SCANNING BRILLOUIN MICROSCOPY

Arch. Sci. Nat. Phys. Math. NS 46, volume spécial

Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

2. Introduction to BRILLOUIN spectroscopy

BRILLOUIN spectroscopy is a well-established optical spectroscopic technique to
investigate mechanical as well as magnetic properties of matter (e.g. SANDERCOCK
1982, KRÜGER 1989, HILLEBRANDS 2005). The technique bases on the phenomenon
of inelastic laser light scattering, for which the incident photons are scattered by
thermally driven elementary excitations in matter, like sound waves (acoustic
phonons) or spin waves (magnons) (BRILLOUIN 1922, MANDELSTAM 1926, GROSS
1930, FABELINSKII 1968, CHU 1974, BERNE & PECORA 1976, DIL 1982). Note that
BRILLOUIN spectroscopy gives access to hypersonic waves and spin waves without
exciting them explicitly by transducers as necessary e.g. for ultrasonic pulse-echo
techniques. Since manifold introductory review articles and monographs on
BRILLOUIN scattering are available (FABELINSKII 1968, CHU 1974, BERNE & PECORA
1976, DIL 1982, SANDERCOCK 1982, KRÜGER 1989, HILLEBRANDS 2005) and since
the current article focuses on scanning BRILLOUIN microscopy, we give only a short
introduction to the theoretical background of BRILLOUIN scattering. In a first
reading, the sections marked with an asterisk* 2.1 (except figure 2.1 and the related
explications) and 2.4 can be skimmed over.

2.1. Scattering of laser light by thermally excited sound

waves*
The theory of inelastic scattering of visible light by thermally excited hypersonic
waves travelling through transparent matter will be recapitulated within a statistical
framework (CHU 1974, BERNE & PECORA 1976). Remember that indeed the
continuum of sound waves within condensed matter can be correlated to spatio-
temporal fluctuations of the mass density, or more generally, of the strain tensor
components (AULD 1973).
ConsiderConsider
a monochromatic
a monochromatic
laser beam
laser
that
beam
can that
be decomposed
can be decomposed
into planar
into waves,
planar
incident
waves, incident
on a dielectric
on a dielectric
sample.sample.
The electric
The electric
part ofpart
eachofincident
each incident
planarplanar
light wave
light
can
wavebecan
described
be described
as: as:
, (2.1)

11
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
Scanning Brillouin
Brillouin microscopy
microscopy Arch.
Arch. Sci.
Sci. Nat.
Nat. Phys.
Phys. Math.
Math. NS
NS 46,
46, Special
Special volume
volume

where denotes the wave vector in the medium, the position vector in the
sample’s coordinate system, the wave’s angular frequency, the electric field
amplitude and defines the direction of polarisation. For the sake of simplicity, we
assume that within anisotropic matter, the incident and scattered electromagnetic
waves represent eigenstates of the electromagnetic field. By this means we exclude
effects related to birefringence. The spatially and temporally fluctuating dielectric
properties of the sample are described by the dielectric tensor . If the
components of the dielectric tensor at optical frequencies fluctuate only spatially,
but not temporally, elastic light scattering can occur. In that case, the scattered
electromagnetic waves generally propagate along other directions than the incident
one while the energy is conserved: and , with denoting the
scattered wave vector. In the domain of materials science, typical candidates for
elastic light scattering processes are polycrystalline materials and nanocomposites
possessing optical heterogeneities in the 100 nanometer to micrometer range.
range.
Inelastic light scattering occurs if the components of the dielectric tensor at optical
frequencies do not only fluctuate spatially, but also temporally. In this
context, two aspects need consideration: the spatially and temporally fluctuating
elementary excitations of the sample that couple to its optical properties and the
strength of this coupling. The spatio-temporal elementary excitations of the sample
can be divided into relaxational fluctuations, like fluctuations of the entropy,
entropy, and
and
propagating fluctuations, like fluctuations of the mass density (BERNE
ERNE & PECORA
ECORA

1976). The corresponding modes are either diffusive or propagating ones. Sound
waves (also denoted as acoustic phonons) are generally induced by thermally
excited fluctuations of the strain tensor components, which degenerate in ideal
liquids to mass density fluctuations. The elasto-optical coupling between the strain
fluctuations and the optical fluctuations is described by the Pockels tensor (NYE
YE

1972, VACHER
ACHER & BOYER
OYER 1972). For most materials, the elasto-optical coupling for

shear strain is much weaker than that for longitudinal strain (NYE
YE 1972, VACHER
ACHER &

BOYER
OYER 1972).

