Polarimetry as a single-point measurement at normal incidence was used in this study. The experimentally measured Stokes vector was then used for the determination of , hence, the ratio of , which is equivalent to in s,p-polarisations defined in the plane of incidence. Noteworthy, is the reflectance of s- and p-pol. at normal incidence is the same for the E-field components from uniform material. However, anisotropy of light scattering can be present from uneven surfaces for the two perpendicular orientations of the incident E-field. This is explored in the current study. If only anisotropy in scattering or absorbance within the skin depth is present, the polarisation ellipsis should be in the principle axis plane (), i.e., . Here the is the absorption coefficient [cm−1] and k is the imaginary part of the complex refractive index ).
Similarly, the
or phase retardance due to birefringence within the skin depth or normal/anomalous dispersion regions around the absorption line (at fixed wavelength) as well as depolarization due to scattering can appear as retardance due to birefringence
:
. As for usual transmittance measurements, birefringence causes the opening of the ellipsis (a larger ellipticity angle
) and its orientation
; for
a circular polarisation is obtained, the ellipsis becomes a circle (
Figure 1). Left or right circular polarisation depends on the sign of
with positive being LHC or anti-clockwise (looking into the beam) and RHC for the clockwise case.
When the short wavelength is used, scattering is strong
and skin depth is shallow
. We used
nm cw-laser to determine Stokes vectors from normal reflection from different materials of industrial relevance: carbon fiber reinforced polymer (CFRP), laser polymerised grating patterns. Experiments were carried out at four sample orientation angles using polarimeter. The same four angles are used to reveal the orientation and anisotropy using linear polarizers in 4-pol. camera (
Figure 1a).
3.1. Linear Patterns at Different Degrees of Alignment
Figure 3 and
Figure 4 show
and
calculated from Stokes vector in reflection. The common feature is that the linear structures are 7-15
m in diameter while the focal spot is considerably smaller
m for
focusing. The CFRP sample has a black appearance with carbon fibers aligned preferentially in one direction. The polymerised SZ2080
TM resist grating of period
m was coated by
nm Au film by sputtering. When measured from the Au side, the reflected polarisation was the same as that of the incident beam almost regardless of orientation, same was observed for flat Au mirror or Si wafer surface.
Figure 4 shows results were laser was irradiating the sample from the uncoated glass side. In both cases of samples, the reflected Stokes parameters had a qualitatively similar behavior. When the delay
was high and approaching
, which would correspond to the birefringence defining a
-waveplate condition, the auxiliary angle
, which corresponds to negligible
component. Thus, no circular polarisation was formed in reflection, i.e., the same linear polarisation as that of incidence (
) only phase delayed upon reflectance. When light back-reflects from interface with higher refractive index material (impinging from air
), the phase change of
occurs. Interestingly, reflection from optically flat absorbing materials such as 100-
m-thick kapton or
cm epoxy puck, there was a recognisable ellipticity angle
. This can be attributed to light the scattering and depolarisation at subsurface regions.
Figure 2.
Polarimetry of CFRP at 405 nm. (a) Normalised Stokes vector at different sample orientation angles measured for 40 s. (b) Azimuth and ellipticity of the polarisation ellipsis over measured time. Laser power 55 mW.
Figure 2.
Polarimetry of CFRP at 405 nm. (a) Normalised Stokes vector at different sample orientation angles measured for 40 s. (b) Azimuth and ellipticity of the polarisation ellipsis over measured time. Laser power 55 mW.
Figure 3.
(a) Microscopy image in reflection of carbon fiber reinforced polymer (CFRP) with apparent prevalent horizontal alignment of fibers. (b) The averaged azimuth and ellipticity angles
, respectively, calculated from the measured Stokes vector at different orientation angles
of the sample;
corresponds to horizontal
x-axis (see raw data in
Figure 2). (c) The delay
and auxiliary angle
vs
; the trend of fit by
is plotted, where
and
,
. Illumination with cw-laser at 405 nm.
Figure 3.
