
Nor
mal
ized
neu
tron
cou
nts
-505
0.8 0.9 1.0 1.1 1.2 1.3 1.4
(L a 0 .2 5P r 0 .7 5)0 .7C a 0 .3M n O 3 , O -1 8la-o18c
H R F DT = 2 9 3 K
6 0 8 0 1 0 0 1 2 0 1 4 0 1 6 0 1 8 0T em p era tu re , K
1 E + 1
1 E + 2
1 E + 3
1 E + 4
1 E + 5
1 E + 6
1 E + 7
1 E + 8
cm)
resis-c
O -1 8
O -1 6
(L a 0 .2 5P r 0 .7 5)0 .7C a 0 .3M n O 3
Giant oxygen isotope effect in (La0.25Pr0.75)0.7Ca0.3MnO3 (LPCM-
75)
N.A. Babushkina et al., Nature 391 (1998) 159
25
7 .6 7 5
7 .6 8 0
7 .6 8 5
7 .6 9 0
7 .6 9 5
Latt
ice
para
met
ers
(Å)
b-75c
b '
T C OT A F MT F M
O -1 6
O -1 8
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0T emperature (K)
5 .4 3 5
5 .4 4 0
5 .4 4 5
5 .4 5 0
5 .4 5 5
5 .4 6 0
Latt
ice
para
met
ers
(Å)
a
c
O -1 6
ac-75c
O -1 6
O -1 8
/ O -1 8
Temperature dependencies of lattice parameters a and c (bottom) and b (top) for the O-16 and O-18 samples. The vertical lines mark the temperatures of CO, AFM, and FM transitions. Between TFM and room temperature the parameters of both samples are coincide.
(La0.25Pr0.75)0.7Ca0.3MnO3,
16O / 18O (O-16 / O-18)
16O / 18O – Latt. Param.
Giant oxygen isotope effect in (LPCM-75). Lattice parameters.
26
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0
1 5 6 .0
1 5 6 .5
1 5 7 .0
1 5 7 .5
1 5 8 .0<
Mn-
O-M
n> (
degr
.)
O -1 8
angsr-c
O -1 6
T F M (O -1 6 )
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0T em p era tu re (K )
1 .9 5 5
1 .9 6 0
1 .9 6 5
1 .9 7 0
<M
n -
O>
(Å
)
mno1-c
O -1 8
O -1 6T F M (O -1 6 )
Interatomic distances and
valent angles changes after
oxygen isotope (16O→18O)
exchange in LPCM-75.
16O / 18O
Giant oxygen isotope effect in (LPCM-75). Structural
parameters.
27shema
Diffraction experiment for
measuring of internal stresses
inside material or component:
• highly accurate,
• completely nondestructive,
• multi-phase materials,
• in situ mode.
incident neutron beam
diaphragm
component(sample)
By two detectors at detectors at 90 one can measure stresses in both Q1 and Q2 directions simultaneously.
gauge volume
Neutron diffraction: an effective, nondestructive technique
for determining residual stresses (applied research).
28Tar-1
Stress rig on neutron beam Tensile grip design
Typical shape and size of a sample
Loading device “TIRAtest”
29adapter
Residual stresses in bimetallic steel-zirconium adapter
Cross-section of bimetallic adapterwall
Bimetallic adapter placed at HRFD
steel Zr
30Karta-1
The diffraction (111) peak width distributionfor steel region.
Axial deformation map for steel region.The first zirconium screw tooth: Y=0; X=5.
Residual stresses in bimetallic steel-zirconium adapter
31Tem
Condensed Matter Division & IBR-2:
Last 5 years Ph.D. thesis.
1. V.V. Luzin “Texture in bulk samples: experimental and model investigation”
NSVR & SKAT, 1999.
2. V.Yu. Kazimirov “New ferroelectrics – ferroelastics (CH3)2NH2Al(SO4)26H2O”
NERA, 1999.
3. О.V. Sobolev “Inelastic neutron scattering by water solutions and micro-dynamics
of hydration” DIN, 2000.
4. А.N. Skomorokhov “Phonon-maxon area in excitation spectra of liquid helium”
DIN, 2000.
5. D.V. Sheptyakov “Structural peculiarities of complex copper oxides
superconductors” HRFD & DN-12, 2000.
6. D.P. Kozlenko “Structure and dynamics of ammonium halides”
DN-12, 2001.
32Tem
7. Т.А. Lychagina “Texture and elastic properties of materials: neutron diffraction
studies” SKAT, 2002.
8. S.V. Kozhevnikov “Effect of spatial splitting of polarized neutron beam:
investigation and application” SPN, 2002.
9. G.D. Bokuchva “Neutron diffraction studies of internal stresses in bulk materials”
HRFD, 2002.
10. D.Е. Burilichiev “Texture and elastic anisotropy of earth mantle rocks
at high pressure” SKAT, 2002.