The spatially
The and temporally
spatially and fluctuating
temporally dielectric tensor
fluctuating at optical
dielectric frequencies
tensor can
at optical
be describedcan
frequencies as: be described as:

12
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

, (2.2)

with denoting the spatially and temporally averaged dielectric tensor and
the fluctuating part of the dielectric tensor. The transversely polarized
phonons are responsible for the off-diagonal entries of . The directions of
polarization of the incident planar light wave and of the chosen inelastically
scattered light wave yield the components according to:

. (2.3)
These dielectric fluctuations can be described by the spatio-temporal autocorrelation
function of , with V being the scattering volume and the considered time
interval:

(2.4)

The dynamic structure factor of the scattered light component travelling in

the -direction results from the spatio-temporal FOURIER transformation of the
autocorrelation function of :

, (2.5)

with designating the acoustic phonon’s wave vector and

(with being the angular frequencies of the involved scattered
electric fields; see section 2.2) its angular frequency. The spectral power density
, which is closely related to the dynamic structure factor, is
experimentally accessible by BRILLOUIN spectroscopy. The factor depends on
the intensity of the incident light. As will be delineated below in a rough overview,
the BRILLOUIN lines of the spectral power density are intimately related to the
hypersonic properties of the sample, since these lines are due to dielectric
fluctuations induced by thermal fluctuations of the strain tensor components
(SOMMERFELD 1945, GRIMVALL 1986, LANDAU & LIFSHITZ 1991).
As described
As described
in KONDEPUDI
in KONDEPUDI
& PRIGOGINE
& P(1998), the (1998),
RIGOGINE thermally
theexcited
thermally
fluctuations
excited
fluctuations
of the strain of
tensor
the strain
components
tensor develop
components
according
develop
to according
the same laws
to theassame
macroscopic
laws as
macroscopic
deformations deformations
of small amplitude.
of smallWithin
amplitude.
the frame
Withinofthe
linear
frame
response
of linear
theory,
response
the

13
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
ScanningBrillouin
Brillouinmicroscopy
microscopy Arch.
Arch.Sci.
Sci.Nat.
Nat.Phys.
Phys.Math.
Math.NS
NS46,
46,Special
Specialvolume
volume

strain
theory, the strain
can be related
can be
to related
the thermally
to the thermally
excited excited
fluctuating
fluctuating
elastic elastic
force
density
force density via thevia
elastic
the elastic
susceptibility
susceptibility
tensor tensor , according
, according
to: to:
.. (2.6)
(2.6)
Considering
Considering the
the storing
storing and
and dissipative
dissipative parts
parts of
of the
the elastic
elastic interaction
interaction by
by the
the
symmetric
symmetric forth
forth rank
rank tensors
tensors of
of the
the elastic
elastic moduli
moduli and
and viscosities
viscosities
(with
(with k,k,l,l,m,
m,nn==1,1,2,2,3),
3), the
the strains
strains evolve
evolve with
with time
time like
like
damped
damped oscillators.
oscillators. The
The components
components of
of the
the inverse
inverse elastic
elastic susceptibilities
susceptibilities
correspond
correspondtoto(L
(LANDAU
ANDAU&
&LLIFSHITZ
IFSHITZ1991,
1991,KKONDEPUDI
ONDEPUDI&
&PPRIGOGINE
RIGOGINE1998):
1998):

,, (2.7)
(2.7)

with
with denoting
denoting the
the mass
mass density
density and
and the
the Kronecker
Kronecker symbol.
symbol. The
The tensor
tensor
can
canbe
bediagonalised
diagonalisedinindependence
dependenceof
of and
and , ,which
whichresults
resultsin:
in:

(2.8)
(2.8)

with
with
(2.9)
(2.9)
where
where characterizes
characterizesthe
thepolarization
polarizationstate
stateof
ofthe
thesound
soundwave
waveand
and
denotes
denotes the
the effective
effective elastic
elastic modulus
modulus for
for the
the given
given wave
wave vector
vector and
and polarization.
polarization.
The
The three
three complex
complex eigenfrequencies
eigenfrequencies correspond
correspond toto the
the
poles
polesof
ofequation
equation(2.9)
(2.9)with:
with:
(2.10)
(2.10)
and
and
.. (2.11)
(2.11)
Here
Here designates
designates the
the acoustic
acoustic damping
damping and
and the
the
eigenfrequencies
eigenfrequencies of
of the
the undamped
undamped sound
sound waves
waves for
for aa given
given wave
wave vector
vector . . The
The
related
related eigenvectors,
eigenvectors, i.e.
i.e. the
the polarization
polarization vectors
vectors of
of the
the three
three sound
sound waves,
waves, are
are
orthogonal
orthogonal toto each
each other.
other. For
For p=1,
p=1, the
the mode
mode isis generally
generally quasi-longitudinally
quasi-longitudinally
polarized:
polarized: its
its polarization
polarization vector
vector isis almost
almost collinear
collinear toto the
the direction
direction of
of propagation
propagation
(A
(AULD
ULD1973).
1973).Two
Twoquasi-transversely
quasi-transverselypolarized
polarizedmodes
modesare
aredescribed
describedby
byp=2
p=2and
and
p=3.
p=3. For
For elastically
elastically isotropic
isotropic solids,
solids, all
all modes
modes are
are purely
purely longitudinally
longitudinally or
or

14
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

transversely polarized, i.e. the propagation and polarization vectors are either
collinear or perpendicular (AULD 1973). Moreover, the two transversely polarized
modes are degenerated for isotropic solids. These shear modes do even not
propagate at all in ideal isotropic liquids, where the term ‘ideal’ implicates the
absence of viscoelastic behaviour. In contrast, if the acoustic modes couple to
molecular structural relaxations in a liquid, transversely polarized sound modes can
be detected at sufficiently high frequencies (CHU 1974, BERNE & PECORA 1976,
KRÜGER 1989).

Fig. 2.1. BRILLOUIN spectrum of a homogeneous elastically anisotropic solid

containing the B
Brillouin
RILLOUINdoublets
doubletsofofthe
the quasi-longitudinally
quasi-longitudinally (p=1
(p=1 or
or qL)
qL) and the
two quasi-transversely (p=2, 3 or qT1, qT2) polarized sound modes. (In the
following the notation ‘qL, qT’ will be used.) Angular frequency or
, hypersonic attenuation: or
or ,, height
height ofof SStokes
TOKES or

Anti-Stokes
Anti-STOKESlines:
lines: or
or .. The
The central
central line
line (suppressed in the
figure) corresponds to the RAYLEIGH line, reflecting elastically scattered light and
diffusive modes.

15
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

In the classical limit, the fluctuation-dissipation theorem (KONDEPUDI & PRIGOGINE

1998) relates the polarization-independent dynamic structure factor to the
imaginary part of the susceptibility by:

. (2.12)

Note that the opto-acoustic coupling is not part of the so-defined dynamic structure
factor, and therefore has to be accounted for by an appropriate prefactor.
In the present rough overview, the relationship between the experimentally
accessible spectral power density and the elastic

susceptibilities, described by equation (2.12), permits us to sense that the angular

frequencies and attenuations of the sound waves can be determined

from the measured BRILLOUIN spectrum. A typical BRILLOUIN spectrum for a

homogeneous anisotropic solid is given in figure 2.1. In the centre of the BRILLOUIN
spectrum appears the RAYLEIGH line, corresponding to the elastically scattered light
and the diffusive modes. The three BRILLOUIN doublets are positioned
symmetrically to the RAYLEIGH line on the horizontal angular frequency axis
. In order to calculate the intrinsic hypersonic attenuations the

instrumental broadening has to be deconvolved from the measured BRILLOUIN

spectrum. The angular frequency and attenuation correspond to the position and the
half width at half maximum of the BRILLOUIN lines, respectively. The statistical
error of the hypersonic angular frequency typically lies in the one-tenth of percent
regime, whereas that of the attenuation is larger by roughly a factor of 10. An
increasing half width at half maximum of the BRILLOUIN lines indicates a decreased
lifetime of the considered phonon mode . The here described lifetime of the

phonon (or temporal attenuation of a sound wave) and the spatial attenuation of a
sound wave known from ultrasonic investigations are related by the sound velocity.

