Visualisation of structured lubricants in
Robert J. Elkington and Dr. Monica Ratoi
National Centre for Advanced Tribology at Southampton (nCATS) at the University of Southampton, UK
The layered, lamellar phase of lyotropic liquid crystals display promising tribological properties possessing low
shear strength between layers, solid like elasticity and high load carrying capacity perpendicular to their layered
structure. Being able to visualise and study the behaviour of LLC in high pressure contacts at a range of speed, slide-
roll ratio (SRR) and temperature conditions can facilitate the understanding of the mechanism of action behind their
low friction properties.
A microscope setup has been developed that is capable of collecting real time, high contrast videos of film
formation, bulk alignment, and flow of liquid crystal containing lubricants in an EHD ultra-thin film tribometer. This
project aims to describe an economic set of methods to evaluate qualitatively the behaviour of liquid crystals in and
around tribological contacts.
This is demonstrated with two types of liquid crystals; lamellar lyotropic Oleic Acid/Triethanolamine and
smectic thermotropic 8CB
Unlike conventional lubricants, liquid crystals (LC) exist as a material state between solid and liquid, often
described as disordered solids or ordered liquids. They flow like a liquid, but molecules can order themselves in a
crystal-like way; they possess transnational order in one or two dimensions. LCs exhibit characteristic properties of
liquids such as fluidity, low shear strength, and anisotropy of optical, thermal, and electromagnetic properties. It has
long been known that the structured order of certain LC compositions can form surface aligned ordered layers which
can easily slip over each other and hence display some very promising tribological properties [1, 2]. LC lubricants and
additives have attracted little attention within tribology when compared to more conventional chemical lubricant
Lamellar phase liquid crystals are of particular interest for their low friction properties as they possess low
shear strength between layers and perpendicular to the layered lamellar structure the properties are similar to a solid,
possessing solid like elasticity, rigidity, and load carrying capacity. The low friction mechanism of lamellar LCs is
analogous to graphite with a sheet-like structure which has stronger interactions within each lamella than between
the lamellae . When a LC lamellar phase is present between loaded surfaces their transverse rigidity is able to
separate the surfaces and also provide a low coefficient of friction due to the low shear planes between layers.
LC phases can be formed by a huge variety of mesogenic (a compound that displays liquid crystal properties)
molecules of which there are two main types: thermotropic liquid crystal (TLC) phases which depend on temperature;
and lyotropic liquid crystal (LLC) phases which depend on temperature and mesogen concentration in solvent . TLCs
are generally made from nanometre scale rod-like molecules. It is convention to refer to the TLC lamellar phase as
smectic and this typical structure is illustrated in Figure 1. Figure 2 shows a lamellar LLC structure; which occurs when
a suitable concentration of an amphiphilic mesogen is dissolved in a solvent to form bilayers separated by solvent.
Lamellar LC lubricants have been shown to be highly effective high pressure, high speed lubricants where the
best conventional lubricants may break down causing an increase in friction and surface damage . The lubricating
properties of LC molecules have been the subject of a variety of studies. It has been consistently reported that liquid
crystals, pure and as additives, give lower friction than many conventional lubricating oils [6, 7, 2].
LC structures show a clear load and shear dependence. At low loads LC molecules align imperfectly and give a
relatively thick film compared to isotropic fluids; this is due to the strong interaction of LC molecules adsorbing at the
surface interface. LC molecules align at a proximate surface; in the case of a high energy surface they will adopt a
planar alignment with the long axis (termed the director vector) parallel to the surface; in the case of a low energy
surface the director will align normal to the surface in a homeotropic alignment . Previous research showed as load
is increased the film thickness reduces, the shear rate increases leading to shear alignment of the LCs in the direction
of the velocity vector [9, 10].
It is important to understand the presence and extent of molecular alignment of LC lubricants in and around
concentrated contacts to understand how alignment influences film formation, rheological properties, and the friction
force between rubbing surfaces. The qualitative behaviour of LC lubricants is difficult to evaluate due to their high
dependence on shear, pressure, temperature and molecular orientation. Many techniques have already been used to
investigate liquid crystal lubricant orientation in contacts, namely Raman, X-ray diffraction, atomic force microscopy
(AFM), Fourier-transform infrared spectroscopy (FTIR), polarised optical interferometry, and scanning electron
microscopy (SEM) [11, 12]. However, these methods are difficult to employ in situ, require specialist operators, and
are expensive to purchase and run.