11. М.V. Avdeev “The investigation of the fractal properties of global proteins
surface” YuMO, 2002.
12. V.I. Bodnarchuk “Interaction of polarized neutrons with non-collinear
magnetic structures” REFLEX, 2003.
13. А.Kh. Islamov “Structure and properties of lipid membranes: neutron
diffraction studies” DN-2, YuMO, 2003.
Condensed Matter Division & IBR-2: Last 5 years Ph.D. thesis.
33User-Pr
User program at the IBR-2 spectrometers
Experts’ commissions
Diffraction:H. Tietze-Jaensh, GermanyP. Mikula, Czech Rep.V.A. Somenkov, Russia
Inelastic Scatt.:P. Alexeev, RussiaW. Zajak, PolandI. Padureanu, Romania
Neutron optics:H. Lauter, FranceD.I. Nagy, HungaryA.I. Okorokov, Russia
SANS:G. Pepy, FranceA.N. Ozerin, RussiaJ. Pleshtil, Czech. Rep.J. Teixeira, France
Time-sharing (14 spectrometers)
FLNP (35%)
Externalregular (55%)
Externalfast (10%)
User statistics
FLNP, 25%
Germany, 17%
Russia, 31%
Poland, 5%
France, 3%
Others, 19%
34Tem
Conclusions
Neutron scattering at the IBR-2 has the excellent present
and good prospect for future because:
IBR-2 is one of the best neutron sources for condensed matter studies;
Parameters and performance of neutron spectrometers at the IBR-2
are at a world top level;
There exists a realistic program for development of spectrometers;
The staff is well experienced and there is a good balance between
aged and young scientists;
There exists a good collaboration with many Institutions.
35
END
36Tem
Our problems
1. Neutron guide tubes. 2. Detectors.
DN-12 diffractometer: intensity gain-factor after installation of a neutron guide tube.
Multi-element back-scattering detector for FSD diffractometer.
37Tem
The first steps of TOF neutron scattering
for condensed matter research in FLNP (1963 – 1980)
The first TOF diffraction patterns obtained at a pulsed neutron source
(Buras, Nietz, Sosnovska, 1963).
Inverted geometry for inelastic scattering (Bajorek, 1964).
Geometrical focusing in TOF diffraction (Holas, 1966).
Diffraction and inelastic scattering with pulsed magnetic field (Nietz, 1968).
Comb-like neutron moderator (Nazarov, 1972).
The first TOF structural experiment (Balagurov, 1975).
The first TOF SANS (small-angle) experiment (Ostanevich, 1975).
Correlation spectrometry at pulsed neutron source (Kroo, 1975).
The first 2D & 3D TOF diffraction patterns (Balagurov, 1977, 1980).
Axial geometry for SANS (Ostanevich, 1978).
Spin-flipper with extended working area (Korneev, 1979).
38Tem
Development of TOF technique for condensed matter research
at the IBR-2 in 1981 – 2003
The first mirror polarizer for TOF spectrometer (Korneev, 1981).
Neutron guide tubes for pulsed neutron source (Nazarov, 1982).
Axial geometry for SANS (Ostanevich, 1982).
The first real-time TOF experiments with ts1 min. (Mironova, 1985).
Fourier-diffractometer at pulsed neutron source
(Aksenov, Balagurov, Trounov, Hiismaki, 1992).
The first TOF experiments with sapphire-anvil high pressure cell
(Somenkov, Savenko, 1993).
Inelastic scattering experiments at TOF reflectometer (Korneev, 1995).
Combined electronic & geometrical focusing (Kuzmin, 2001).
39Diffr.-IBR2
The most important parameters of a pulsed sourcefor neutron scattering experiment
Resolution
IntensityAverage power
SpectrometerPulsed source
Pulse width
Experiment
Duration
Quality of data
What does it mean for the IBR-2 ?
40Diffr.-IBR2
Diffractometers at the IBR-2
1. HRFD – high resolution Fourier diffractometercrystal structure of powders
2. DN-2 – multi-purpose diffractometersingle crystals, magnetic structures, real-time studies
3. DN-12 – diffractometer for microsampleshigh pressure experiments
4. FSD / EPSILON – stress diffractometersinternal stresses in bulk samples
5. SKAT / NSVR – texture diffractometers texture of rocks and bulk samples
41izluch
Radiations for diffraction studies of internal stresses
Radiation Accessibility Resolution Resolution Scanning Experiment over d over x depth geometry
-----------------------------------------------------------------------------------------------------------------X-ray +++++ +++ +++ + +++
Synchrotron ++ +++++ +++++ +++ ++radiation
Neutron ++ ++ + +++++ +++++-----------------------------------------------------------------------------------------------
With TOF neutron diffractometer (pulsed neutron source) determination of stress anisotropy is possible! up to 3 cm in steel,
6 cm in Al
42sdvig
Peak shift for E=200 GPa and loading of 20 MPa and 200 MPa
Peak shift under loading for d/d ≈ 0.001