For a very small temporal hypersonic attenuation, i.e. , the angular

frequency is not renormalized by the attenuation (see equation (2.11)). Several

16
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

mechanisms are known to contribute to the hypersonic attenuation, like structural

relaxation processes with their main relaxation frequencies in the GHz regime
(BERNE & PECORA 1976, KRÜGER 1989).

2.2. The kinematic approach

In the frame of a quantum-mechanical description, BRILLOUIN scattering results
from inelastic scattering of light photons by acoustic phonons. Applying the law of
conservation of energy to this scattering process allows one to relate the hypersonic
angular frequency of the phonons to the angular frequencies and of the

incident and scattered light, respectively, according to:

. (2.13)
The sign ‘+’ corresponds to the annihilation of phonons (Anti-STOKES scattering),
and the sign ‘-’ to the creation of phonons (STOKES scattering) (see figure 2.1 in
section 2.1). The energy transfer between an incident light photon and an acoustic

phonon equals to about of the photon’s energy. Since typical frequencies of

visible light are about , the angular frequencies of the involved acoustic

phonons are usually in the GHz regime. Similarly the law of conservation of
momentum relates the wave vector of the hypersonic wave to the wave vectors

and of the incident and scattered light according to:

. (2.14)

A schematic representation of this law is given in figure 2.2. Using the inner
scattering angle , the norm of the wave vector equals to:

. (2.15)

17
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

Due to the very small energy transfer between phonons and photons, is a

valid approximation leading to:

. (2.16)

If denotes the vacuum laser wavelength and n the sample’s refractive index, one
obtains:

. (2.17)

Note that in BRILLOUIN scattering the acoustic wave vector is selected by

adjusting the adequate scattering geometry, and that the phonon’s frequency is the
usually complex response. As elucidated in section 2.1, in general three acoustic
phonons, one quasi-longitudinally polarized and two quasi-transversely polarized
are determined for one selected wave vector in an elastically homogeneous solid
(AULD 1973).

Fig. 2.2. Schematic representation of momentum conservation during an inelastic

light scattering process. Sample represented in blue; , : incident/scattered
light wave vector within the sample; : wave vector of the acoustic phonon, and
: inner scattering angle.

For a typical vacuum laser wavelength of , the phonon wavelength

equals to some hundred nanometres and is hence of the same order of
magnitude as the laser wavelength. Thus, optical elastic scattering, like RAYLEIGH or
MIE scattering (BORN & WOLF 1999) in a heterogeneous sample is in most cases
accompanied by acoustic RAYLEIGH or MIE scattering (MORSE & INGARD 1968). For

18
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

sufficiently small hypersonic attenuation ( ), the phase velocity of the quasi-

longitudinally (qL) and quasi-transversely (qT) polarized acoustic modes depends
on the phonon wavelength and frequency f according to:

. (2.18)

Or, using equation (2.17):

. (2.19)

Knowing in addition the sample’s mass density, equation (2.19) allows the
calculation of the related elastic moduli (AULD 1973):
. (2.20)

2.3. Classical scattering geometries

Three common scattering geometries, defining the -vector involved in the
scattering process, are depicted in figure 2.3. In classical BRILLOUIN spectroscopy, a
typical scattering volume is about . The 90N scattering geometry, shown
in figure 2.3a, is a commonly used scattering geometry due to its easy alignment as
, where denotes the outer scattering angle (i.e. the angle between the
incident and scattered light beam outside the sample). Similarly easy to handle is the
backscattering geometry depicted in figure 2.3b, with . The
backscattering geometry is especially suitable in case of non-transparent samples as
the properties within the scattering volume can often still be probed close to the
sample’s surface. The major difference to the situation depicted in figure 2.3b is that
for a non-transparent sample the scattering volume is much more reduced in the x3-
direction (see also section 3.2). Note that in the backscattering geometry for
elastically isotropic samples only information about longitudinally polarized sound
waves can be gathered because of symmetry reasons (VACHER & BOYER 1972).
During the last years, the backscattering geometry has proven to be highly
promising for studying structural processes in dependence of time for transparent