Figure 1 Smectic TLC, the vector n denotes the average direction of the long axis of the molecules
Figure 2: The structure of a lamellar lyotropic mesophase consists of surfactant bilayers separated by solvent.
A brief introduction to polarised light microscopy
This report will investigate the applications of low cost polarised light microscopy (PLM) techniques for direct
visualisation of molecular orientation inside a tribological contact. PLM is a contrast enhancing technique used to
observe specimens that are visible due to optical anisotropy. A basic PLM transmission microscope is equipped with
two crossed linear polarisers, one in the light path before the specimen, and a second polariser (analyser) above the
specimen. The high degree of long-range orientational order of lamellar LCs will give a highly anisotropic specimen
which is optically uniaxial and strongly birefringent.
Birefringence is the optical property of a material that has a refractive index that depends on the propagation
direction of the incident light and is measured as the maximum difference between the refractive indices of the
material. Figure 3(a) shows a prolate spheroid model of a uniaxial liquid crystal molecule, birefringence of an LC sample
is due to the index of refraction along the long axis (extraordinary axis, ne) being different to the index of refraction
perpendicular to the short axis (ordinary axis, no). The birefringence (B) is expressed by:
𝐵𝑖𝑟𝑒𝑓𝑟𝑖𝑛𝑔𝑒𝑛𝑐𝑒 (𝐵)= |𝑛− 𝑛|
Plane polarised light incident on a birefringent sample is split into two mutually perpendicular planes. At the
analyser the two wavefronts combine where the relative retardation (Γ) of the wavefront will give an interference
colour reminiscent of the Michel-Lévy interference colour chart depending on the sample thickness (t) and
birefringence. Retardation is expressed as:
𝑅𝑒𝑡𝑎𝑟𝑑𝑎𝑡𝑖𝑜𝑛 (Γ)= t ∙ |𝑛− 𝑛|
As the incident light is polarised, any transmitted light that does not interact with a birefringent sample will
be removed by the analyser (a linear polariser crossed relative to the incident light) leaving only the image from the
interference with the anisotropic sample. For a sample of thickness t the phase shift (𝛿) between the ordinary and
extraordinary ray is expressed as:
𝑃ℎ𝑎𝑠𝑒 𝑠ℎ𝑖𝑓𝑡 (𝛿)= 2𝜋
𝜆∙ Γ = 2𝜋
𝜆∙ t ∙ |𝑛− 𝑛|
where λ is the wavelength of plane polarised light .
Figure 3(a) shows that plane polarised light incident on the axis corresponding to ne. The wavefront only
coincides with this refractive index and no birefringence will be observed, the light beam only interacts with no. Figure
3(b) shows how light incident on a LC molecule tilted in a shear flow will interact with two refractive indices, both the
ordinary and extraordinary indices. This light will be subject to a birefringent effect and produce an image at the
analyser demonstrating an anisotropic effect, and hence LC structure in the sample. A similar technique using shear
induced polarised light imaging techniques has already been on a cone-and-plate rheometer for investigating
polymeric and LC materials .
Figure 3: (a) optical indicatrix of a uniaxial liquid crystal where the semi axes correspond to the extraordinary (ne) and ordinary (no) refractive
index with the incident light parallel to the extraordinary axis. This models a homeotropically aligned liquid crystal. (b) optical indicatrix of a
uniaxial liquid crystal with a tilt towards the direction of shear with incident light oblique to the ordinary and extraordinary axes.
Materials and Methods
Two types of liquid crystals were used in these experiments; lamellar lyotropic LCs of triethanolammonium
oleate with triethanolamine acting as the solvent ; and room temperature smectic 8CB TLCs. Room temperature
lamellar lyotropic LCs of triethanolammonium oleate (TEOL) were prepared at ambient temperature directly from its
constituents, oleic acid (reagent grade, > 99%) and triethanolamine (regent grade, > 99%) purchased from Sigma
Aldrich in a 1.6:1 molar ratio. This lamellar LC was first reported by Friberg and has been confirmed to give a lamellar
structure in this concentration [16, 15]. A thermotropic ambient temperature smectic LC 4'-n-Octyl-4-
biphenylcarbonitrile (8CB) was purchased from TCI chemicals UK Ltd. The LC properties were confirmed using a
research grade polarised light microscope and low angle XRD. Glycerol (reagent grade, > 99%) was purchased from
Fischer-Scientific to be used as an optically isotropic control.
