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ABSTRACT
See-through optical components are being intensively studied in applications such as Head-up-displays (HUD) and
Head-mounted-displays (HMD). In particular, volume holographic optical elements (vHOE) have received a lot of
attention due to their unique optical (angular and spectral selectivity) and mechanical (lightweight and thin)
characteristics which make them perfectly suitable for use in integrated optical components like spectacle lenses and car
windshields. Bayfol® HX photopolymer films prove themselves as easy to process recording materials for vHOEs. The
Bayfol® HX instantly developing holographic photopolymer film provides full color capability and adjustable diffraction
efficiency as well as an unprecedented optical clarity when compared to classical volume holographic recording
materials like silver halide emulsions (AgX) or dichromated gelatin (DCG). Besides the recording step, no pre- or post-
processing is necessary and easy mass production of vHOEs in a completely dry roll to roll process is possible.
The layout of a typical Bayfol® HX film consists of a light-sensitive photopolymer layer coated onto a transparent
substrate and protected on the other side by a cover film. The substrate is particularly beneficial, not only for easy
handling of the film during holographic recording, but also for further mechanical processing steps which are required to
embed the film into a finished optical component. However for certain applications it is desirable to remove the substrate
before or after recording. This will allow the user to make full use of the high flexibility of the photopolymer layer, for
example if it comes to curved surfaces that have to be covered. Also more complex stack geometries can be realized in
which the photopolymer layer could be embedded in optically well designed cavities or mechanically demanding setups.
To facilitate this, we developed Bayfol® HX film grades in which the substrate has a lower adhesion to the photopolymer
layer compared to the protective cover film. Therefor the substrate can be removed first in contrast to existing Bayfol®
HX film grades which only allow to remove the protective cover film. On the other hand the adhesion of the protective
cover film can also be well controlled, so that it can be specifically selected according to the needs of the surface to
which the photopolymer layer has to be transferred to. In this paper we demonstrate versatile application processes
making use of these transfer grades of Bayfol® HX films with respect to adhesion design, integration in complex stacks
and application on curved surfaces.
Keywords: holographic photopolymer, volume holographic optical element, head-mounted displays, head-up displays,
processing methods, transfer film.
1. INTRODUCTION
In recent years we have seen a strong increase in the developments and efforts to commercialize devices in the area of
Augmented Reality (AR) displays 1. Many players in the electronics and transportation industry consider such devices as
one of the next big development step for human machine interfaces (HMI) 2. However, until today this information
technology revolution is still in the very beginning since there are some fundamental optical problems to be overcome.
One of the main issues relates to the use of traditional refractive optics which leads to bulky systems, if the trade-off
between large field of view (FOV) and small display size has to be tackled. Diffractive optics realized as surface
holograms are able to resolve this trade-off to some extent. However the fact that surface holograms do not have a strong
selectivity and are realized as surface structures makes them visible to ambient light. Volume holographic optical
elements (vHOEs) show strong selectivity and multiple optical functions can be recorded in the same volume called
multiplexing. Due to the strong selectivity of vHOEs these multiple optical functions can be addressed separately with
virtually no X-talk in contrast to surface holograms. Combined with the high transparency in the Off-Bragg condition
*friedrich-karl.bruder@covestro.com; phone +49 214 6009 6205
Figure 1: Schematic drawing showing the typical three layer stack of Bayfol® HX film.
1.2. Customization of Bayfol® HX Photopolymer Films
For industrial applications it is important to provide a consistent and simple to process material. A major benefit of the
Bayfol® HX recording material is that it does not require any post processing after holographic recording like chemical
treatments or thermal baking – briefly dubbed as instant recording media. For a specific application as discussed before it
is also important to simplify the recording process including the mass replication of vHOEs. Figure 2 shows the different
aspects in which these materials can be customized. On one side the photopolymer recording properties like refractive
index modulation (∆n1 of > 0.05) have been realized for specific grades and film thicknesses can be varied on a wide
range (1 µm up to 70 µm) which is important for tuning the angular and spectral bandwidth according to application
requirements. Also the sensitizer chemistry can be adjusted in terms of light sensitivity, wavelength response and
bleaching properties.
Figure 3: Instrumentation to measure the peel force. Left the Zwick Z2.5, middle and right the 90° jig.
The measured magnitude of the peel force F is normalized to the width W of the test stripe and given in N/mm.
A general description of the respective stacks with their suitable layer sequence is depicted in Figure 4. We have to note
that to achieve a high enough stiffness of the stack a 1 mm thick plastic (usually polycarbonate (PC) or polystyrene (PS)
is used) support has to be adhered to the plastic / photopolymer (non-bleached or bleached / exposed) / plastic layer stack
to measure the correct peel force.