19
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
Scanning Brillouin
Brillouin microscopy
microscopy Arch.
Arch. Sci.
Sci. Nat.
Nat. Phys.
Phys. Math.
Math. NS
NS 46,
46, Special
Special volume
volume

materials
materials (P
(PHILIPP
HILIPP et al. 2009,
et al. 2009, 2011,
2011, SSANCTUARY
ANCTUARY et al. 2010).
et al. 2010). Indeed,
Indeed, the
the large
large
scattering
scattering volume
volume in
in the
the -direction
-direction allows
allows for
for aa comparatively
comparatively high
high temporal
temporal
resolution
resolution as
as B RILLOUIN spectra
BRILLOUIN spectra can
can be
be recorded
recorded fast.
fast. Equations
Equations (2.17)
(2.17) and
and (2.18)
(2.18)
allow
allow for
for calculating
calculating the
the phonon
phonon wavelengths
wavelengths and
and sound
sound velocities
velocities for
for both
both
scattering
scattering geometries
geometries (using
(using or
or ,, respectively).
respectively). The
The related
related
values,
values, both
both dependent
dependent on
on the
the sample’s
sample’s refractive
refractive index,
index, are
are indicated
indicated in
in table
table 2.1.
2.1.

Fig.
Fig. 2.3.
2.3. Representation
Representation of
of (a)
(a) the
the 90N
90N scattering
scattering geometry,
geometry, (b)
(b) the
the backscattering
backscattering
geometry,
geometry, and
and (c)
(c) the
the scattering
scattering geometry
geometry (here:
(here: outer
outer scattering
scattering angle
angle
).). Sample
Sample represented
represented in
in blue,
blue, scattering
scattering volume
volume in
in red.
red. (1)
(1) laser
laser beam
beam
incident
incident on
on the
the sample,
sample, (2)
(2) laser
laser beam
beam leaving
leaving the
the sample,
sample, (3)
(3) selected
selected direction
direction of
of
the
the inelastically
inelastically scattered
scattered light
light emerging
emerging from
from the
the scattering
scattering volume.
volume. ,, ::
incident
incident and
and scattered
scattered wave
wave vector,
vector, :: wave
wave vector
vector of
of the
the acoustic
acoustic phonon.
phonon.
:: sample
sample coordinate
coordinate system.
system.

The scattering
The geometry,
scattering with withbeingbeing
geometry, strictly between
strictly 0° 0°and
between and90°,
90°, is
is
specifically
specifically adapted
adapted to
to many
many experimental
experimental challenges
challenges (e.g.
(e.g. K
KRÜGER
RÜGER et al. 1978a,
et al. 1978a,
1981,
1981, 1986,
1986, K RÜGER 1989).
KRÜGER 1989). ItIt possesses
possesses the
the special
special attribute
attribute that
that the
the adjusted
adjusted
phonon
phonon wave
wave vector
vector is
is independent
independent of
of the
the sample’s
sample’s refractive
refractive index
index nn in
in case
case
of
of optically
optically isotropic
isotropic samples.
samples. Indeed,
Indeed, applying
applying SSNELL
NELL’s
’s law
law to
to figure
figure 2.3c
2.3c allows
allows
for
for expressing
expressing the
the inner
inner scattering
scattering angle
angle in
in dependence
dependence of
of the
the outer
outer scattering
scattering
angle
angle ::
.. (2.21)
(2.21)

