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Large dynamic range small-angle diffractometer D22

Small-angle scattering is a technique that measures the deviation to small angles (much less than one degree to several degrees) of an X-ray or neutron beam due to structures of small size in the sample. “Small” means dimensions of a few tenths to about 100 nanometres, such as clusters in alloys, polymers, or biological macromolecules.

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State of the Art

 D22 - State of the Art


Roland P. May Institut Max von Laue - Paul Langevin, F-38042 Grenoble Cedex 9

1. Introduction

1.1. Small-angle (neutron) scattering

SANS is produced by heterogeneities in matter (that can be as well defined as identical viruses in aqueous solution). If these are randomly oriented, every atom pair contributes a sin (Qd) / (Qd) term to the scattering of a sample, where d is the distance between the two atoms of the pair, and Q the momentum transfer, Q = (4π/λ) sin Θ, with 2Θ, the full scattering angle and λ, the wavelength.

Inhomogeneities of sizes larger than atomic distances (10 to 1000 Å) produce scattering patterns with interesting Q ranges 1/D < Q < 10/D, if D is the dimension of the inhomogeneities. The scattering angle 2Θ corresponding to the upper Q limit for D=100 Å is about 9.1 ° for neutrons of 10 Å wavelength.

In most cases, the sample and/or the sample environment are rather bulky. Therefore, SANS instruments usually have to be large themselves in order to yield the desired resolution. Small SANS instruments can only serve a very limited number of applications. For reasons of intensity, a relatively large beam divergence, i.e. a beam cross-section larger than the sample size is accepted as well as wavelength resolutions Δλ/λ of up to about 20 %.

1.2. Neutron properties

Discovered by Chadwick in 1932

Rest mass
mn = 1.6749543(86) x 10 -24 g
     = 1.008665012(37) u

Temperature dependence of the wavelength
λ(T) [nm] = h / (3m n kT)1/2 = 2.5159 / T1/2
λ(293 K) = 0.147 nm

Electric charge
q n = - (1.5 ± 2.2 ) x 10 -20 e

Life time
t = λ 1/2 / ln 2 = 925 ± 11 s

Magnetic moment
µn = -1.04187564(26) x 10 -3 µ B
     = -1.91304308(54) µN

Frequency
nn = 1.978x10 12 [s -1 ] / λ [nm]

Speed
v n = h / (m n λ) = 395.6 [m/s] / λ [nm]

Spin 1/2

Total reflection: Ultra-cold neutrons, neutron guides

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2. History

    1983: Proposal (R.P. May, R. Oberthür, P.A. Timmins and A.F.Wright)

    1987 (September): Final proposal (R.P. May, M. Thomas) endorsed by Instrument Subcommittee

    1989 (December): Delivery of detector tube and collimation by ABT (SIGRI)

    1992 (December): Delivery of detector by CERCA (after 24 months)

    1995 (February): First tests after reactor overhaul: first users in April

    1996 (April): Start of permanent operation after repair of detector

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3. Location

3.1. Guide Hall


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3.2. View of D22


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4. Features

4.1. Wavelength selection and collimation


"Classical" pin-hole small-angle scattering instrument
 

Wavelength selection

  • DORNIER velocity selector 25 cm long, 28 300 rpm, resolution 10% (fwhm), 4.6 < l < 42 Å for 0 ° tilt

Collimation system

  • guide cross-section 55 x 40 mm
  • 8 drums of lengths varying as a geometical series to yield free flight paths of 1.4 to 17.6 m
  •  three positions: guide in / apertures (/ optical elements)
  • 3 attenuators and 4 round apertures (5, 10, 20, 30 mm diameter), computer controlled
  • manually remotely controlled aperture at 19.1 m from sample

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4.2. Detector

  • 3He, 2 bars; sensitive surface: 0.96 m x 0.96 m
  • 16 K pixels of 0.75 x 0.75 cm
  • minimal distance 1.35 m, maximal distance 18 m
  • can be translated by half its width, i.e. 50 cm
  • can be rotated around its vertical axis (25 °)
  • Q-range: 0.7x10-3 Å-1< Q < 1 Å -1
    • Qmax/Qmin up to 50, typically 20 with offset, 10 without

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4.3. Sample position

  • table for mounting equipment in air, e.g. sample changer, shear apparatus
  • vessel ("cloche") for working in vacuum
  • electromagnets (1.4 T)
  • furnace (up to 1300 °C)
  • "orange" cryostats with support permitting direct-beam and reference measurements
  • remotely controlled heating/cooling bath (about -10 / +80 °C)

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4.4. Flux


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4.5. Sample zone and sample-preparation lab


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4.6. Cryostats and rack plate


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4.7. Robot

 A robot arm for manipulating radioactive (and other) samples


ISEL automation

ISEL automation

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5. Experiments

5.1. Proliferating Cell Nuclear Antigen (PCNA)

P. Schurtenberger et al. (1998) J. Mol. Biol. 275, 123-132

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5.2. The diffusion of oxygen in silicon single-crystals

S. Rycroft and R.J. Stewart (Univ. Reading)


The small-angle neutron-scattering from SiO2 precipitates in a single crystal of silicon which has been heat treated for 500 hours at 600°C; the neutron beam was incident along a <100> direction. The central cross arises from the cushion shaped SiO2 precipitates lying on (100) planes with their edges along <110> directions.