Perpendicular microscope setup
The Ultra-Thin Film Measurement System (PCS Instruments, UK) is a computer-controlled bench-top
instrument for simultaneous measurement of friction coefficient and film thickness of lubricants in the
elastohydrodynamic (EHD) lubricating regime. The instrument is capable of loads of 0 – 50 N, speeds of 0 – 4 ms-1, and
a slide/roll ratio from pure rolling up to pure sliding. The high pressures and velocity gradients in EHD contacts produce
very high shear stresses that can promote alignment of LC molecules in and around the contact.
This instrument uses optical interferometry to measure ultra thin films in a Hertzian contact made between a
transparent glass disc and a highly reflective AISI 52100 steel ball. Hence the tribometer is already equipped with a
monoscope and a contact geometry designed for in situ microscopy and was determined to be a suitable test bed for
mounting PLM to view LCs inside a tribological contact in a range of conditions. It is assumed that the glass disc is
optically isotropic (i.e. not birefringent) and the reflection at the steel ball does not significantly contribute to the
phase shift of the light, thus any birefringent effect observed is from the sample.
Figure 4: Schematic of optical components required for PLM on EHD tribometer
Figure 4 shows a schematic of the optical components required to image LCs and is based on the components
typically used to image birefringent specimens in a reflection mode. This setup uses a broad-band light source (a white
halogen lamp). The contact is made between a plain glass EHD disc and reflective steel ball. The optical path is
described as follows. The light passes through a polariser such that plane polarised light enters the beam splitter that
is reflected down a 10x objective at 90° to the shear (contact) plane. The light is reflected at the steel ball and hence
makes a double pass through the sample inside the contact. The light will then pass through the beam splitter up to
the quarter wave plate, analyser (second linear polariser), and into the CCD camera.
If the lubricant sample is not birefringent then there will be no change of polarization state in the light
reflected. This will not be transmitted through the analyser as the axis is orthogonal to the axis of light polarization
and the image will be one of total extinction i.e. completely dark. With a birefringent sample the polarization state of
the light will be rotated after passing through the sample. The light will be transmitted through the analyser and as
the orientation of the axes of polarisation will be different to the orthogonal, an image showing birefringence will be
A quarter waveplate (QWP) is included as a contrast enhancing technique in cases where the optical path is
small, as the QWP will increase the path difference between the ordinary and extraordinary wavefronts. Furthermore,
by aligning the fast and slow axes of the waveplate with the ordinary and extraordinary wavefronts it is possible to
infer the alignment direction of the LCs. Here, the phase shift for the sample is expressed as:
𝑃ℎ𝑎𝑠𝑒 𝑠ℎ𝑖𝑓𝑡 (𝛿)= 2𝜋
𝜆∙ 2h ∙ |𝑛− 𝑛|
where h is film thickness at that point (2h accounts for the light beam making a double pass).
Figure 5 shows a labelled diagram of the optical setup installed on the EHD tribometer. This setup will be used
to detect shear alignment of LCs inside the EHD Hertzian contact. As the microscope is 90° to the contact (shear) plane
no image will be produced if the sample inside is aligned homeotropically between the disc and the ball and to detect
this a microscope mounted at an oblique angle is required.
Figure 5: Labelled diagram of optical setup on EHD
Oblique microscope setup
A second optical setup was developed, operating in the same way as the microscope previously described, but
instead entering the contact at an oblique, 45° angle. Due to scattering and reflection effects at the air-glass interfaces
a 633 nm (red) laser was employed as a much brighter light source was required. This setup was used to investigate
LC samples in conditions that would promote the presence of homeotropically aligned structures in the contact (i.e.
structures that would not display birefringence when viewed with the microscope normal to the contact).
Figure 6: Schematic of optical components required for PLM at an oblique (45°) angle on the EHD tribometer
Figure 6 shows a schematic of the optical components in the oblique microscope setup. The optical path is as follows.