20
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
Scanning Brillouin
Brillouin microscopy
microscopy Arch.
Arch. Sci.
Sci. Nat.
Nat. Phys.
Phys. Math.
Math. NS
NS 46,
46, Special
Special volume
volume
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume
Combining
Combining equations
equations (2.19)
(2.19) and
and (2.21)
(2.21) then
then directly
directly leads
leads to
to the
the n-independent
n-independent
sound
sound velocity
Combining expression
equations
velocity for
(2.19) for
expression the
andthe scattering
(2.21) then geometry
directlygeometry
scattering given
leads to the in
in table
table 2.1.
n-independent
given 2.1.
Because
Because of
of the
sound velocitythe usually
usually small
expression forbirefringence
small the of
of anisotropic
scattering
birefringence samples,
geometry
anisotropic given the
samples, expressions
in table
the 2.1.
expressions
indicated
indicated in table 2.1 are also high quality approximations for the phonon wave
Because in
of table
the 2.1
usually are also
small high quality
birefringence of approximations
anisotropic for
samples, the
the phonon
expressions
wave
vector and
indicated the
in sound
table velocities
2.1 are also of optically
high qualityanisotropic samples,
approximations for with
the absolute
phonon errors
wave
vector and the sound velocities of optically anisotropic samples, with absolute errors
being
vector usually
being usually smaller
and the sound
smaller than
than 0.1%
velocities
0.1% (K
of optically
(KRÜGER al. 1986).
anisotropic
RÜGER et
et al. 1986). Hence,
samples, this
this scattering
with absolute
Hence, errors
scattering
geometry is
is especially
being usually
geometry smaller useful
especially if
if high
than 0.1%
useful (Kprecision
high RÜGER etacoustic
precision data
al. 1986).
acoustic are
are needed
dataHence, for
for samples
this scattering
needed samples
geometry
of
of is especially
unknown
unknown optical useful
optical if highFor
properties.
properties. precision
For acoustic
instance
instance it
it isdatafrequently
is are neededemployed
frequently for samplesfor
employed for
of unknowndependent
temperature optical properties.
measurementsFor ofinstance
samples itwithis anfrequently
unknown employed
refractive for
index
temperature dependent measurements of samples with an unknown refractive index
temperature dependent
evolution measurements K of samples1989,
with an RÜGER
unknown refractive index
evolution versus
versus temperature
temperature (e.g. RÜGER 1989, K
(e.g. KRÜGER KRÜGER et al. 1990,
et al. 1990, 1994,
1994,
evolution
JJIMÉNEZ versus temperature (e.g. K RÜGER 1989, K RÜGER et al. 1990, 1994,
IMÉNEZ RIOBÓO et al. 1990, PHILIPP et al. 2008). As thoroughly described in
R IOBÓO et al. 1990, P HILIPP et al. 2008). As thoroughly described in
J IMÉNEZ 3,
chapter RIOBÓO
this et al. 1990,geometry
scattering PHILIPP etis al.often
2008).combined
As thoroughly
with described in
angle-resolved
chapter 3, this scattering geometry is often combined with angle-resolved
B chapter 3, spectroscopy
this scattering geometry is often combined with angle-resolved
RILLOUIN spectroscopy to
BRILLOUIN to precisely
precisely determine
determine the
the elastic
elastic tensor
tensor properties
properties ofof
B RILLOUIN spectroscopy to precisely determine the elastic tensor properties of
anisotropic samples. Commonly, an outer scattering angle of is chosen
anisotropic samples. Commonly, an outer scattering angle of is chosen
anisotropic
because samples. Commonly, ancorresponding
outer scattering angle ofgeometry is is called
chosen
because of the easy alignment. The corresponding scattering geometry is called the
of the easy alignment. The scattering the
because of the easy alignment. The corresponding scattering geometry is called the
90A scattering geometry.
90A scattering geometry.
90A scattering geometry.

Table
Table 2.1.
2.1. Expressions
Expressions for
for the
the phonon
phonon wavelength
wavelength and and the
andthe sound
thesound
sound velocity
velocity
Table 2.1. Expressions for the phonon wavelength velocity
for
for different scattering geometries for optically isotropic samples.
for different
different scattering geometriesfor
scattering geometries foroptically
opticallyisotropic
isotropicsamples.
samples.
Scattering
Scattering 90N
90N backscattering
backscattering 90A
90A
Scattering 90N backscattering 90A
geometry
geometry
geometry
Phonon
Phonon
Phonon
wavelength
wavelength
wavelength

Sound
Sound velocity
Sound velocity
velocity

21
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
ScanningBrillouin
Brillouinmicroscopy
microscopy Arch.
Arch.Sci.
Sci.Nat.
Nat.Phys.
Phys.Math.
Math.NS
NS46,
46,Special
Specialvolume
volume

