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The separation of coherent and incoherent Compton X-ray scattering

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BRIT. J. APPL. PHYS.,

1964, VOL. 15

The separation of coherent and incoherent Csmpton X-ray scattering

W. RULAND Union Carbide European Research Associates, sa., 95 rue Gatti de Gamond, Bruxelles 18, Belgium
MS. received 29th May 1964
Abstract. A theoretical and experimental study of the possibility of separating coherent and incoherent Compton x-ray scattering by monochromatization of the

scattered radiation is carried out. It is shown that this possibility depends on the profile of the Compton line as well as on the resolution of the monochromator. An approximate treatment of the problem is developed and an application to carbon and organic materials is given.
1. Introduction

X-ray studies of disorder and thermal motion involve an accurate determination of the diffusecoherent scattering. Using counter techniques, monochromatization of the scattered radiation can be carried out with relative ease which should, in principle, enable a separation of the coherent scattering from Compton and fluorescence scattering. The latter can generally be eliminated without difficulty; the elimination of the former, however, poses some problems which are due to the effect of the finite resolution of a monochromator and the width of the Compton line. The present report deals with the theoretical and practical aspects of these problems with special attention to carbon and organic materials.

2. Theoretical
The monochromatization of scattered radiation can be defined by

I(e) = J M(A)h(e, A) d/\

where I(0) is the intensity of the monochromatized scattering, h(0, A) the distribution of wavelengths scattered under the Bragg angle 0 and M(A) a distribution representing the pass-band\of the monochromator. If h(0, A) is given by the wavelength distribution of Compton scattering the elimination of this Scattering can be assessed by the attenuation O(8) defined bv

For Compton energies Ec large compared with the binding forces of the electrons in the irradiated material, the wavelength distribution is completely determined by the momentum distribution J(q) (DuMond 1933). These distributions have been calculated for a number of elements (Kirkpatrick, Ross and Ritland 1936, Hicks 1937, Duncanson and Coulson 1945, March 1954). The observed Compton profles (Burkhardt 1936, Kappeler 1936, Kirkpatrick, Ross and Ritland 1936) show that there are considerable differences between the proses of free and bound atoms. For the purpose of the present work, the DuMond approach is not strictly valid, since the basic condition for its applicability, high values of Ec, is in general not fidlilled in the range of 0 and A of interest in x-ray diffraction work. If EC is comparable with the binding forces of the electrons, the Compton profle is composed of a line spectrum (the ComptonRaman effect) and a continuous spectrum. This effect has been discussed by Schnaidt
1301

1302

W. Ruland

(1934), Sommerfeld (1937), Franz (1937) and recently by Das Gupta (1959). The line spectrum is due to discrete energy transitions below the ionization energy and is in principle equivalent to the &e structure of the x-ray absorption edges. In solids there is a number of low energy transition probabilities due to the band structure, which can produce Compton scattering of nearly the same wavelength as the coherent Scattering at small angles. This means that it is difficult to separate coherent and incoherent scattering at relatively small angles even with monochromators of high resolution. Since the calculation of the Compton profile for solids as well as its accurate determina. tion is rather difficult the following approximation is made for the evaluation of equation (1). For large values of Ec, the integral width of the Compton profde dq is a constant when the profile is taken as a function of q = - -c A 2 A, sin 0 where c is thevelocity of light (generally given in atomic units), A = A - Ac, Ac the average value of the Compton wavelength distribution and A, the incident wavelength. The integral width A h of the wavelength distribution is thus given by
Ah
=

A , sin 0

2 - Aq.
C

For smaller values of Ec, A q can be considered as a function of Ec, which means that it is a function of s = 2 sin O/ho since sin2 0 = Ec = 2h -s?. mc h,2 2mc One can thus write generally

We introduce furthermore the assumption that for the determination of Q (equation (1)) the Compton profile can be approximated by a unique type of distribution h which is centred on dhc, the Compton shift, and whose width is proportional to AA. This gives

if h is considered to be normalized. For a given wavelength of the incident beam and a given material, Q can thus be calculated as a function of s with the knowledge of dq(s), M(h) and Ahc.
3. Determination of the Compton prome

A Philips fluorescence spectrometer has been used for the determination of the Compton profde of graphite, diamond and some polymers. Since the scattering angle (defined by the positions of the focus, the sample and the analyser crystal) cannot be varied over a wide range, a series of different wavelengths for the incident beam have been used: chromium K,B and Ka tungsten La, gold La, molybdenum K,B and Ka. A typical recording is shown in figure 1. The advantage of the fluorescence spectrometer is a high intensity yield, the disadvantage is a low resolntion for the Compton profile due to the rather large divergence of the incident beam. It is thus not possible to observe the Compton-Raman effect, but taking the divergence into account by appropriate corrections for the integral width of the Compton profYe A&) values can be obtained with relatively high accuracy. An example is given in figure 2 which shows clearly that A q is not constant in the range of s generally occurring in x-ray diffraction work. A number of functions have been tested in an attempt

The separation of coherent and incoherent Compton x-ray scattering

1303

x [A,
Figure 1. Distribution of wavelength scattered under 0 = 47" with I., = 1.4763 A (WLa,) for polyethylene. Figure 3. Observed and calculated intensity difference between a Y and an Sr filter, l o = 0.7107 A, polyethylene.