The 3 mW 633 nm HeNe laser emits polarised light, a half wave plate is used to rotate the plane of polarisation (in lieu
of rotating the laser) to adjust LC image quality. Light enters the glass disc at a 45° angle, some light is reflected at the
glass-air interface, but a sufficiently bright beam enters the glass disc and LC sample through a 10x objective. The light
is reflected at the small flat central area of the Hertzian contact at 45°, through the disc, and into a second polariser
(analyser) with an axis orthogonal to the laser output polarisation. This then passes into a CCD camera and lens to
focus the image onto the CCD chip. The phase shift for this geometry is expressed as:
𝑃ℎ𝑎𝑠𝑒 𝑠ℎ𝑖𝑓𝑡 (𝛿)= 2𝜋
cos (45°) ∙ |𝑛− 𝑛|
where h is the film thickness at that point, the
(°) factor comes from the double light pass through the sample at
an angle of 45°.
As monochromatic light (laser) is used a colourful interference pattern is not possible. In cases where the
sample is not birefringent there will be no change in the state of polarisation and the light will stop at the analyser,
producing no image in the Hertzian contact. If the sample is birefringent then the state of polarisation will be rotated,
and light will pass through the analyser producing an image inside the Hertzian contact area. Figure 7 shows a labelled
diagram of this setup installed on the EHD tribometer.
Figure 7: Labelled diagram of oblique microscope used on EHD
Results and Discussion
At 25 °C TEOL and 8CB were in a lamellar phase. Small amounts of each LC sample were placed on glass
slides and viewed through a microscope equipped with crossed polarisers. The PLM images of TEOL and 8CB are
shown in Figures 8 and 9 respectively. Both samples show a characteristic streaky texture indicative of a lamellar
phase [17, 16].
Low angle x-ray diffraction measurements confirmed the TEOL mixed at a 1:1.6 triethanolamine and oleic
acid molar ratio has a lamellar structure with an interlayer spacing of 38 Å, this is indicated by a clear peak around
2.6° shown in Figure 10.
Figure 8: PLM image showing optical pattern of lamellar LLC TEOL at 25 °C, note the 'oily streak' texture characteristic of a lamellar lyotropic
liquid crystal phase
Figure 9: PLM image showing optical pattern of smectic 8CB at 25 °C
Figure 10: Low angle X-ray diffraction measurements showing a clear peak at 2.6° which corresponds to an interlayer spacing of 38 Å. A second
smaller peak can be seen around 5.2° which corresponds to 19 Å, the height of half a bilayer.
Perpendicular microscope experiments
A small amount of TEOL was placed between the steel ball and glass disc of the EHD tribometer. As the static
load is increased the LC is observed to align radially towards the centre of the contact, the point of the highest load.
Figures 11(a), (b) and (c) show this transition as the load is increased to 20 N. In the absence of the load [Fig. 11(a)]
the TEOL appears isotropic when viewed through the microscope showing the sample is not aligned. As the load is
increased to 3 N [Fig. 11(b)] a Maltese cross strain pattern becomes noticeable around the Hertzian contact, when the
principal directions of the hemispherical stress pattern in the glass form a zero angle with the polariser or analyser
axis isogyres appear resulting in the Maltese cross pattern . This is not the result of the birefringent sample as a
similar Maltese cross stress pattern can be seen with optically isotropic glycerol [Fig 11(d)].
Above 3 N a sudden transition is observed where the TEOL align radially towards the centre of the Hertzian
contact. As load is increased the observed alignment does not change significantly; increasing the load only increases
the size of the contact. This alignment is demonstrated in Fig 11(c) at a load of 20 N, corresponding to a maximum
contact pressure of 0.51 GPa. This image is composed of two distinct regions; the dark centre of the image including
the Hertzian contact and the surrounding dark area; and the area populated with yellow and blue domains of
birefringent LC structures. In static conditions there is only a very thin squeeze film inside the Hertzian contact area,
so thin that it would not interact significantly regardless of the LC orientation. The dark area surrounding the HC
indicates an area where the lamellae are orientated with their layer normal parallel to the glass surface (aligned
homeotropically and light orthogonal to the lamellar planes will not experience a birefringent effect). High pressures
have been shown to promote highly ordered homeotropic alignment of lyotropic, lamellar structures . This will be
further investigated with the oblique microscope.
