Conclusion
In my thesis I have dealt with the theory of the X-ray reflectivity. I have applied it to the
study of the following types of multilayered samples:
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planar multilayers with various stacking sequences (single layer, periodic, quasiperiodic),
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rough multilayers, and
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multilayer gratings (multilayers with a lateral structure).
My aim was to develop and present several theories together using one unified formalism
while pointing out the links with the X-ray diffraction theories. The theories discussed are:
- the kinematical theory,
- the distorted-wave Born approximation,
- the dynamical theory, and
- various approximations of the dynamical theory (single-reflection
approximation, two-beam and multiple-beam approximations).
These theories have been compared by their analytical expressions as well as by numerical
simulations. I discussed their regions of good coincidence as well as their differences.
Further, I demonstrated the use of numerical simulations to fit measured data. This allowed
me to reveal structural parameters of the samples we analyzed in our laboratories.
The first part of the thesis has been devoted to the representation of scattering in reciprocal
space. Here, the relations between the angular movements during an experiment and the
appropriate scans in reciprocal space have been described. These formulae have
been applied by programming the motor movements of the goniometers for synchrotron
measurements.
Further I discussed the specular reflectivity from planar multilayers. Firstly, the kinematical
theory has been formulated. I calculated its diffraction integral by the stationary-phase method,
whose validity is not restricted to the first Fresnel zone contrary to the Fraunhofer approximation
mostly employed in calculating the kinematical treatments. Further, the usual dynamical theory
of reflectivity has been formulated, from which I derived the single-reflection approximation.
Dynamical and kinematical Fresnel coefficients have been compared.
The kinematical theory and the single-reflection approximations were successful especially for
the calculation of the reflectivity pattern of a quasiperiodic Fibonacci multilayer. By applying
the fundamental theorems from the physics of quasicrystals I have shown that the reflectivity
curve exhibits a self-similarity and two integers are needed to describe the peak positions.
Furthermore, specular and non-specular X-ray reflection from rough multilayers has been
discussed. The statistical properties of randomly rough interfaces have been employed in the
specular reflectivity from both the kinematical and dynamical theories. I applied the simulations
in fitting the experimental curves for sandwich multilayers and periodic multilayers. Further
diffuse scattering from rough multilayers has been briefly discussed and the distorted-wave Born
approximation (DWBA) employed for quantitative analysis. I presented the main features of
incoherent diffuse scattering on a measured map from a periodic multilayer.
The main contribution of this work treats X-ray reflection from multilayer
gratings. I solved this problem using the kinematical theory, the distorted-wave
Born approximation and the rigorous dynamical theory. The dynamical theory has
been treated in the framework of the matrix modal eigenvalue method. The
multiple-beam approximations have been derived from the dynamical theory. As a
limiting case of a single-scattering theory I formulated and thoroughly discussed
the two-beam approximation. The kinematical theory was treated by the stationary
phase method.
All three theories have been formulated within one general formalism. This made
their discussion and comparison easier and transparent. It allowed me to
generalize the Fresnel coefficients involved in conventional specular X-ray
reflection from planar multilayers for the lateral diffraction case. In the
kinematical theory, they were expressed by Fresnel reflection coefficients of
kinematical diffraction, whereas in the dynamical theory the "interface" matrix of
Fresnel coefficients has been generalized. Further I have shown that the
formalism used in all the theories is suitable not only for periodic gratings, but
also for calculating the reflection from more complicated quasiperiodic Fibonacci
gratings.
My main interest has been devoted to short period gratings (period d at
about 1 micrometer) and wavelengths around 1 A, but also larger period gratings
have been briefly discussed. A detailed discussion was performed for a short
period surface grating (SG, d = 8000 A) with the wire to period ratio one half and
for a wavelength of 1.54 A. The theories have been compared analytically as well
as numerically bearing these values in mind. The proposed treatment enabled me to
separate the single scattering and the multiple (dynamical) scattering effects.
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The single-scattering ("two-truncation rod" scattering) regions, where the calculation by
the dynamical theory, two-beam approximation and the DWBA coincide, were determined:
- most of the profile of the strong truncation rods (kinematically
non-forbidden) for
angles of incidence outside the critical angles of the grating materials (the discussed
SG),
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the whole profile of the strong truncation rods for a grating fulfilling the conditions
of validity of the two-beam approximation (the measured multilayer grating),
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most of the profile of the strong truncation rods calculated by the DWBA.