Figure 2. Integral width dq of the Compton proae as function of s for polyethylene.

to approximate the results by an analytical expression. a constant for high values of s, a function of the type

Since A&)

should tend towards

Seems to be a reasonable approach. and a obtained by a least-squares fitting of such a function to the experiValues of dqmax mental data are given in the table together with some A h values.

1304 Sample
Diamond

W. RuIand

4
3.39 3.05 2.86 3.00 3.55

A A (e = 450)
>bo

2.0

1.542

= 0.711

(4

(4

Graphite Polyethylene hTylon6 Teflon

0.63 0.53 0.52 0.54

0.037 0.036 0.034 0.035

0.55

0.041

0.023 0.021 0.020 0.020 0.024

A comparison of the Aqmax values with the theoretical Aq values given by Duncanson and Coulson (1945) (carbon 1.57, fluorine 2.84) for free atoms shows the expected magnitude of the effect of the binding forces on the Compton proae. The results of the measurements with the spectrometer were checked with Woflans (1934) a t e r technique. Figure 3 shows a comparison of the observed and Calculated intensity difference between a Y and an Sr filter for M O K a as incident radiation using Aq(s) as given by equation ( 4 )and a Cauchy distribution to represent the Compton profile for the calculated curve. The filters were produced from the oxides embedded in polyethylene as already described (Ruland 1959). The thickness of the filters was chosen such that the pass-band defined by the difference of the absorption functions has a constant value between the Y and the Sr absorption edge and is effectivelyzero outside the edges. Except for a small shift in the position the two curves are very similar, which shows that the interpolation of the d q values as well as the approximation of the profile are consistent with the experiment. The differencein position is explained by the effect of the binding forces on the Compton shift as discussed by Ross and Kirkpatrick (1934) and Bloch (1934). If we consider this effect to be given by

we find a value of about 1 . 5 x as for D , which is to be compared with 1.63 x calculated by Bloch (1934) and 1 e48 x as measured by Ross and Kirkpatrick (1934) for carbon. Equation (5) is of course only valid for high Compton energies aild therefore not generally applicable in the h and 0 range used in x-ray diffraction. For copper radiation, for example, Dho2would have the value 0.0036 A and Ahc would become negative for 0 < 23if equation (5) is valid in this range of Compton energies. The validity of equation (5) can, however, be extended towards lower Compton energies with an approximation which correlates D to dq(s). One can assume Aq to be approxmately proportional t o the square root of the total binding energy of the electrons. The fact that Aq decreases with decreasing s can be explained by the decrease of that part of the binding energy which is involved in the Compton process; Aq as function of s is thus a measure of the effective binding energy for the Compton process. D is, after Ross and Kirkpatrick (1934) and BIoch (1934), to a first approximation proportional to the binding energy, which means that D(s) can be taken approximately as proportional to the square of A&). With this approach, negative values of Aqc are avoided and DA,2 becomes less important for longer wavelengths than would be expected if D were taken independent o f t

4. Determination of the pass-band function M The determination of the pass-band function M(h) has been carried out using a PUPS diffractometer with a flat topaz single crystal as analyser. A continuous wavelength distribution in the region of non-zero values for M(h) was produced by using the white radiation of a M O tube lo study M in the Cu region and a Cu tube for the MO region. The regions were measured with and without monochromatization ;the ratio of the former intensity to the latter yields M(h) directly after conversion from the 6 to the h scale. The resolution of the analyser crystal coaid be obtained from the width of the characteristic

The separation of coherent and incoherent Compton x-ray scattering

1305

fines of the impurities in the target material. Three types of monochromatization have been studied: flat Siilgle crystals in reflection position, Ross filters and pulse-height dis,imination. For the first type, a LiF and a pentaerythritol crystal have been chosen, for the second type Ni, CO and Fe filters for Cu radiation and Zr, Y and Sr iiIters for MO radiation have been produced from the oxides embedded in polyethylene. Pulse-height discrimination was studied with a xenon-filled proportional counter in the Cu region only.

A-A, (A!

L A , tAi

Figure 4. Pass-bands of a flat LiF monochromator crystal, (200) reflection.

Figure 5. Pass-bands of a flat pentaerythritol monochromator crystal, (002) reflection.

Figure 6. Pass-band of a Ni-Co filter set. (NO and Co,O, in polyethylene.)

Figure 7. Pass-bands related to channel widths (in v) for the discrimination of a pulse-height distribution from a xenon-Hled proportional counter. 1.54 A equals 50 v on the pulse-height scale.

Typical results are shown in figures 4, 5, 6 and I. A number of pass-band functions are obtained for a given crystal monochromator by varying the slit system. The relatively high yield of the flat-crystal monochromators ( e 1 5 %) is due to the small divergence of the beam diffracted by the analyser crystal. Under normal diffractoneter conditions the yield of the monochromators is much lower. The ripples on the pass-band functions for Ross filters are due to the h e structure of the absorption edges. Owing to the density fluctuations in the oxide filters the effective absorption is somewhat different from that for filters of uniform thickness. This effect lowers the optimum yield, but allows a better zero fit at both absorption edges.