Figure 4: Left: shows the configuration when the layer B adheres less to the photopolymer as the layer A. Right: shows the
configuration when the layer A adheres more to the photopolymer as the layer B. In this case layer B peels 1st and is
already removed. The residual free photopolymer surface is adhered to the plastic support with super glue (cyano-
acrylate) WK-20 from Wekem GmbH, Germany.
It is important to recognize that the layer sequence of the stack under test has to be adapted to the interface for which the
peel force has to be measured. In case the peel force of the layer has to be tested that peels 1st the remaining layer
adjacent to the photopolymer is adhered with a double sticky tape with high enough adhesion (for example Master-Carr,
Scotch 3M USA) to the plastic support (see Figure 4, left). It is important that the double sticky tape sticks smoothly to
both surfaces as air bubbles may cause peak outliers in the force – displacement curve. In case the peel force of the layer
has to be tested, that has the higher adhesion to the photopolymer as the one that peels 1st the residual free photopolymer
surface is adhered to the plastic support (PC) with super glue (cyano-acrylate) WK-20 from Wekem GmbH, Germany
(see Figure 4, right). This process is described a bit more in detail. One liner of a 1 mm thick Makrofol® DE1-1 film is
removed, cleaned with ethanol and dried at room temperature. The free photopolymer surface of the photopolymer is
smoothly attached to this liner-free side of the 1 mm thick Makrofol® DE1-1 film. The stack is put into a holder. The
For the use as protective cover film the highest peel forces are observed for PC and PET and the medium peel forces are
observed for PA. This roughly correlates with the polarity of the chemistry of the protective cover film. By this the
lowest values of the peel force are observed for the non-polar olefin type PP and PE. An exception is TAC which shows
similar low peel forces like PP and PE. And also a PET treated with a specific primer PETwP could change the peel
force behavior dramatically compared to the bare PET protective cover film.
For the use as substrate again the highest peel forces are observed for PC and PET and the medium values are seen for
PA and this time TAC. This makes again sense in terms of the polarity of the substrates. However they are significantly
higher (order of magnitude(s)) than the respective peel forces if those films are used as protective cover films. On PP and
PE coating of our photopolymer formulation is not possible because of their low surface energy. It would also not make
sense as long as we have to record through such substrates as they are not of optical quality. However the specific
PETwP substrates offer excellent coating properties for our photopolymer formulations and exhibit similar low adhesion
as the lowest peel forces of the protective cover films indicate. Therefor PETwP are suitable candidate substrates for a
transfer grade of Bayfol® HX film.
In a transfer grade the peel force of the protective cover film towards the photopolymer layer in the non-bleached state
has to be higher as the peel force of the substrate to the non-bleached photopolymer layer. Therefore, as a protective
cover film, that could be combined with the PETwP substrate to facilitate a transfer grade, we can focus on PC, PET and
PA based on the peel forces in Table 1. PET is not an as good candidate as PC or PA as protective cover film in this case
as it has birefringence and this will limit the ways how to record a vHOE through it. If we want to remove also the
remaining protective cover film after vHOE recording and bleaching, the peel force of the protective cover film towards
the bleached / exposed photopolymer layer has to be as low as acceptable. Based on the data given in Table 1 PA is the
preferred candidate as a protective cover film.
As Table 1 only was used to get a rough overview and does not contain all the necessary peel forces we will showcase in
the following in more detail how to control adhesion for specific cases.
At first we investigate the thickness dependency of the peel forces for a fixed photopolymer formulation (∆n ~ 0.045)
coated on a PETwP substrate and using PA as protective cover film. Respective photopolymer films were coated on the
pilot line. The results are shown in Figure 6. We varied the thickness d of the photopolymer layer from 1.3 µm to 3.0 µm
to 5.0 µm and finally to 10.0 µm. The peel forces were measured according to the procedures described in the
subsections 2.1. to 2.4. for the protective cover film and for the substrate in the non-bleached and as well in the bleached
state. Obviously the peel force of the protective cover film PA is more or less independent on d and on the state of the
photopolymer layer, either non-bleached or bleached / exposed. However the peel force of the substrate increases with d
in the non-bleached state as well as in the bleached / exposed state. By this the peel force of the substrate in the non-
Figure 6: Dependency of peel forces on the photopolymer layer thickness d. Photopolymer formulation fixed (∆n ~ 0.045).
To facilitate a Bayfol® HX film grade that can act as a transfer grade in the non-bleached state at larger d the peel force
of the protective cover film towards the non-bleached photopolymer layer has to be increased. According to what we
learned from Table 1 and the discussion of the results the use of PC as protective cover film would be the logical step.