(a) Microscopy image in reflection of carbon fiber reinforced polymer (CFRP) with apparent prevalent horizontal alignment of fibers. (b) The averaged azimuth and ellipticity angles
, respectively, calculated from the measured Stokes vector at different orientation angles
of the sample;
corresponds to horizontal
x-axis (see raw data in
Figure 2). (c) The delay
and auxiliary angle
vs
; the trend of fit by
is plotted, where
and
,
. Illumination with cw-laser at 405 nm.
Figure 4.
(a) Microscopy image in reflection of SZ2080TM resist grating polymerised by fs-laser direct write. The schematic drawing shows sample’s structure: polymerised rods protruding for m out of cover glass (m thickness) and coated with nm of Au. (b) The azimuth and ellipticity angles , respectively, calculated from the measured Stokes vector at different orientation angles ; corresponds to horizontal x-axis. (c) The delay and auxiliary angle vs ; the trend of fit by is plotted, where and , . Illumination with cw-laser at 405 nm.
Figure 4.
(a) Microscopy image in reflection of SZ2080TM resist grating polymerised by fs-laser direct write. The schematic drawing shows sample’s structure: polymerised rods protruding for m out of cover glass (m thickness) and coated with nm of Au. (b) The azimuth and ellipticity angles , respectively, calculated from the measured Stokes vector at different orientation angles ; corresponds to horizontal x-axis. (c) The delay and auxiliary angle vs ; the trend of fit by is plotted, where and , . Illumination with cw-laser at 405 nm.
Figure 5 shows ellipsometry spectra for complex refractive index
. At selected absorbance peak of 304 nm, the angular dependence of
was fitted by
function. It has a twice lower angular frequency
(typical for absorbance with folding at
in transmission) as compared with the polarimetry fit at 405 nm which had
dependence (typical for birefringence in transmission). The phase difference/delay
can result from reflection from the surface which has anisotropic features and complex composition (e.g., carbon fibers and polymer composite matrix). Upon reflection there is
phase shift when light travels from low-to-high index
n material and reflects back (typical for incidence from air). For absorbing surfaces, it can be different when the real part of permittivity (epsilon)
becomes less than 1 (as of air’s). In
Figure 5 such spectral region is at
m region where
. No phase change upon reflection would occur in this region called epsilon-near-zero (ENZ), especially for the sample orientation when polarisation of incident light is aligned to the carbon fibers at
.
From ellipsometry data on CFRP at visible-IR range
-anisoptropy typical for absorbance is dominating. At the used 405 nm illumination in reflection at the normal incidence, the CFRP has low-
k and large-
n, hence
and will define the phase change upon reflection (
Figure 3). This phase change has
-dependence typical for the phase delay
. Light scattering is dominating for the polarimetry measurement, since scattering is related to
n, hence to
, rather absorbance and its dichroism, which is related to
k.
Reflected laser beam from electrically conductive mirror surfaces was maintaining its linear polarisation as expected [
16]. For metals described with Drude model, permittivity
[
2], here
is used to make distinction from the above used
k when definition of refractive index is
. According to the Drude model
, where
is conductivity,
is the cyclic frequency. Hence, from the real and imaginary parts of the permitivity:
and
. Depending on the wavelength
, the actual phase change upon reflection from the surface is defined by the real part of the effective permittivity
.
3.2. Azimuthaly Changing Orientation: Laser Ablated Ripples
Linear grating-like patterns investigated by polariscopy in Sec.
Section 3.1 were larger than the focal diameter. Here, we analyse the orientation of a grating-like laser ablated ripples on the surface of Si (
Figure 6) [
19]; such ripples with changing orientation can also be inscribed inside transparent materials [
20]. Ripples have periods comparable or smaller than the focal diameter. Ripples were made by laser ablation with
J energy pulses. They were focused using a cylindrical lens
mm at position 180 mm before the objective lens of numerical aperture
(Mitutoyo). The vertical line of 1 mm width at
(long axis) and
m wide (short axis) focal region was formed. Ablation width was
m (
Figure 6); the ablation threshold fluence of Si is
J/cm
2. Ablation was carried out at 100 kHz repetition rate with 10 pulses per micron along the scan at speed
mm/s. Different rotation speeds of
-waveplate were used along the scan resulting in different lengths of patter for full rotation for
(
Figure 6a). The period of ripples on Si was
[
21] as expected for conductive non-transparent samples (
Figure 6b); it has the highest intensity in FFT map. Such azimuthally patterned gratings are used to discriminate left-hand from right-hand circular polarised light upon reflection. Here we use them to study polarisation changes upon reflection of linearly polarised incident 405 nm laser light.