1306

W. Ruland

5. Calculation of the attenuation function

Inspection of equation (3) shows that Q takes the form of a convolution of & f and h. It has been shown that h can be approximated by a distribution of the Cauchy type. por kfas given by crystal monochromators or narrow channels in pulse-height discrimination an approximation by a Cauchy distribution is also reasonable, whereas for Ross filters M can be approximated by a step function. If the integral width of M as expressed by a Cauchy distribution is b and its value for the incident wavelength is taken as unity, Q is given by

Since Ah and Ahc are both functions of A,, and s (equations (2) and ( 5 ) ) , Q can be CoEputerJ as function of s for any given A,. Figures 8 and 9 show Q functions calculated for polyethylene, Cu or MO radiation and a variety of b values.

Figure 8. Attenuation Q calculated as function o f s for 3.0 = 1.5418 A, Cauchy type Passbands (integral widths b) and polyethylene: ---- observed Q values for LiF monochromator; - . - . - observed Q values for pentaerythritol monochromator; . . . . . . . . . . observed Q values for pulse-height discrimination, 4 v channel.

Figure 9. Attenuation Q calculated as function o f s for j., = 0.7107 A, Cauchy type passbands (integral widths b) and polyethylene.

If M is a step function (Ross filters) and unity at A,

1
00 5: 0.
OSL

\\
05 10~r8-,15

Zr-Y

O 5 s&,

IO

20

25

Figure 10. Attenuation Q calculated as function of s for A. = 1.5418 A, Ni-Co and Ni-Fe filter sets, and polyethylene.

Figure 11. Attenuation Q calculated as function of s for i., = 0.7107 A, Zr-Y and Zr-Sr filter sets, and polyethylene.

The separation of coherent and incoherent Compton x-ray scattering

1307

where xc = ho A h and A x is the position of the absorption edge of the second filter. Figures 10 and 11 show calculations for polyethylene, Ni-Co and Ni-Fe iilter sets for CU radiation and Zr-Y and Zr-Sr filter sets for MO radiation.

6, Experimental check O f attenuation functions For a given monochromatization the ob( :ved scattering intensity is
Iobs =
n

f Q Iincoh)

where k is a normalization factor and Icoh and Iiocoh the normalized coherent and incoherent intensities. If the observed intensity is Il for one kind of monochromatization and I , for another, and kl and kz are the corresponding normalization factors, one finds

If is not expected to vary considerably in the region where Q, is non-zero, one can measure Ql by a comparison of normalized scattering intensities. This measurement has been carried out on scattering, monochromatized by flat LiF and pentaerythritol crystals, and pulse-height discrimination. The results are shown in figure 8 (broken lines). The results agree fairly well with the calculations; for the higher resolution (LiF, b U 0.007 A) the observed Q values are somewhat higher than the calculated ones.
7. Discussion The observed and calculated attenuation functions show the importance of the Compton profle for the separation of coherent and incoherent scattering. Although a complete separation is not possible crystal monochromators of high resolution can effectively attenuate the medium and wide angle Compton scattering. Since the correction for the remaining Compton scattering at smaller angles involves information on the Compton proae it will often be preferable to use a combination of ROSS filters and pulse-height discriminaticn, which are chosen such that the Compton scattering is not affected by the monochromatization, and to eliminate the Compton scattering by calculation.

el

Acknowledgments The author is indebted to Mr. J. M. Gilles for stimulating discussions during the course of this work and to Mr. J. P. Pauwels for technical assistance. Thanks are also due to Dr. J. L. de Vries and Mr. L. Caeymaex, N.V. Philips, Gloeilampenfabrieken, Eindhoven, for providing part of the work facilities. References
BLOCH,F., 1934, Phys. Rev., 46,674. BURKHARDT,G., 1936, Ann. Phys., Lpz., 26, 567. DASGUPTA,K., 1959, Phys. Rev. Letters, 3, 38. DUMOND, J. W. M., 1933, Rev. Mod. Phys., 5, 1. DUNCANSON, W. E., and COVLSON,C. A., 1945, Proc. Phys. Soc., 57, 190. FRANZ, W., 1937, Ann. Phys., Lpz., 29, 721. HrCKS, B., 19:7, Phys. Rev., 52, 436. ~ P E L E R H., , 1936, Ann. Phys., Lpz., 27, 129. K~~~~ATN P., cK Ross, , P. A., and -AND, H.O., 1936, Phys. Rev., 50, 928. MARCH,N. H., 1954, Proc. Phys. Soc., A67, 9. Ross, P. A,, and KIRKPATRICK,P., 1934, Phys. Rev., 46, 668. RULAND,W., 1959, Acta Cryst., 12, 679. SCHNPIDT, F., 1934, Ann. Phys., Lpz., 21, 89. SOMMERFELD, A., 1937, Ann. Phys., Lpz., 29,715. WOLLAN, E. O., 1934, Phys. Z., 35, 353.