Neutron Scattering

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15 . Polymer Dynamics D. Richter 15.1 Introduction In our every day life plastics or polymers play a very important role . Polymeric materials are used, because they are durable, cheaply to produce, easily to process and because they exhibit very versatile and favorable mechanical properties, e .g . depending on temperature or time the same polymer may be viscose, rubber elastic, very tough with high impact strength or even brittle . In the simplest case polymers are long linear chain molecules, build from one repeating unit, the monomer ; such polymers are called linear homopolymers . Since in gerreral rotational isomers may be easily formed at each bond of the chain backbone, long chain polymers possess a very large number of irrternal degrees of freedora which contribute importantly to the entropic part of the molecules free energy . At length scales somewhat larger than the size of the monomer, the detailed chemical structure of the chain building blocks ceases to be of importance and very general properties determined by the statistical mechanics of the chains prevail, e .g . the conformational entropy follows from the number of possible arrangements of a chain sequence in space . According to the central lirait theorem the most probable arrangement is that of a Gaussian coil, e .g . the polymer chain performs a rarrdom walk in space . If pieces of the chain are now stretched an errtropic force arises and acts on these stretched segments endeavouring to restore them to the most probable contorted state . Such forces are the basis ofrubber elasticity . This lecture aims to identify general principles of chain motion on a molecular scale which underlie the macroscopic mechanical properties, and presents concepts and experimental results on these motional mechanisms in space and time . Thereby, we restrict ourselves to melts ofhoraopolymers . <strong>Neutron</strong> scattering with its space time sensitivity on a molecular and atomic scale unravels the details of the molecular motions in question . Commencing at the scale of the single bond, where movements take place at a pace as in normal liquids, quasielastic neutron scattering (QENS) provides insight into local relaxation processes . At longer length scales first the entropy driven Rouse motion and at even larger distances the effect of entanglement 15-1
constraints due to the mutual interpenetration ofchains comes into the observation range. The most powerful technique suitable for these investigations, the neutron spin echo spectroscopy (NSE) operates in the time domain and uncovers a time range from about 2ps to 200ns and accesses momentum transfers between 0.0lÂ -1 and 3A -1 . The second important high resolution technique is neutron backscattering providing an energy resolution of about 1 ~ueV and covering a Q-range 0.1
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Forschungszentrum Jülich in der He
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Forschungszentrum Jülich GmbH Inst
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Contents . . 1 Neutron Sources H .
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1 . Neutron Sources Harald Conrad 1
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d) f, = v a, , q - ti = P a, - 0 .3
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Period Example Flux (D [1013 1950-6
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In stage 1 the primary proton knock
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get as heat, the rest is transporte
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down power and stronger absorption
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Appendix Neutron Sources - an overv
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led remotely. It is rauch more conv
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2 . Properties of the neutron, elem
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In the 60's the ferst high flux rea
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Hot neutrons in reactors are obtain
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elated values for the FRJ-2 reactor
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2 .5 Scattering amplitude and cross
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(A+k2 ) yr = u(Z:) yr V( u~r)= z "
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_du _ mn \2 A2-~2z r2~ I(k' IVI k)I
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E ô ô x z w 0 z _w U N Figure 2 .
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scattering is observed with the ave
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For a spherical electron distributi
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A more thorough introduction to neu
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3 . Elastie Seattering from Many-Bo
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Q = Q = k2 + k2 - 2kk' cos2B (3 .3)
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3 .2 Fundamental Scattering Theory
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The meaning of (3 .l4) is immediate
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1 . e. in the second approximation,
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The saure problem will bc dealt wit
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ALQ) = Y-bfe'Q'-rB(r-(n .a+m .b+p»
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du LQ) = ALQJ2 = e'Q .A' . * -i e-
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Tab . 3.1 : The scattering lengths
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We note immediately that we should
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These magnetic structures can be un
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M1LQ)=Q-MQ)xQ M(Q)= IM (r)e i Q " d
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Orbital magnetic spin angular ,,- m
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aQ . r 3 àQ . N . QR . aQ .t k _ML
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Schweika Analysis Polarization W .
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ducing a complex component and were
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ir v s ftft 3956 2 s 2 0.81[X] 80 c
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Some polarizers using Bragg reflect
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Different to the coherent nuclear s
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where QBG denotes the background .
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4 .4 Applications We now consider e
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Fig. 4 .3 .4 probably represents th
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. occur only in the non-spin flip c
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The results for the magnetization d
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a large solid angle with polarizers
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scattering to spin-flip scattering
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An experimental verification of thi
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Correlation Functions Measured by S
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In real liquids however usually an
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The term in big parentheses of equa
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4 0 -5 0 5 10 15 20 ho) [meV] Figur
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Figure 5 .5 : The pair correlation
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Figure 5 .6 : Partial differential
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Then equation (5 .21) can be conver
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The route from expression (5 .27) t
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In addition it is often useful to d
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2 . The pair correlation function h
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G(r, t) G(r, t) i(Q, t) r Q i(Q, t)
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Insertion of this result into (5 .6
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With this example we can also demon
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6. Continuum description : Grazing
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Starting point is the exact atomic
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For specular reflectivity measureme
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v v z l 2r V(z) = 2 -2erfC~ with er
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F{dV(z)/dz ) to calculate the refle
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Equation (6 .13) also shows that th
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ut is completely reflected . The cr
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0.4° . The full dynamical theory c
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1) If no magnetic induction B (whic
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Diffractometer Gernot Heger
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select a special wavelengths band (
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" The direction of the reciprocal l
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Bragg-intensities of single crystal
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monochromator, on the mosaic spread
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complex sample environments, such a
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the diffraction plane) two further
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Small-angle Scattering and Reflecto
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L= (1) ( k ) a e -(k/k T ) 2 Ak (8
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possible neutron wave lengths betwe
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figure and with neutrons of about 1
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1 .0 Danvinkurve 0 .8 0 .6 0 .4 0 .