LC structures become visible approximately 400 µm from the centre of the HC, this is an area where the
pressure on the fluid is substantially lower and the fluid film is thicker. The visible LC structures are aligned radially
and correspond to lamellae with a layer normal at a tilted or perpendicular angle to the incident light. The yellow and
blue colours are a result of interactions at the fast and slow axis of the QWP. There is no noticeable gradient of
birefringence indicating that all the lamellae are orientated by the same degree which would suggest the lamellae are
orientated with the layer normal perpendicular to the incident light. A very similar well-defined boundary has been
observed for lamellar phase LCs induced by a critical shear rate in work done by Mykhaylyk et al . In this case the
transition has been induced by a critical pressure.
Figure 11: Static alignment of TEOL (between a glass disc and steel ball) as load is increased from 0 to 20 N (a) no contact, 0 N (b) isotropic
stress pattern begins to appear as load is increased from 2 to 3 N (c) radial alignment of TEOL around Hertzian contact, the fast and slow axis of
the QWP are marked. (d) glycerol viewed through the same setup at 20 N, a stress pattern is still visible around the Hertzian contact
Figure 12: Annotated image of elliptical Hertzian contact showing TEOL alignment along the entrainment direction (U). The inlet pool, HC area,
outlet pool, and axes of the QWP are marked.
Figure 12 shows an annotated image of a TEOL lubricated elliptical EHD contact in dynamic conditions (20
mms-1 with a 50% SRR and 20 N load). Interesting information for TEOL in this setup is visualised in the inlet and outlet
pools of the EHD contact where birefringent structures are visible. By using a larger size elliptical contact, the contact
pressure in and around the contact is lower at the same applied (20 N) load and the front of the visible LC appears
closer to the HC area. However, the elliptical roller used in this contact geometry was not fixed about its transverse
axis and at high speeds would oscillate slightly leading to obscured blurry images of the HC. In Figure 12 faint Newton
rings can be observed below the contact but this detail is lost at speeds above 50 mms-1.
Figure 13 shows TEOL behaviour in a range of speeds with a 20 N load and 50% SRR. At low speeds [Figures
13(a) and 13(b)] show the inlet pool contains separated domains of alignment with only some of the LC structure
appearing light blue along the slow axis of the QWP. As speed is increased to 20 mms-1 [Fig 13(c)] the LC in the inlet
pool align homogenously in the entrainment direction with a much more stable flow. Figure 14 shows an enlarged
image of the of the inlet at 5 mms-1 and 20 mms-1.
At higher speeds [Figures 13(d) and 13(e)] the entrainment direction dominates the LC alignment in the inlet
pool up to speeds of around 200 mms-1 at which point the homogenous alignment began to break down at the entry
of the inlet pool [Fig 13(f)]. This is characterised by dark spikes appearing demonstrating a definite change in LC
structure in this region, a gradient of colour is seen indicating that this feature is still birefringent and therefore
structured. Whilst it is not shown in this figure, the appearance of these spikes consistently preceded starvation,
though the exact structural significance of these features is unknown.
These tests were repeated for a state of pure rolling (0% SRR) and pure sliding (100% SRR). At low speeds (5 –
20 mms-1) an increase in sliding (SRR) leads to homogenous TEOL alignment in the contact inlet at lower speeds. In the
case of 100% SRR complete alignment was observed in the inlet at a speed of 10 mms-1. This further demonstrates
lamellar LCs sensitivity to shear.
In all tests no birefringence effect was observed inside the HC which suggests the structure inside the contact
is homeotropically aligned as light orthogonal to lamellar planes will experience no birefringence.
Figure 13: Images of elliptical EHD contact lubricated with TEOL at 20 N, 50% SRR at speeds of (a) 5 mms-1 (b) 10 mms-1 (c) 20 mms-1 (d) 50
mms-1 (e) 100 mms-1 (f) 200 mms-1. The entrainment direction and QWP axes are marked on (a) and is the same for each case. The white
dashed ellipses indicate the location of the HC in (e) and (f).
Figure 14: Enlarged images of inlet pool of EHD contact lubricated with TEOL at 20 N, 50% SRR, at (a) 5 mms-1 and (b) 20 mms-1.