2.4.
2.4. Determination
Determination of
of elastic
elastic tensor
tensor components
components for
for
anisotropic
anisotropic matter*
matter*
Scanning
Scanning acoustic
acoustic microscopy
microscopy applied
applied toto inhomogeneous
inhomogeneous and
and heterogeneous
heterogeneous
anisotropic
anisotropic materials
materials only
only makes
makes sense
sense ifif inin addition
addition toto the
the spatial
spatial variations
variations of
of
elastic
elastic properties
properties accompanying
accompanying local
local symmetry
symmetry changes
changes are
are recorded.
recorded. Otherwise
Otherwise
both
both effects,
effects, i.e.
i.e. spatial
spatial symmetry
symmetry changes
changes and
and inherent
inherent elastic
elastic modulus
modulus variations,
variations,
can
can hardly
hardly be
be discriminated.
discriminated. AA purposeful
purposeful experimental
experimental approach
approach consists
consists inin the
the
combination
combination of
of scanning
scanning BBRILLOUIN
RILLOUIN microscopy
microscopy with
with angle-resolved
angle-resolved BBRILLOUIN
RILLOUIN

spectroscopy.
spectroscopy. First
First aa recapitulation
recapitulation of
of the
the determination
determination of
of the
the elastic
elastic modulus
modulus
tensor
tensorisisproposed
proposedbefore
beforeproceeding
proceedingtotothis
thiscombined
combinedexperimental
experimentaltechnique
techniqueininthe
the
next
nextsection.
section.
As shownAs
in the previous
shown sections,
in the in BRILLOUIN
previous sections, spectroscopy
in BRILLOUINthe adjustment of the
spectroscopy the
scattering
adjustmentgeometry permits to
of the scattering select apermits
geometry phononto wave
select vector
a phonon with
wave avector
desired
direction and norm.
with a desired Angle-resolved
direction BRILLOUIN spectroscopy
and norm. Angle-resolved BRILLOUIN allows a comparably
spectroscopy allows a
easy access easy
comparably to the elastic
access properties
to the in a given
elastic properties in scattering volume volume
a given scattering for many
for
differently orientedoriented
many differently ’s within one plate-like
’s within sample sample
one plate-like (e.g. KRÜGER et al. 1985,
(e.g. KRÜGER et al.
1986,
1985, 1990,
1986,1994, 2001).
1990, Furthermore,
1994, in a homogeneous
2001). Furthermore, anisotropic material,
in a homogeneous this
anisotropic
technique yields
material, this for a given
technique yieldsphonon wavephonon
for a given vector wave
at vector
best threeatsound velocities
best three sound
(A ULD 1973).
velocities The 1973).
(AULD term ‘atThe
best’ means
term that the
‘at best’ opto-acoustic
means coupling coefficients
that the opto-acoustic coupling
must be so large
coefficients must that sufficiently
be so large that intense phonon
sufficiently linesphonon
intense appear lines
in theappear
BRILLOUIN
in the
spectrum.
BRILLOUINForspectrum.
a given Forthea related
given phonon modesphonon
the related are orthogonally
modes arepolarized, but
orthogonally
these polarizations
polarized, but theseare usually neither
polarizations purelyneither
are usually longitudinal
purely nor purely transversal.
longitudinal nor purely
The evaluation
transversal. Theofevaluation
a BRILLOUIN
of aspectrum doesspectrum
BRILLOUIN not immediately
does notlead to the material-
immediately lead to
describing elastic susceptibility,
the material-describing elastic i.e. the fourth rank
susceptibility, i.e. elastic modulus
the fourth ranktensor.
elastic modulus
For moderate or negligible acoustic losses this problem is solved by combining the
tensor.
constituting
ForCHRISTOFFEL
moderate orequation (AULD
negligible 1973)losses
acoustic with athis
statistically
problem representative
is solved by
dataset of measured Csound
combining the constituting velocities
HRISTOFFEL (KRÜGER
equation (AULD 1986,
1973)
et al. KRÜGER
with 1989).
a statistically
The CHRISTOFFEL
representative equation combines
dataset the measured
of measured with
sound velocities the components
(KRÜGER of
et al. 1986,
the elasticThe
KRÜGER 1989). modulus matrix equation
CHRISTOFFEL (Vcombines
OIGT notation; AULD 1973):
the measured with the
components of the elastic modulus matrix (VOIGT notation; AULD
1973):