We first coated photopolymer films - this time on the production line - with thicknesses d = 1.3 mm and d = 3.0 µm of
the photopolymer formulation (∆n ~ 0.045), using PETwP as substrate and PA or PC as protective cover films. The
results of the measurement of the peel forces are depicted in Figure 7.
Figure 7: Dependency of the peel forces on the photopolymer thickness d and the chemistry of the protective cover film.
Photopolymer formulation fixed (∆n ~ 0.045).
Again for d = 1.3 µm and d = 3.0 µm in the non-bleached state the peel forces of the protective cover film PA and the
substrate PETwP are very similar with the peel force of the PA protective cover film being slightly higher.
Experimentally the substrate peels 1st in the non-bleached state for d = 1.3 µm and d = 3.0 µm for the protective cover
film PA, as expected. When we use PC as a protective cover film its peel force towards the non-bleached photopolymer
layer is significantly higher than that of PA. And again experimentally the substrate peels 1st in the non-bleached state for
d = 1.3 µm and d = 3.0 µm for the protective cover film PC.
To further extend the insights gained so far to thicker photopolymer layers we coated in the pilot line a d = 15 µm thick
photopolymer formulation (∆n ~ 0.045) on the PETwP substrate and varying the chemistry of the protective cover film in
a wider range, meaning using TAC, PE, PA and PC. The results are shown in Figure 8. As expected from all previous
insights only the photopolymer film using the PC as protective cover film can be used as a transfer grade of Bayfol® HX
film in the non-bleached state. For PA as a protective cover film the peel force towards the non-bleached photopolymer
at the given thickness d = 15 µm is simply not large enough.
Figure 9: Dependency of the peel forces on the chemistry of the protective cover film. Photopolymer formulation fixed (∆n
~ 0.035).
The most significant change by changing the photopolymer formulation is an increase of the peel force of the substrate
towards the photopolymer layer especially in the non-bleached state. In addition the peel force of the PC protective cover
film decreases too, so that no transfer grade of Bayfol® HX film can be obtained in the non-bleached state for this
photopolymer formulation.
4. PHYSICAL BONDING
In 21 we described two different ways how to achieve a plastic / vHOE / plastic sandwich layer stack. One way is to use a
compatible OCA that limits the shift of the Bragg condition to a low and reproducible level that can be compensated in
the recording setup already and a second way using a proprietary UV-curable adhesive film. In both ways, besides the
base film an adhesive layer is placed in between the vHOE containing photopolymer film and the final top layer. That
means at least four layers are involved. OCA layers may be too soft and temperature sensitive so that they could not be
applied to FIM as outlined in 21, UV curable adhesive layers may be problematic to use when the plastic / vHOE / plastic
stack has to be formed before recording the vHOE in the photopolymer layer by obvious reasons. Another way to form
Figure 10: Physical bonding after recording to achieve a plastic / vHOE / plastic sandwich layer stack.
First, after recording the vHOE but before bleaching, a cover layer is laminated (preferably a PC cover player) on the
free surface of the photopolymer layer. This non-activated plastic / vHOE / plastic sandwich stack is put into an oven
under dark room illumination at a certain temperature T for a certain time t to activate adhesion between the cover layer
and the free surface of the photopolymer layer. During this stage the peel force between the photopolymer layer and the
cover layer increases dramatically. After that oven step the activated stack is bleached using a UV-VIS lamp (λ) with a
specific dosage E.
4.2. Physical bonding before vHOE recording
This process is most flexible if used in combination with the transfer grade Bayfol® HX film.
Figure 11: Physical bonding before recording to achieve a plastic / vHOE / plastic sandwich layer stack.
In this case the base film of the unexposed photopolymer film can be the thermoplastic substrate itself or in the case of a
transfer grade Bayfol® HX film the remaining protective cover film. The process is the same as before including the
adhesion activation step in the oven. However after that adhesion activation and before bleaching the vHOE recording
has to be performed.
Figure 12: Time – temperature behavior of the peel force obtained by physical bonding. Left: raw data. Right: master curve
@ t = 120 s (means temperatures of t = 30 s and t = 300 s data are scaled). Photopolymer formulation with ∆n ~ 0.03
and thickness d = 70 µm.
Figure 13: Time – temperature behavior of the peel force obtained by physical bonding. Left: raw data. Right: master curve
@ t = 300 s. Photopolymer formulation with ∆n ~ 0.045 and thickness d = 6 µm.
Another example is shown in Figure 13. Here we used a photopolymer formulation giving a ∆n = 0.045 and a
photopolymer thickness d = 6 µm. We used a 250 µm thick PC film (Makrofol® DE1-1) for physical bonding a cover
layer.