Figure 15 shows a sample of 8CB in an elliptical HC under a load of 20 N in static conditions. The HC is obscured by a
reflection effect at the 8CB-glass interface, and the location of the HC is circled by a dashed white line. The colours
immediately above and below the HC are consistent with first, second, and third order interference colours with no
QWP inserted . 8CB has been shown to maintain a homeotropic structure up to pressures above 250 MPa, even
displaying a pressure induced layer expansion .
The area inside the HC displays no birefringence which is expected in static conditions as the squeeze film will
have a thickness on the order of nanometres and will not noticeably change the state of light polarisation. The
interference colour gradient outside the contact shows the 8CB smectic structure is orientated uniformly towards the
contact. Outside this area the LC tilt appears to lose uniformity.
Figure 15: Static elliptical HC lubricated with 8CB at 20 N (max contact pressure 0.3 GPa), the white dashed line indicates the obscured HC area.
NB: QWP is removed
Figure 16: Images of 8CB in a circular point HC at 20 N, 50% SRR at speeds of (a) 10 mms-1 (b) 100 mms-1 (c) 200 mms-1 (d) 500 mms-1. NB: QWP
In dynamic conditions a birefringent effect is observed inside the HC area. At low speeds and 10 mms-1 and
100 mms-1 [Fig 16(a) and 16(b) respectively] very little birefringence is noted inside the contact. As speed increased to
200 mms-1 [Fig 16(c)] an orange colour inside the HC indicates a birefringent effect. At even higher speeds of 500 mms-
1 [Fig 16(b)] the area inside the HC turns light blue. The QWP was removed in these tests so the images could be
compared against an interference colour chart but this shift in colour was not found to match a standard interference
colour scale. However, this effect can only be attributed to a birefringent effect, and the colour change due to an
increase in retardation as the film thickness increases with speed in the HC. These results demonstrate that at high
speeds the lamellar normal of 8CB tilts towards (or lies parallel to) the entrainment velocity vector. This observation
is consistent with other studies that have used in situ Raman spectroscopy [9, 22] and FTIR  to show that C
biphenylcarbonitrile (CB) structures align parallel to the shearing plane in a HC zone.
For comparison, contact images from the same test conditions (with no QWP) are shown for TEOL in Figure
17. In these tests no birefringent effect was observed inside the HC irrespective of speed.
Figure 17: Images of TEOL in a point HC (QWP removed) at 20 N, 50% SRR at speeds of (a) 10 mms-1 (b) 100 mms-1 (c) 200 mms-1 (d) 500 mms-1.
Oblique microscope experiments
An oblique microscope setup was mounted on the EHD tribometer to investigate the presence of LC structures
that are aligned homeotropically in the contact. This case cannot be detected with a microscope normal to the contact
as incident light orthogonal to the lamellar planes will not experience birefringence. When the microscope is set at an
oblique angle, in this case 45°, structures aligned homeotropically will display birefringence when the light ray is
incident on the ordinary and extraordinary refractive index axes.
Due to undesired reflection effects at the glass-air and the glass-lubricant interfaces a very high intensity light
source was required to image the HC. A 633 nm (red) 3 mW HeNe laser was an appropriate intensity. However, it was
found that using a laser gave some undesired speckle patterns and other noise in the image due to imperfect extinction
at the analyser. Images were taken at speeds of 10, 100, 200, and 500 mms-1.
Reference images were taken using optically isotropic glycerol as the test lubricant. Figure 18(a) – 18(d) show
these images which will be used as a control to identify the presence of birefringent effects for the TEOL and 8CB. At
low speeds [Fig 18(a)] a clear Maltese cross is observed due to the deformation of the glass; the centre of the contact
appears black indicating there is no phase shift in the light reflected from the ball. As speed increased [Figures 18(b) –
18(d)] the centre of the HC remains dark, some light is reflected back and reaches the camera due to subtle
imperfections in the optical alignment.