Stokes vector was determined from reflection of 405 nm laser light linearly scanned along the central cross-section of the rotating ripples pattern (
Figure 7). At this wavelength, Si has a high refractive index
since it is close to the absorbance peak at 376 nm for the direct transitions in Si where
. The angles of azimuth and ellipticity were found qualitatively following different angular dependence of the orientation angles of ripples
. The azimuth was close to
dependence (expected for dichroism) while ellipticity
(expected for birefringence). Also the original orientation phase
was perpendicular to each other for the
and
. Interestingly, only high-
conditions were satisfactory for collecting polarimetry data. This might be related to the larger collection angle important for the acquisition of anisotropic scattering. High refractive index of Si
facilitated strong reflection, however, equally a strong scattering. At the region of ripples pattern, which are dark in cross-polarised view, the
as was observed with the linear structures of CFRP and polymer grating. Similar to the cases analyzed above for linear patterns (Sec.
Section 3.1), the phase
was the largest and approaching
when
(d). Such conditions correspond to the linearly polarised reflected light.
When the the focal spot is smaller than the period
of ripples on surface of the sample, the form birefringence
(
is the refractive index of the extraordinary beam (or the fast axis) polarised perpendicular to the grooves and
is for the ordinary beam (slow axis) along the grooves
), which is negative by definition and contributes to the reflected phase [
21]. The form birefringence corresponds to the uniaxial crystal with permittivity
in respect to the optical axis. For the depth of the structure
d, the phase retardance is
(a double path length due to reflection).
Apart from the form-birefringence and anisotropic scattering, strong refractive index changes are taking place at the vicinity of the absorption bands with negative and positive dispersion regions, hence,
at the neighboring wavelengths of the absorption spectral region. This affects the phase of the reflected light assessed from the Stokes polarimetry. Since we used 405 nm wavelength, absorption is usually present in transparent materials such as glasses and polymers. For the Lorenzian absorption spectral lineshape, the absorption
and dispersion
are related to the
k and
n, respectively; here
is the relaxation time (linked to the bandwidth of the line),
is the cyclic frequency of the spectral position of the absorption line. Strong phase
changes in polarimetric measurements due to the dispersion
changes will appear as birefringence near the absorption band
with a sign dependent on the normal or anomalous side from the absorption line [
23].
3.3. Diamond: A Transparent Sample with Grating-Pattern
The previous section analysed ripples on Si at the wavelength, which is strongly absorbed and for the focal spot, which is comparable to or larger than the periodicity of the grating-like pattern. Next, we analyse nano-gratings defined by the electron beam lithography (EBL) in a 5-
m-thick poly-crystalline diamond membrane [
24]. The structure is an optical spin-orbit converter - the q-plate - where the optical slow-axis is rotating with azimuth angle
according to
. Such an optical element will generate an optical vortex beam with topological charge
, i.e., the number of rotations along propagation of a single wavelength. The most efficient spin-orbit conversion upon illumination with circularly polarised light occurs at a longitudinal phase retardance of
between E-field components along the grating pattern ‖ (extraordinary
e-beam) and perpendicular ⊥ to it (ordinary
o-beam). For such condition,
for the height
h of the structure. The form-birefringence
is defining the phase retardance and is dependent on the refractive index of the host material (here diamond with
at visible wavelengths) and a fill-factor of the grating pattern.
Figure 8 shows data of the
q-plate. Optical reflectance image shows distinct patterns in cross-polarised image. The actual structure is shown in SEM images. The focal spot was approximately 3 times larger than the period
of the grating. The ellipticity and azimuth as well as phase and auxiliary angles (c) were following the same trend as for the case of reflective larger scale patterns on CFRP and Au-coated polymerised grating. In the case of the micro-membrane of patterned diamond q-plates, sample was transparent. A large range of
is suitable for detecting changes via polarimetry.