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5.3. Nucleation and growth studied by time-resolved SANS

Homogeneous nucleation and growth of oil droplets studied by time-resolved small-angle neutron-scattering

S.U. Egelhaaf (ILL), P. Schurtenberger (ETH Zürich), J. Morris, U. Olsson, H. Wennerström (Lund University)

 




Figure 1: Oligodisperse oil-in- water microemulsion droplets are quenched into a two phase area. At final equi- librium, smaller droplets coexist with an excess oil phase that nucleates at a few of the initial droplets which subsequently grow (t > 0), allowing the majority of droplets to decrease in size. This growth phase proceeds with a constant number of large drops (t >> 0).

Figure 2: Sequence of scattering curves from a time-resolved small-angle neutron-scattering experiment recorded during the nucleation and growth of an excess oil phase from oil-in-water microemulsion droplets. For clarity only every second measurement is shown. As an example the scattering curve obtained at t = 3150 s is added as an inset.

Figure 3: Time-dependence of the radius of gyration Rg,big  as obtained from a Guinier fit. Also shown is the power law behaviour expected for a classical Ostwald ripening process.



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5.3. The binding of GroEL and GroES (time-resolved SANS)

Jörg Holzinger and Roland May (ILL), Manfred Rößle, Elena Manakova and Hermann Heumann (MPI für Biochemie)

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5.5. He bubble growth in a fusion-reactor steel

 Helium Bubble Growth in a Martensitic Steel for Fusion Reactors

 




Fig. 1 (above): Transmission electron micrograph of He bubbles after implantation of 400 appm He at 250 °C (from the work of Bertsch, 1997).

Fig. 2: Nuclear plus magnetic cross sections of reference and implanted samples for 250 °C (full circles), 825 °C (empty circles), and 975 °C (squares).

Fig. 3: He-bubble volume distributions (a.u. proportional to bubble volume per unit volume vs. bubble size in Å) obtained from the data of Fig. 2: 250 °C (dotted), 825 ° C (dash-dot), and 975 °C (solid).

Our results complete the information available from TEM confirming that a uniform bubble distribution produced by low temperature implantation evolves into a bimodal one, with a population of large bubbles growing when the post-implantation annealing temperature is increased.

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6. Projects

Real-time SANS

  • The high flux allows us to perform real-time experiments
  •  A much faster detector is needed to work correctly at large Q

Polarization & polarization analysis

  • Polarized neutrons were used by Neumann et al.
  • Werner Heil is interested in developing a 3He spin filter

Spin contrast variation

  • Oliver Zimmer is adapting a polarized target station
  • A test experiment to look at the sizes and the time behaviour of polarized regions in polymers and proteins is planned

Time-of-flight SANS

  • Space for three chopper systems exists in the design of D22

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7. People

Design

Detector

Electronics

Hall d'essais

Mechanics

Neutron distribution

Organisation

Programming

Technicians

Klaus Gobrecht

John Hayter

Roland May

Radulf Oberthür

Peter Timmins

Michel Thomas

Werner Wagner

Albert Wright


Roger Chung

Michel Gamon

Bruno Guérard

Jean Jacobé

Anton Oed

André Rambaud

Jochen Uckelmann


Antony Burton

Frédéric Descamps

Reinhard Klesse

Jacques Munnier

Jacques Ratel

Franck Rey

J.-Antoine Vidal-Garcia


Claude Gomez

Marc Locatelli

Anthony Pascaud

Émile Stropiano

Pierre Thomas


Tony Billington

J.-François Carliez

Luc Didier

Guy Gobert

Michel Goursaud

Erwin Hetzler

Jacques Loppé

Philippe Malbert


Alain Beynet

Peter Suttling

Jean-Rémy Villard

Jean-Claude Faudou

Marie-Claude Filhol

Bernard Guérra

Walther Kaiser

Alain Barthélémy

Franck Cécillon

Ron Ghosh

Georges Messoumian

Didier Richard

Michel Roure

Helga Schwab

Odile Tillier

Klaus Wotschack

Michel Bonnaud

David Bowyer

Régis Gay

Pierre George

and many others...

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see also...

... the  D22 "Yellow Book" page (pdf) and the  D22 documentation.

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