Images for TEOL are shown in Figures 18(e) – (h); at all speeds no significant birefringent effect is noted inside
the HC area when compared to the control images taken with glycerol in the contact [Figures 18(a) – 18(d)]. At a speed
of 500 mms-1 the measured film thickness using optical interferometry was approximately 102 nm, which would give
an optical path length of approximately 288 nm (𝑡 =
() = 288 𝑛𝑚, 𝑤ℎ𝑒𝑟𝑒 ℎ = 102 𝑛𝑚). If the LC structure was
homeotropically aligned in the contact, as suggested by the previous experiments [Fig 13] with the microscope normal
to the contact, a noticeable birefringent effect would be expected. This leaves two cases (i) there is no structure at the
contact or (ii) the optical anisotropy of the sample is sufficiently small that the phase shift of the light is small. Previous
work by Lockwood et al which studied this TEOL system in an EHD contact through film thickness, friction, and
rheological testing were not confident in concluding the presence of homeotropic alignment in the contact . This
would support case (i) that concludes the LC is not aligned homeotropically in the contact and would even suggest
there is no long-range order inside the HC. There is still uncertainty about TEOLs unusual lubricating properties due to
the lamellar liquid crystal structure reported in [23, 24]. Case (ii) is not worth dismissing and should be the subject of
further study by measuring the TEOL optical anisotropy.
8CB displayed a clear birefringent effect inside the HC in these tests [Figures 18(i) – 18(l)] when compared to
the control images taken with glycerol [Figures 18(a) – 18(d)]. The birefringence inside the HC only becomes noticeable
at speeds of 100 mms-1 [Fig 18(j)] as the film thickness increases to give an optical path length that gives a noticeable
birefringent effect. This is characterised by an intense reflection at the centre of HC with a sufficient phase shift such
that it is not extinct by the analyser. As the speed, and hence the film thickness and optical path length, increases the
intensity of the reflection increases [Figures 18(k) and 18(l)]. This result confirms that the 8CB sample is tilted or
parallel to the entrainment velocity vector considering the birefringence seen with the normal microscope [Fig 16].
Figure 18: PLM at an oblique (45°) angle to a circular HC at a load of 20 N, 50 % SRR, and speeds of 10 mms-1, 100 mms-1, 200 mms-1, 500 mms-1
imaging samples of glycerol (a) – (d), TEOL (e) - (h) and 8CB (i) – (l)
A low-cost technique has been developed that can produce high contrast images of the flow behaviour and
molecular alignment of structured birefringent lubricants in high pressure tribological contacts. The method described
is appropriate for in lubro investigations of anisotropic liquid crystal lubricants under different conditions of shear,
pressure, entrainment speeds, and temperature. This method is capable of simultaneous friction measurement and
birefringence imaging, while the optical setup can quickly be modified to perform film thickness measurements using
thin film interferometry. With the use of two microscope setups, a perpendicular and oblique setup, it is possible to
investigate the presence of homeotropically aligned liquid crystals by comparing results from each geometry.
This provides a powerful set of methods for investigating the relationship between LC molecular orientation
and tribological properties. The setup is limited to a transparent optically isotropic disc specimen (i.e. glass) but a range
of reflective ball specimens can be used (e.g. CoCr). A future publication will describe the use of these methods to
understand the behaviours of liquid crystal forming biomolecules.
The performance and applications of this method was tested with TEOL and 8CB, both of which are liquid
crystalline with a lamellar structure. The observed behaviour of 8CB with the normal and oblique microscope shows
that they tilt towards the entrainment velocity vector, a finding that is consistent with published results using other
techniques. TEOL did not show birefringence inside the HC under the perpendicular or oblique microscope which
suggests the LC does not align homeotropically inside the contact area. This may be due to the low birefringence of
TEOL, so a thicker film may be required to determine the TEOL structure at the contact. This method was successful
for gaining a new understanding of TEOL lubricant flow in the contact inlet and for characterising the molecular
alignment dependence on speed and shear.
This technique has an excellent potential to go beyond the work that has been described in this report.
Experimental studies of the molecular alignment of lubricants has been growing rapidly in recent years with many
developments in Raman spectroscopy, FTIR spectroscopy, and XRD in the context of tribology for determining in situ
molecular alignment. PLM techniques are a complimentary, visual, low cost method for developing new structured
lubricants and determining their molecular configuration, conformation, and orientation in and around tribological
RJE would like to thank the STLE for honouring him with the E. Richard Booser Scholarship which sponsored this
research. He is grateful to his project supervisors, Dr. Monica Ratoi and Dr. Brian Mellor for their guidance, support,
and encouragement during this project. Additionally, he is thankful for the support from Professor Peter Dobson
(Oxford University, UK) and Matthew Delaney (Optoelectronics Research Centre, University of Southampton, UK) for
help sourcing and developing the optical setups in this project.
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