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Strongly dynamical cases, where multiple-beam scattering among many truncation rods
has to be involved and where the single-scattering theories fail:
- the intensity profile of the weak, kinematically forbidden truncation
rods (non-zero even order truncation rods for the discussed SG),
- the intensity scattered in the grazing incidence geometry where the
incident beam falls parallel to the wires.
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Multiple scattering regions, where the single-scattering theories give still approximate
results and where the multiple interaction between several truncation rods has
to be considered:
- near to the angle of incidence for which the wavefield of the TR +1 becomes
real,
- in the region of the critical angles for the strong truncation rods
and the calculation by the two-beam approximation.
The main advantage of the presented approach is the presentation of the regions of
validity of the single-scattering approximations (kinematical theory, DWBA and the
two-beam approx- imation). I demonstrated that within the two-beam approximation
and the DWBA the scat- tered amplitude of the primary scattering process (the
single scattering between the incidence- transmitted and the diffracted-reflected
waves) is proportional to the Fourier transform of the susceptibility.
This proportionality was also the result of the treatment by the kinematical
theory. However, this theory, equivalent to the first Born approximation, does
not include the effect of refraction, which is of major importance in X-ray
reflectivity.
The first order DWBA employed includes the refraction as well as the main features
of the dynamical theory except for a small known region of strong interaction with
TR +1. This DWBA has been found adequate for calculating the intensity of the
measurable non-forbidden truncation rods, which confirms the legitimacy of the
DWBA for gratings as an example of a "big roughness". This confirms the potential
usability of this method for the studies of scattering by randomly structured
layers (e.g., island-layer structures). In addition, I discussed the regions
where the dynamical effects of multiple scattering prevail and where the full
dynamical theory or the DWBA of higher order have to be employed.
In order to include the structural imperfections of real multilayer gratings into
the calculation, I studied scattering from rough multilayer gratings too. I have
considered both the "side wall" roughness of the grating shape and "interface"
roughness into the matrix dynamical formalisms as well as into the kinematical
theory, from which the generalization of the roughness into the DWBA is
straightforward.
In the dynamical theory, I have found that the elements of the "interface" matrix
have to be multiplied by the characteristic function of the interface roughness
probability distribution. This is similar to the "interface" matrices of Fresnel
coefficients introduced for planar multilayers.
In the kinematical theory, the interface roughness acts as the kinematical
Debye-Waller damping factor on the Fresnel coefficients of kinematical
diffraction. The derived analytical formulae allowed the roughness influence on
the scattered intensity to be predicted, which was verified by the numerical
simulation. The side wall roughness was introduced under the approximation of
single-scattering processes by averaging laterally the Fourier coefficients of the
susceptibility.
Finally, the numerical simulations have been applied to fit the structural parameters of a
partially etched InP/GaInAs multilayer grating.
The scientific perspectives of the X-ray reflection methods. X-ray reflection is nowadays
frequently and successfully applied to the structural studies of different kinds of multilayered
samples. Topics of recent investigations by this technique are:
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interface correlation functions of samples with different types of random
interfaces,
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multilayers with terraced interfaces, e.g., multilayers grown on miscut
substrates,
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laterally structured samples
- with nearly perfect structure (multilayer gratings, quantum wires and dots),
- with large imperfections, like the samples with non-continuous island-like
layers.
In particular, we propose the following studies of the X-ray reflectivity from multilayer
gratings, to which a great deal of this report has been devoted to.
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The discussion here has shown the degree of validity and the limits of the first
order DWBA. In order to extend the application of the DWBA also for the regions
of prevailing effects of multiple scattering (the kinematically forbidden
truncation rods), this method could be expanded into the second order.
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The DWBA could be advantageously used to calculate the incoherent diffuse
scattering from imperfect gratings, using either
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the eigenstates of a laterally averaged planar multilayer with the restriction to
the regions of validity discussed in this work,
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the eigenstates given by the dynamical theory.
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The non-coplanar reflectivity technique can overcome the limitation of the
accessible reciprocal space for the coplanar reflectivity. The presented matrix
dynamical theory using the modal eigenvalue approach has been shown to cope with
the non-coplanar scattering. However, the consistency of the eigenvalue and the
point matching approaches for the strongly dynamical case when the incident wave
falls parallel to the wires has not yet been theoretically confirmed.