22
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

. (2.22)

Here, denotes the sample’s mass density; the eigenvector ,

expressed in the symmetry coordinate system , gives the ‘particle
velocity’, i.e. the oscillation velocity of a volume of the medium being small
compared to the whole sample but large compared to the atomic scale. The particle
velocity reflects the acoustic polarization of the acoustic mode related to the sound
velocity . The -matrix in equation (2.22) is called the CHRISTOFFEL
matrix and is defined for the lowest possible symmetry, the triclinic symmetry, by:

(2.23)

where the unit vector gives the propagation direction

of the acoustic wave, expressed in the symmetry coordinate system .

The matrix representation of the fourth rank elastic modulus tensor for triclinic
symmetry is given by:

. (2.24)

23
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning
ScanningBrillouin
Brillouinmicroscopy
microscopy Arch.
Arch.Sci.
Sci.Nat.
Nat.Phys.
Phys.Math.
Math.NS
NS46,
46,Special
Specialvolume
volume

For
For cubic
cubic symmetry
symmetry the
the CCHRISTOFFEL
HRISTOFFEL matrix
matrix significantly
significantly simplifies
simplifies and
and isis
expressed
expressedas
asfollows:
follows:

.. (2.25)
(2.25)

The
Thethree-dimensional
three-dimensionalsound
soundvelocity
velocitypolar
polardiagram
diagramfor
forcrystals
crystalsof
ofcubic
cubicsymmetry
symmetry
isisstill
stillaathree-sheeted
three-sheetedhypersuperface,
hypersuperface,similar
similartotothe
thelower
lowersymmetries
symmetries(A
(AULD
ULD1973,
1973,
KKRÜGER
RÜGER et al. 1986,
et al. 1986, KKRÜGER
RÜGER 1989).
1989). This
This isis inin contrast
contrast toto the
the degenerated
degenerated optical
optical
phase
phasevelocity
velocitysurface
surfacefor
forcrystals
crystalsof
ofcubic
cubicsymmetry.
symmetry.

Fig.
Fig. 2.4.
2.4. Differently
Differently oriented
oriented symmetry
symmetry coordinate
coordinate systems
systems with
with
respect
respecttotothe
thesample
samplecoordinate
coordinatesystem
system . .The
Theblue
blueface
facedenotes
denotesaaplane
plane
parallel
paralleltotothe
the -plane.
-plane.

The combination
The combination
of the 90Aof scattering
the 90A geometry
scatteringwith
geometry
angle-resolved
with angle-resolved
BRILLOUIN
spectroscopy
BRILLOUIN spectroscopy
is especially suited for determining
is especially suited forthedetermining
elastic tensor
theofelastic
low-symmetry
tensor of
transparent anisotropic
low-symmetry materials;
transparent a materials;
anisotropic task which is hardly
a task which ispossible by other
hardly possible by
experimental techniques
other experimental (e.g. K(e.g.
techniques RÜGERKRÜGER 1990,
et al. et al. 1990,
1994,1994,
2001).
2001).
A prerequisite
A prerequisite
for
this
for this
method
method
is the
is the
availability
availability
of of
plate-like
plate-like
samples
samplesofofthe
thesame
samematerial,
material, each
each
having
havingaadifferently
differentlyoriented
orientedsymmetry
symmetrycoordinate
coordinatesystem
system with
withrespect
respect

24
SCANNING BRILLOUIN MICROSCOPY Arch. Sci. Nat. Phys. Math. NS 46, volume spécial
Scanning Brillouin microscopy Arch. Sci. Nat. Phys. Math. NS 46, Special volume

to the sample coordinate system (see figure 2.4). As elucidated in the

next chapter, rotating the sample plate around an axis being normal to the sample
plane and confining the phonon wave vector within this plane yields the acoustic
indicatrix of this sample cut (KRÜGER et al. 1985, 1986). The determination of the
acoustic indicatrices for a suitable choice of different crystal cuts provides a
representative set of elastic data sufficient to calculate, on the base of the
CHRISTOFFEL equation, the components of the elastic modulus tensor. This will be
exemplarily illustrated in chapter 4 for several crystalline materials.

25