If we compare physical bonding before and after vHOE recording we have to state that if physical bonding is done after
vHOE recording the Bragg condition shifts depending on the recording geometry, T, and t. Higher T results in larger
Bragg detuning, also longer t gives larger Bragg detuning. However the time – temperature behaviour for the Bragg
detuning is different from that of the adhesion. So an optimum for this trade-off between adhesion and Bragg detuning
has to be elaborated in the specific vHOE case. In general a good starting point to optimize physical bonding is using
70°C < T < 100°C and 20 s < t < 600 s. If we do the physical bonding before vHOE recording the Bragg detuning is not
decisive any more, however as we cannot laminate the sticky photopolymer surface to the recoding support anymore, in
general a more complex recoding setup may have to be used.
A further option to optimize physical bonding as described above is to treat he to bonded surface of the cover layer with
UV radiation, plasma or corona.
It should be noted that by the heat treatment used in the physical bonding process the photopolymer film depicted in
Figure 9 on the very right side could be changed into a transfer grade of Bayfol® HX film, as the peel force of the PC
protective cover film can be significantly increased above the peel force to the PETwP substrate in the non-bleached
state.
Figure 14: View into the SAMK High Pressure Forming (HPF) machine of Niebling.
Here each stack was heated 1st within 7.5 s to 110 °C using radiant heaters set to 240°C to 280°C. Immediately
afterwards the heated stack was pushed onto a die for 10 s under high pressure of ~ 100 bar. The die temperature was set
to 120 °C. The die produces a lens shape of 100 mm diameter with a radius of curvature of 180 mm. The whole cycle
including heating and high pressure forming took 17.8 s.
An example of a formed sheet is depicted in Figure 15, left side. Still the coloration caused by the sensitizer dye of the
initiator system can be seen, as no exposure or bleaching has been done. On the right side of Figure 15 the formed sheet
is put between crossed polarizer sheets. Obviously there is only low birefringence in the formed area with the centre free
of any birefringence. Also wrinkle formation is completely suppressed and no delamination of the PC / photopolymer /
PC sandwich stack was observed, which proof that the obtained adhesion by physical bonding at all interfaces was
sufficient. According to the previously reported results the peel forces should be in the range of 0.3 N/mm.
s
Figure 15: Left: 3D formed PC / photopolymer / PC stack. Right: 3D formed lens between crossed polarizers.
The process described in subsection 4.2. and further sketched in Figure 11 is now extended by the HPF process between
the physical bonding step and the vHOE recording. Figure 16 shows the extended flow chart of the whole process.
Figure 18: Contact copy to record the diffusor in the 3D formed PC / photopolymer / PC stack.
The master was laminated on the convex side of the 3D formed copy stack including also the TG1 photopolymer. Again
an incoherent pre-exposure was done with a green LED using a dosage of ~ 3 mJ/cm2 in the vHOE plane to further
suppress the recording of noise holograms in the copy 19. After that the copy was recorded with the reference beam
incident on the concave side of the 3D formed copy stack using again 1.375 mW/cm2 intensity at an exposure time of 10
s. This setup assures that the curvature of the diffuse object used in the master recording into a plane master film is
compensated in the copy process, so that in reconstruction again a plane diffusor is obtained, as if we would have
recorded it in the before described direct two beam recording.
8. EVALUATION
The scheme of reconstruction of the real image of the copy vHOE using the phase conjugated reference beam is depicted
in Figure 19.
9. CONCLUSION
In this paper we first demonstrated how a transfer grade of Bayfol® HX film can be generated by carefully selecting the
substrate and the protective cover film and how the involved adhesion forces at the interfaces can be controlled. The
transfer grade allows to peel off the substrate first and if properly designed the bare photopolymer layer can be retained
after recording as the protective cover film can be removed too. In addition to (UV) OCA bonding, as demonstrated in
earlier papers, we introduced physical bonding by heat activation as another possibility. Physical bonding reduces the
layers involved to form a plastic / photopolymer / plastic stack and can be applied before or after recording a vHOE into
the photopolymer layer. Especially in combination with the transfer grade concept, physical bonding is a powerful tool to
enhance the possibilities to integrate vHOEs into plastic sandwich layer stacks that are compatible with state of the art
plastic processing. We proofed this by showing the integration of the photopolymer layer into a plastic sandwich stack
that undergoes a 3D forming - using high pressure forming - of this sandwich stack before recording. Finally we
recorded successfully a vHOE into this 3D formed stack that reconstruct a plane image of a diffusor. This further
demonstrates the extremely high flexibility of the Bayfol® HX film technology platform in recording and integrating
vHOEs in plastic optical parts. This in turn allows lightweight and thin design of complex optical devices using cost
effective plastic processing technology.
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