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tails. This reflection curve leads
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For the Nickel film one gets a thic
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I The rotor of a velocity selector
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multiplier are arranged in a quadra
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9 . Crystal spectrometer : triple-a
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machine which will be followed by a
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10 .3 Beaur shaping Due to the fact
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G.k=zGz . (11) This case is fulfill
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tribution of bisecting planes (ntos
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directions which is exploited for t
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Fig . 14) Dispersion surfaces for B
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whereby E and v,, denote energy and
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[1] B . N. Brockhouse, in Inelastic
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10 . Time-of-flight spectrometers M
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Tnloderator /K V7 2/m/s A/nm Aiw/eV
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10.2 .1 Interpretation of spectra A
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----~ Probe ' (Chopper 2) Zeit I Ch
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the similar intensity distribution
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is performed without Jacobian due t
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10.2 .6 Crystal monochromators The
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larger energy transfers . However i
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10.3 Inverted TOF-spectrometer In t
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constant offset to the TOF . To be
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sample size of cm and a detection p
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Contents 10 .1 Introduction . . . .
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11 . Neutron spin-echo spectrometer
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2 0 L Tr -0 L 2 ArDet Figure 11 .1
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initial velocity-reassemble at the
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distribution (current sheets) that
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esults, where il is an irrelevant c
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10000 - 8000 - co 6000 - C ô 4000-
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e0 oX n .5 1 .0 1 .5 so 0 .0 0 .0 1
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nel" coils) the required homogeneit
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Figure 11 .9 : S(Q, t)IS(Q) of a 2
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Contents 11 .1 Introduction . . . .
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12 . Structure determination G . He
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Important: Thc measured Bragg inten
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determination of accurate atomic pa
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The knowledge of the overall occupa
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(even anharmonic) effects. This com
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Fig . 4 . Coordination ofthe D20 mo
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fenoelectric phase of orthorhombic
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Page 274: 13 Inelastic Neutron Scattering Pho
Page 277 and 278: Figurel Schematical drawing of a ge
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Page 281 and 282: s - ' f N .mwn .I )oo K L .~um..un
Page 283 and 284: esults from the quantum mechanics o
Page 285 and 286: y absorption . 13 .1 .3 Magnetic in
Page 287 and 288: Figure 7 The plane in reciprocal sp
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Page 293 and 294: 16 14 12 F.. . 10 ô 8 q 6 cr 4 G.
Page 295 and 296: 21 [ooç 1 " - 19 18 17 16 "" 298 K
Page 297 and 298: n = v - cap[i(pga . - wt)] (13 .22)
Page 299 and 300: Y c 3 c Cc E Figure 16 Magnon dispe
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Page 308 and 309: 2 P(Q) = 1 ~exp(-Ii - j'6 Q2 ) (14
Page 310 and 311: fraction. In the region of large Q
Page 312 and 313: with the partial structure factor S
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Page 316 and 317: For the intramolecular and intermol
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Page 320 and 321: scaling behavior of the susceptibil
Page 322: 15 Polymer Dynamics Dieter Richter
Page 327 and 328: (15 .3) T ß ( E)=T ô exp E k,T -
Page 329 and 330: This incoherent approximation does
Page 331 and 332: 10 an 0 2 0 Figure 15.4 : Relaxatio
Page 333 and 334: In order to test Eq .[15 .9] the re
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Page 337 and 338: 1 3kBT ~ z 2 72 2 p2 a = f2 N2 P =W
Page 339 and 340: S (Q,t) = 12 fdu exp ~ -u_ (S2Rt) v
Page 341 and 342: We now use these data, in order to
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Page 365 and 366: Fie. 16.4: Scattering geometry for
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Page 369 and 370: Here, J;j denotes the exchange cons
Page 371 and 372: Fig. 16.8 : Contour plot of the mag
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0.0001 0.001 0 .01 0.1 2 Fig. 16 .1
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17 Translation and Rotation M . Pra
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17.1 Introduction Atomic and molecu
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17 .2.2 Diffusion, microscopic appr
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0.6 H20 2 x2tÄ z ) Figure 17 .2 :
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The scattering function of a polycr
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e (2) 1 (j 1, 0 > - 0,1 >), respect
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leads to the eigenvalue problem ~q
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allow a good determination of the E
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m Eu W Figure 17 .7 : Eigenenergies
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-so o so Energy transfer (NeV) Ener
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Bibliography [1] T. Springer, Quasi
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18 . Texture in Materials and Earth
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Further important structure related
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The axes of the cartesian Kp coordi
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4.0 Experimental Texture Analysis T
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Fig. 18.14: Variation of reflection
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measurements can be performed in tr
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Apart from the global description o
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In the following, two experimental
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The neutron diffraction pole figure
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dependent pole densities, and (4) g
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Schriften des Forschungszentrums J
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Forschungszentrum Jülich in der He
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Neutron Scattering

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